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@article{nokey,

title = {Real-time probing of the interplay between spinodal decomposition and crystallization during morphological evolution in printed organic solar cells},

author = {J S Zhang and L Xie and Z R Li and Y C Zhang and M B Faheem and G J Pan and A Buyan-Arivjikh and X Z Jiang and L X Li and M Schwartzkopf and B Sochor and S K Vayalil and Q Qiao and Z Y Ge and P M\"{u}ller-Buschbaum},

url = {\<Go to ISI\>://WOS:001529811300001},

doi = {10.1016/j.nanoen.2025.111301},

issn = {2211-2855},

year  = {2025},

date = {2025-10-01},

journal = {Nano Energy},

volume = {143},

abstract = {The performance of organic solar cells (OSCs) strongly depends on the phase separation and crystalline properties within the active layer. However, the lack of deep understanding of morphological evolution, particularly regarding spinodal decomposition and crystallization mechanisms, presents substantial challenges in achieving precise morphological control. In this work, we systematically investigate the film formation of PBDB-TF-TTz: BTP-4F-24 blends during slot-die coating while comparing o-xylene and chlorobenzene (CB) as solvents to create distinct polymer/solvent/non-solvent systems. The complex interplay between the spinodal decomposition and crystallization processes is elucidated through complementary in situ grazing incidence small-angle Xray scattering (GISAXS) and in situ grazing incidence wide-angle X-ray scattering (GIWAXS) together with the calculation of spinodal curves. Our findings indicate that CB-processed active layers generate larger initial clusters, promoting domain coarsening while suppressing crystallization. In contrast, o-xylene-processed films exhibit optimized phase separation, larger crystallites, and face-on molecular orientations, enhancing charge transport. Additionally, polymer-dominated thermodynamic and kinetic evolution plays a critical role in shaping out the final morphology. Consequently, OSCs fabricated with o-xylene achieve higher power conversion efficiency than those processed with CB. These insights enrich the understanding of morphological evolution and provide valuable guidelines for morphology optimization.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Interfacial and solvent dehydrogenation engineering enables long-life high-voltage lithium-ion batteries},

author = {S Amzil and Y Y Xiao and D H Ma and J P Li and T H Xu and Z Z Ru and L H Cao and M Yang and S Y Luo and M Q Wu and M L Peng and Y H Li and S Tian and J Gao and Y Yu and P M\"{u}ller-Buschbaum and T Cai and F Zhao and Q Li and Y J Cheng and Y G Xia},

url = {\<Go to ISI\>://WOS:001523364200001},

doi = {10.1016/j.mser.2025.101051},

issn = {0927-796X},

year  = {2025},

date = {2025-09-01},

journal = {Materials Science \& Engineering R-Reports},

volume = {166},

abstract = {High-voltage lithium-ion batteries (LIBs) using LiNi0.8Mn0.1Co0.1O2 (NCM811) cathode materials present a promising avenue for increasing energy density. However, achieving stable operation at elevated voltages is hindered by chemical instability in ethylene carbonate (EC)-based electrolytes, leading to parasitic interfacial reactions. Herein, we introduce 2-hydroxy-5-nitro-3-(trifluoromethyl) pyridine (HNTFP) as a multifunctional electrolyte additive to mitigate EC dehydrogenation and minimize interfacial side reactions. Leveraging the unique functional groups of HNTFP (NO2, CF3, and C\textendashO), we demonstrate the formation of a robust hybrid/ inorganic cathode electrolyte interphase (CEI) on high-voltage cathodes and a fluorine-rich solid electrolyte interphase (SEI) on graphite anodes. These interphases enable 4.5 V-charged NCM811||graphite full cells to achieve a capacity retention of 92 % over 500 cycles, while commercial 1 Ah pouch cells retain 89 % over 1000 cycles. This study provides a fresh perspective on electrolyte additive design and underscores the transformative potential of HNTFP in enabling long-life, high-voltage LIBs with superior stability and performance.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Emerging low-dimensional perovskite resistive switching memristors: from fundamentals to devices},

author = {S L Wang and H Lian and H F Ling and H Wu and T X Xiao and Y J Huang and P M\"{u}ller-Buschbaum},

url = {\<Go to ISI\>://WOS:001558650900003},

doi = {10.29026/oea.2025.240316},

issn = {2096-4579},

year  = {2025},

date = {2025-08-24},

journal = {Opto-Electronic Advances},

volume = {8},

number = {8},

abstract = {With the exponential growth of the internet of things, artificial intelligence, and energy-efficient high-volume data digital communications, there is an urgent demand to develop new information technologies with high storage capacity. This needs to address the looming challenge of conventional Von Neumann architecture and Moore's law bottleneck for future data-intensive computing applications. A promising remedy lies in memristors, which offer distinct advantages of scalability, rapid access times, stable data retention, low power consumption, multistate storage capability and fast operation. Among the various materials used for active layers in memristors, low dimensional perovskite semiconductors with structural diversity and superior stability exhibit great potential for next generation memristor applications, leveraging hysteresis characteristics caused by ion migration and defects. In this review the progress of low-dimensional perovskite memory devices is comprehensively summarized. The working mechanism and fundamental processes, including ion migration dynamics, charge carrier transport and electronic resistance that underlies the switching behavior of memristors are discussed. Additionally, the device parameters are analyzed with special focus on the effective methods to improve electrical performance and operational stability. Finally, the challenges and perspective on major hurdles of low-dimensional perovskite memristors in the expansive application domains are provided.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Biopolymer-Templated Hierarchical 3D-Structured Gold Nanoparticle/Graphene Oxide Hybrid Materials for Ultrasensitive Surface-Enhanced Raman Scattering},

author = {Y J Guo and G J Pan and S Tu and Y Bulut and J G Zhou and A Jeromin and T F Keller and A Stierle and G Nemeth and F Borondics and B Sochor and S K Vayalil and L D S\"{o}derberg and P M\"{u}ller-Buschbaum and S V Roth},

url = {\<Go to ISI\>://WOS:001552302100001},

doi = {10.1002/adfm.202515801},

issn = {1616-301X},

year  = {2025},

date = {2025-08-19},

journal = {Advanced Functional Materials},

abstract = {Surface-enhanced Raman scattering (SERS) is a highly advantageous analytical technique for detecting trace biological and chemical compounds. However, significant challenges remain in the cost-effective fabrication of large-area and homogenous SERS substrates. A simple and scalable approach utilizing a layer-by-layer spray deposition followed by thermal annealing is proposed to fabricate cellulose nanofibril (CNF) films loaded with gold nanoparticles (Au NPs) and graphene oxide (GO) hybrids as SERS substrates. These hybrid 3D structures comprising CNF/Au NPs/GO significantly enhance SERS sensitivity by both electromagnetic enhancement and chemical enhancement. Incorporating CNF as a 3D network enables a more uniform distribution of Au NPs/GO. Thermal annealing further induces hotspots. For instance, the annealed CNF/Au NPs/GO hybrid thin films achieve a detection limit of 1.0 x 10-13 m and a high enhancement factor of 4.97 x 1011 for Rhodamine 6G. Grazing incidence small-angle X-ray scattering combined with nano-Fourier-transform infrared spectroscopy is first used to confirm the combined Raman enhancement mechanism of localized surface plasmon resonance and interface charge transfer with high spatial resolution. Therefore, the proposed methodology establishes a robust framework for the scalable fabrication of ultrasensitive SERS substrates.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Anchoring and Competition: Weakly Solvated Structure of Glymes Enhances Stability in Lithium Metal Batteries Operating under Extreme Conditions},

author = {T L Zheng and M Q Wu and J W Xiong and M Yang and W Z Guo and Q H Zeng and H W Yu and T H Xu and W P Xie and Y Y Xiao and Z J Xu and Y X Liang and Z R Li and R X Qi and G J Pan and X T Shi and H B Zhao and X H Li and Y Y Xia and Y J Cheng and Y G Xia and P M\"{u}ller-Buschbaum},

url = {\<Go to ISI\>://WOS:001549938900001},

doi = {10.1002/anie.202511336},

year  = {2025},

date = {2025-08-14},

journal = {Angewandte Chemie-International Edition},

abstract = {Lithium metal batteries (LMBs) face challenges from unstable and fragile solid electrolyte interphases (SEIs). In this work, we successfully develop a novel electrolyte by effectively modulating the competitive solvation process in LMBs. In this formulation, the C \& horbar;O \& horbar;C motifs of glymes are competitively substituted by other anions and solvents to achieve single oxygen site coordination, thereby facilitating a weak solvation effect. At an apparent concentration of 1.25 M, a solvated sheath enriched with anions and single oxygen-bound complexes is formed, which significantly enhances lithium metal compatibility and promotes rapid desolvation kinetics. The designed electrolyte using weakly solvated structures exhibits remarkable stability at both 25 degrees and 80 degrees C, enabling the lithium iron phosphate (LFP)||Li cell to achieve over 2000 cycles (capacity retention: 90%) and 500 cycles (capacity retention: 96%), respectively. Interestingly, the low N/P ratio LFP||Li (N/P = 1.8) full battery maintains a stable capacity over 50 cycles, and the commercial 1.1 Ah LFP||Li pouch cell shows a great stability (capacity retention: 91.0%, CE: 99.82%) over 20 cycles. The distinctive solvation regulation strategy has paved a novel research avenue for the realization of high-performance LMBs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Structural Evolution During Repeated Spray Deposition of FeCl3-Doped Poly(Styrene)-b-Poly(4-Vinyl Pyridine) Layers},

author = {S S Yin and W Cao and S Tu and S Z Liang and Y Q Zou and T Tian and G J Pan and Z J Xu and L X Li and L Y Y Cheng and Y J Cheng and M Schwartzkopf and S V Roth and L J Zhai and P Muller-Buschbaum},

url = {\<Go to ISI\>://WOS:001522403500001},

doi = {10.1002/admi.202500298},

issn = {2196-7350},

year  = {2025},

date = {2025-07-04},

journal = {Advanced Materials Interfaces},

abstract = {Nanostructured hematite (alpha-Fe2O3) films exhibit significant potential for energy, environmental, and medical applications. In the present work, a large-scale spray coating deposition method, scanning electron microscopy, and in situ grazing-incidence small-angle X-ray scattering are combined to investigate the structure formation mechanism of pure poly(styrene)-b-poly(4-vinyl pyridine) (PS-b-P4VP) and hybrid PS-b-P4VP/FeCl3 films during and after spray deposition. Under the film deposition conditions specified in this experiment, a layered pure PS-b-P4VP film, a sponge-like hybrid PS-b-P4VP/FeCl3 film, and a porous alpha-Fe2O3 film are obtained upon completion of the deposition. The morphological differences between the investigated pure PS-b-P4VP and hybrid PS-b-P4VP/FeCl3 films result from the interplay among the complexation between FeCl3 and P4VP segments, the crystallization of the P4VP segment, and the surface diffusion of the FeCl3 species. The findings of this work can offer both experimental and theoretical guidance for designing spray-deposited block copolymer and hybrid films.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Temperature-dependent thermal behavior of BTP-4F-12-based organic solar cells},

author = {Z Li and J Zhang and S A Wegener and Y Yan and X Jiang and K Sun and G Pan and T Zheng and M Schwartzkopf and S K Vayalil and C-Q Ma and P M\"{u}ller-Buschbaum},

url = {https://www.sciencedirect.com/science/article/pii/S2211285525004021},

doi = {https://doi.org/10.1016/j.nanoen.2025.111043},

issn = {2211-2855},

year  = {2025},

date = {2025-07-01},

journal = {Nano Energy},

volume = {140},

pages = {111043},

abstract = {Heat is one key factor contributing to performance decreases, which would lead to inevitable morphological changes in the active layers. Common research with ex-situ characterizations ignored the degradation process kinetics, which hinders a comprehensive insight into the underlying thermal degradation mechanisms in organic solar cells (OSCs). In this study, the device thermal stability of BTP-4F-12-based solar cells is investigated with operando tracking of grazing-incidence wide/small-angle X-ray scattering (GIWAXS/GISAXS), providing a deep understanding of temperature-dependent degradation processes. The OSCs show a harsh open-circuit voltage (VOC) loss with increasing temperature, which recovers mostly after getting cooled to low temperature. This behavior is attributed to the charge carrier recombination, π-π stacking distances, and aggregated domains at various temperatures. The irreversible loss of FF and short-circuit current density (JSC) during aging is due to changes in crystallinity and dense π-π stacking. Furthermore, no obvious correlation is found for the sharp decreased FF for the final aged solar cells, suggesting that such a degradation originates not from high temperature but more likely from the heating/cooling process. PBDBTCl-DTBT:BTP-4F-12 solar cells suffer from a more severe thermal degradation compared with PBDB-TF-T1:BTP-4F-12, where the bad miscibility of donor and acceptor is not beneficial to an optimized stable active layer and the intrinsic thermal properties of the polymer donor also affect significantly the stability of the blend films and solar cells. This study reveals a temperature-dependent thermal degradation of OSCs, which broadens our knowledge from common ex-situ characterizations and deepens our understanding of thermal degradation mechanism.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Analogue Molecular Doping Engineering Enables High Ionic Conductivity of Polyvinylidene Fluoride-Based Polymer Electrolytes},

author = {M H Li and T Tian and X Q Yang and Y L He and D S Zhang and P M\"{u}ller-Buschbaum and S B Yang and B Li},

url = {\<Go to ISI\>://WOS:001494651200001},

doi = {10.1021/acsnano.5c04141},

issn = {1936-0851},

year  = {2025},

date = {2025-05-22},

journal = {Acs Nano},

volume = {19},

number = {21},

pages = {20084-20095},

abstract = {Solid polymer electrolytes (SPEs) based on polyvinylidene fluoride (PVDF) are promising candidates due to their outstanding mechanical properties and intrinsic safety features. Unfortunately, the crystalline alpha phase of PVDF limits the mobility of lithium ions, thus leading to low lithium ion conductivity. Herein, a molecular doping strategy is proposed to achieve high lithium ion conductivity of the PVDF-based electrolyte (md-PVDF) via introducing polyvinylidene dichloride (PVDC) to reduce the generation of the harmful alpha phase of PVDF. As the molecular analog of PVDF, PVDC is homogeneously dispersed in PVDF at arbitrary concentrations, and it disrupts the crystallization of the PVDF matrix. Moreover, the chlorine functional group in doping molecular PVDC not only enhances the dissociation of Li salt but also reduces the energy barrier of lithium-ion migration. Consequently, the resulting md-PVDF electrolytes show significantly high ionic conductivity (1.4 x 10-3 S cm-1 at room temperature). The lithium symmetric batteries with md-PVDF electrolytes cycle stably for over 2000 h at 0.1 mA cm-2, and the Li||LFP batteries display excellent cycling stability over 500 cycles at a high rate of 5 C. In addition, the md-PVDF electrolytes exhibit outstanding low-temperature performance, achieving an ionic conductivity of 3.0 x 10-4 S cm-1 at -5 degrees C. This work demonstrates a strategy to improve the ionic conductivity of SPEs and to realize fast charging of solid-state lithium.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Engineering Conjugated Bridges in TPE-BT-Based Donor\textendashAcceptor Molecules for Optimized Resistive Random Access Memory},

author = {X Liu and H Lian and L Zhao and Z Qin and T Xiao and X Jiang and T Guan and S Wang and P M\"{u}ller-Buschbaum and Q Dong},

url = {https://doi.org/10.1021/acsami.5c03859},

doi = {10.1021/acsami.5c03859},

issn = {1944-8244},

year  = {2025},

date = {2025-05-14},

journal = {ACS Applied Materials \& Interfaces},

volume = {17},

number = {19},

pages = {28459-28471},

abstract = {Four donor\textendashacceptor (D-A) type organic small molecules, namely, 4,7-bis(4-(1,2,2-triphenylvinyl)phenyl)benzo[c][1,2,5]thiadiazole(TPE-BT), 4,7-bis((4-(1,2,2-triphenylvinyl)phenyl)ethynyl)benzo[c][1,2,5]thiadiazole(TPE-ynl-BT), 4,7-bis(5-(4-(1,2,2-triphenylvinyl)phenyl)thiophen-2-yl)benzo[c][1,2,5]thiadiazole (TPE-Th-BT), and 4,7-bis((5-(4-(1,2,2-triphenylvinyl)phenyl)thiophen-2yl)ethynyl)benzo[c][1,2,5]thiadiazole(TPE-Th-ynl-BT), each incorporating unique conjugated bridges, are designed, synthesized, and integrated into resistive random access memory (RRAM) devices. Current\textendashvoltage (I\textendashV) measurements indicate that the TPE-BT, TPE-ynl-BT and TPE-Th-BT based devices exhibit write-once-read-many-times (WORM) characteristics, while TPE-Th-ynl-BT based devices show a stable flash-type switching behavior. In comparison to TPE-BT, the memory devices constructed with TPE-ynl-BT, TPE-Th-BT and TPE-Th-ynl-BT, which include additional conjugated bridges, exhibit nonvolatile memory capabilities with reduced threshold voltages, higher ION/IOFF (104:1), enhanced stability, and improved reproducibility. The photophysical, electrochemical analyses, and X-ray diffraction (XRD) results reveal that incorporating conjugated bridges within molecular structures can enhance data storage performance while reducing power consumption. Our findings demonstrate that these conjugated bridges play a crucial role in optimizing electrical memory characteristics and resistive switching behavior. Moreover, the device fabricated with TPE-Th-ynl-BT is effectively applied to logic gate circuits and American Standard Code for Information Interchange (ASCII) art function, highlighting its promising potential as a smart sensor within artificial intelligence (AI) networks.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Overcoming efficiency and cost barriers for large-area quantum dot photovoltaics through stable ink engineering},

author = {G Shi and X Ding and Z Liu and Y Liu and Y Chen and C Liu and Z Ni and H Wang and K Ito and K Igarashi and K Feng and K Zhang and L L\"{u}er and W Chen and X Lyu and B Song and X Sun and L Yuan and D Liu and Y Li and K Lu and W Deng and Y Li and P M\"{u}ller-Buschbaum and T Li and J Zhong and S Uchida and T Kubo and N Li and J M Luther and H Segawa and Q Shen and C J Brabec and W Ma},

url = {https://doi.org/10.1038/s41560-025-01746-4},

doi = {10.1038/s41560-025-01746-4},

issn = {2058-7546},

year  = {2025},

date = {2025-04-07},

journal = {Nature Energy},

abstract = {The bottom-up construction of electronics from colloidal quantum dots (CQDs) could innovate nanotechnology manufacturing through printing. However, the unstable and expensive semiconductive CQD inks make the scaling up of CQD electronics challenging. Here we develop a strategy for engineering the solution chemistry of lead sulfide (PbS) CQD inks prepared from a low-cost direct synthesis method. By creating an iodine-rich environment in weakly coordinating solvents, we convert the iodoplumbates into functional anions, which condense into a robust surface shell. The fully charged electrostatic surface layer prevents aggregation and epitaxial fusion of CQDs, yielding stable inks. By eliminating the fusion-induced inter-band states, we print a compact CQD film with uniformity in three dimensions, flattened energy landscape and improved carrier transport. We achieved a certified efficiency of 13.40% on 0.04 cm2 cells, with a 300-fold increase in active area, scaling up to a 12.60 cm2 module with a certified efficiency of 10%.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Fabrication of Cobalt Oxide-Block Copolymer Nanostructured Hybrid Films via a Mixed Solvent System},

author = {E Metwalli and M H Darweesh and C Oberleitner and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1002/app.57089},

doi = {https://doi.org/10.1002/app.57089},

issn = {0021-8995},

year  = {2025},

date = {2025-04-06},

journal = {Journal of Applied Polymer Science},

volume = {n/a},

number = {n/a},

pages = {e57089},

abstract = {The synthesized cobalt oxide (CoO) nanosheets embedded within a polymer matrix hold significant potential for applications in sensors, organic electronics, catalysis, organic photovoltaics, and energy storage devices. Using a facile and efficient preparation technique, we combine an organometallic cobalt(II) precursor, a polystyrene-block-polymethyl methacrylate (PS-b-PMMA) diblock copolymer (DBC), and organic solvents to ensure complete dissolution of all components without inducing precipitation or micro-phase separation in the liquid phase. Through a straightforward thermal annealing process, the cobalt salt within the DBC thin films undergoes decomposition, resulting in the formation of CoO nanosheets with a uniform and dense distribution pattern matching the morphology of the DBC. Fourier transform infrared spectroscopy (FTIR) confirms selective phase separation of the cobalt salt within the DBC, while x-ray photoelectron spectroscopy (XPS) indicates the conversion of the salt into CoO. The morphology of the CoO/DBC hybrid films is characterized using atomic force microscopy (AFM), scanning electron microscopy (SEM), and x-ray scattering techniques. This study demonstrates a simple and effective route to prepare a well-defined arrangement of metal oxide clusters, achieving a highly confined particle self-assembly process compared to alternative solution-based methods.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Slurry Additive Approach Enables a Mechanically Robust Binder for Silicon\textendashCarbon Anodes in Lithium-Ion Batteries},

author = {J Feng and X Wu and S Amzil and M Li and X Liu and M Yang and T Yan and P M\"{u}ller-Buschbaum and Y-J Cheng and J Gao and Y Xia},

url = {https://doi.org/10.1021/acsami.4c22330},

doi = {10.1021/acsami.4c22330},

issn = {1944-8244},

year  = {2025},

date = {2025-03-26},

journal = {ACS Applied Materials \& Interfaces},

volume = {17},

number = {12},

pages = {18339-18350},

abstract = {Silicon\textendashcarbon (Si/C) composites hold great promise as substitutes for conventional graphite anodes in high-specific-energy lithium-ion batteries (LIBs). However, their performance is hindered by silicon’s substantial volume expansion during cycling, which can lead to electrode degradation. Traditional poly(acrylic acid) (PAA) binders often struggle to maintain electrode integrity under these conditions. To address this challenge, polyether modified polyurethane acrylic (PUMA) is used as physicochemical cocrosslinking polymer. PUMA offers superior mechanical properties, elasticity, and interfacial stability, enabling it to effectively accommodate silicon’s volume changes and prevent electrode fracture. Through a simple preparation process, we used PUMA as a slurry additive in combination with PAA to form a functional composite binder, facilitating the construction of a stable and robust SEI film. This is conducive to alleviating the volume expansion of silicon and ensuring the cycling stability of the electrode. In Si/C450 half-cells, electrodes enhanced by our binder show a remarkable longevity, maintaining 97.26% of their capacity post 200 cycles at 0.5 C. The full cells Si/C450||NCM811 display a notable performance, achieving a capacity retention of 82.10% after 100 cycles at 0.2 C. These findings underscore the potential of our innovative binder design in enhancing the efficacy of silicon-based anodes in high-energy LIBs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Sandwich-like Hybrid Electrospun Membrane-Based Efficient Hydrogen Evolution System by the Push\textendashPull Double Piezoelectric Effect Driven by Water Flow},

author = {N Hu and D Gao and W Wang and L Lei and H Fan and P M\"{u}ller-Buschbaum and Q Zhong},

url = {https://doi.org/10.1021/acs.langmuir.5c00489},

doi = {10.1021/acs.langmuir.5c00489},

issn = {0743-7463},

year  = {2025},

date = {2025-03-24},

journal = {Langmuir},

abstract = {An efficient photocatalytic hydrogen evolution is realized by a push\textendashpull effect from the piezoelectricity of a flexible hybrid membrane introduced via the water flow energy. The flexible hybrid membrane possesses a sandwich-like structure, prepared by sequentially electrospinning poly(vinylidene fluoride) (PVDF), depositing graphitic carbon nitride with Pt atoms (g-C3N4@Pt), and again electrospinning PVDF. Due to the piezoelectric property of PVDF, the deformation of the obtained sandwich-like hybrid PVDF/g-C3N4@Pt/PVDF membrane triggers two electric fields with the same direction in the top and bottom PVDF membranes. Therefore, either electrons or holes photogenerated by g-C3N4@Pt are attracted to one electric field and repelled by another. This push\textendashpull effect induces a directional movement of charge carriers, which not only eases the separation but also hinders the recombination. Based on this favorable effect and finite element simulations for stress distribution on the membrane, the position of the sandwich-like hybrid PVDF/g-C3N4@Pt/PVDF membrane is optimized. The hydrogen evolution rate strongly increases to 5401 μmol h\textendash1 g\textendash1 under water flow, which is 240% to that of g-C3N4@Pt nanosheets. Thus, the sandwich-like hybrid membrane with a push\textendashpull effect is very suitable for hydrogen production in natural aqueous environments rich in water flow and solar energy, such as lakes and rivers.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Tuning the Morphology of Spray-Coated Biohybrid Beta-lactoglobulin:TiBALDh Films with pH for Water-Based and Nanostructured Titania},

author = {J E Heger and J Reitenbach and L P Kreuzer and G Pan and T Tian and L F Huber and N Li and B Sochor and M Schwartzkopf and S V Roth and A Koutsioubas and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/jacsau.5c00097},

doi = {10.1021/jacsau.5c00097},

year  = {2025},

date = {2025-03-19},

journal = {JACS Au},

abstract = {The whey protein beta-lactoglobulin (β-lg) is used as a biotemplate for the water-based synthesis of nanostructured and foam-like titania films based on its variation in supramolecular structure when denatured at different pH values. Acting as a matrix, β-lg is mixed with the water-soluble titania precursor Ti(IV) bis(ammonium lactate)dihydroxide (TiBALDh) to promote biotemplated titania precipitation. Since TiBALDh is in chemical equilibrium with anatase titania nanoparticles and Ti(IV)-lactate complexes, and this equilibrium shifts with varying pH, the influence of the pH value on the final film morphology becomes essential. This work investigates this influence for three pH values: pH 7, pH 5, i.e., close to the isoelectric point of β-lg, and pH 2. Spray coating, a method of industrial relevance, is used to fabricate biohybrid β-lg:TiBALDh foam-like films. The obtained films are calcined to combust biotemplate β-lg and achieve nanostructured titania films. To understand the influence of pH on the film morphology, grazing-incidence small-angle and wide-angle X-ray scattering (GISAXS/GIWAXS) and grazing-incidence small-angle neutron scattering (GISANS), in combination with scanning electron microscopy (SEM), are applied to both the biohybrid and biotemplated titania films. With these techniques, information about domain sizes, porosity, and crystal structure is obtained with high statistical significance. Fourier-transform infrared spectroscopy (FTIR) probes the interaction of TiBALDh and β-lg on the molecular level as a function of pH. The results underline pH as a suitable tool for tuning the morphology in biotemplated titania films.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Dinitrile-Assisted Electrolyte Helps Overcome Temperature Challenges of Lithium Batteries},

author = {M Wu and S Luo and T Xu and T Zheng and Z Ru and S Amzil and Y Xiao and Y Li and M Peng and W Xue and J Gao and Y Gao and Y-J Cheng and P M\"{u}ller-Buschbaum and Y Xia},

url = {https://doi.org/10.34133/energymatadv.0181},

doi = {10.34133/energymatadv.0181},

year  = {2025},

date = {2025-03-19},

journal = {Energy Material Advances},

volume = {0},

number = {ja},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Unveiling the Li/Electrolyte Interface Behavior for Dendrite-Free All-Solid-State Lithium Metal Batteries by Operando Nano-Focus WAXS},

author = {Y Liang and F C Apfelbeck and K Sun and Y Yan and L Cheng and G Pan and T Zheng and Y Cheng and A Davydok and C Krywka and P M\"{u}ller-Buschbaum},

doi = {10.1002/advs.202414714},

issn = {2198-3844},

year  = {2025},

date = {2025-03-01},

journal = {Adv Sci (Weinh)},

volume = {12},

number = {12},

pages = {e2414714},

abstract = {Poly(ethylene oxide) (PEO)-based solid composite electrolytes suffer from poor conductivity and lithium dendrite growth, especially toward the metallic lithium metal anode. In this study, succinonitrile (SN) is incorporated into a PEO composite electrolyte to fabricate an electrode-compatible electrolyte with good electrochemical performance. The SN-doped electrolyte successfully inhibits the lithium dendrite growth and facilitates the SEI layer formation, as determined by the operando nanofocus wide-angle X-ray scattering (nWAXS), meanwhile, stably cycled over 500 h in Li/SN-PEO/Li cell. Apart from the observation of lithium dendrite, the robust SEI layer formation mechanism in the first cycle is investigated in the SN-enhanced composite electrolyte by nWAXS. The inorganic electrochemical reaction products, LiF and Li(3)N, are found to initially deposit on the electrolyte side, progressively extending toward the lithium metal anode. This growth process effectively protected the metallic lithium, inhibited electron transfer, and facilitated Li⁺ transport. The study not only demonstrates a high-performance interfacial-stable lithium metal battery with composite electrolyte but also introduces a novel strategy for real-time visualizing dendrite formation and SEI growth directing at the interface area of electrolyte and metallic lithium.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A high-frequency artificial nerve based on homogeneously integrated organic electrochemical transistors},

author = {S Wang and Y Wang and X Cai and B Wang and C Zhao and G Pan and C Harder and Y Bulut and B Zhang and S Zhang and Y Kong and K Huang and B Xie and P M\"{u}ller-Buschbaum and S V Roth and L Yang and Y Li and Y Han and G Bao and W Ma},

url = {https://doi.org/10.1038/s41928-025-01357-7},

doi = {10.1038/s41928-025-01357-7},

issn = {2520-1131},

year  = {2025},

date = {2025-03-01},

journal = {Nature Electronics},

volume = {8},

number = {3},

pages = {254-266},

abstract = {Artificial nerves that are capable of sensing, processing and memory functions at bio-realistic frequencies are of potential use in nerve repair and brain\textendashmachine interfaces. n-type organic electrochemical transistors are a possible building block for artificial nerves, as their positive-potential-triggered potentiation behaviour can mimic that of biological cells. However, the devices are limited by weak ionic and electronic transport and storage properties, which leads to poor volatile and non-volatile performance and, in particular, a slow response. We describe a high-frequency artificial nerve based on homogeneously integrated organic electrochemical transistors. We fabricate a vertical n-type organic electrochemical transistor with a gradient-intermixed bicontinuous structure that simultaneously enhances the ionic and electronic transport and the ion storage. The transistor exhibits a volatile response of 27 μs, a 100-kHz non-volatile memory frequency and a long state-retention time. Our integrated artificial nerve, which contains vertical n-type and p-type organic electrochemical transistors, offers sensing, processing and memory functions in the high-frequency domain. We also show that the artificial nerve can be integrated into animal models with compromised neural functions and that it can mimic basic conditioned reflex behaviour.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {The Role of Fluorine-Functionalized Organic Spacers for Defect Passivation and Low-Dimensional Phase Formation in 3D MAPI Perovskite Solar Cells},

author = {A Semerci and J Urieta-Mora and S Driessen and A Buyruk and R Hooijer and A Molina-Ontoria and B Alkan and S Akin and M Fanetti and H Balakrishnan and A Hartschuh and S Tao and N Mart\'{i}n and P M\"{u}ller-Buschbaum and S Emin and T Ameri},

url = {https://doi.org/10.1002/adfm.202423109},

doi = {https://doi.org/10.1002/adfm.202423109},

issn = {1616-301X},

year  = {2025},

date = {2025-02-14},

journal = {Advanced Functional Materials},

volume = {n/a},

number = {n/a},

pages = {2423109},

abstract = {Abstract Widespread application of organic-inorganic halide perovskites (OIHP) still faces a major obstacle in mitigating moisture-induced degradation. Integrating organic spacers, as defect passivation facilitators along with low-dimensional phase (LDP) formation is an effective approach to enhance the efficiency and robustness of 3D methyl ammonium lead iodide (MAPI) in photovoltaics (PV). Here, the formamidinium cation (FA+) employing 3,5-difluorobenzene-1-carboximidamidium iodide (2F), 4-(trifluoromethyl)benzene-1-carboximidamidium iodide (3F), and 2,3,4,5,6-pentafluorobenzene-1-carboximidamidium iodide (5F) organic spacers as passivation layer in 3D/LDP OIHP solar cells is utilized. Fluorine atom position and quantity in organic spacers change the optoelectronic characteristics of the perovskites, enhancing hydrophobicity, facilitating LDP formation, and augmenting dipole moments, thereby facilitating charge separation processes. PV performance analysis reveals that 3F-treated 3D/LDP devices achieve the highest efficiency of 19.22%. Experimental results and density functional theory (DFT) studies attribute the higher performance of 3F-modified devices to effective LDP formation, enhanced passivation of defect states at perovskite surfaces and grain boundaries, the highest dipole moment and lowest band gap among the evaluated spacers. The stability tests show that, after 1000 h, 3F- and 5F-modified 3D/LDP OIHP devices retain over 85% of their initial efficiency. This research opens novel avenues for designing appropriate organic spacers to attenuate defects in 3D/LDP PV devices.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Suppressed Degradation Process of PBDB-TF-T1:BTP-4F-12-Based Organic Solar Cells with Solid Additive Atums Green},

author = {Z Li and S Vagin and J Zhang and R Guo and K Sun and X Jiang and T Guan and M Schwartzkopf and B Rieger and C-Q Ma and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.4c21699},

doi = {10.1021/acsami.4c21699},

issn = {1944-8244},

year  = {2025},

date = {2025-02-12},

journal = {ACS Applied Materials \& Interfaces},

volume = {17},

number = {6},

pages = {9475-9484},

abstract = {Solid additives have garnered significant attention due to their numerous advantages over liquid additives. This study explores the potential of the green-fluorescent conjugated polymer denoted Atums Green as a solid additive in green-solvent-based PBDB-TF-T1:BTP-4F-12 solar cells. Even tiny amounts of Atums Green doping significantly improve the device performance. For the reference solar cell without any additive, we find that device degradation is not caused by chemical redox reactions but by changes in crystallinity and microstructure evolution during aging in air under illumination. Operando GIWAXS and GISAXS are used to investigate the structure evolution. We discover a four-stage degradation process for the reference cell. In general, the lattice spacing and crystallite coherence length decrease, while the domain sizes increase, which causes the loss of shirt-circuit current JSC and fill factor FF. Furthermore, a decomposition component is detected in GIWAXS and GISAXS, corresponding to the loss of the open-circuit voltage VOC. Atums Green doping effectively suppresses the evolution of crystallinity and domain sizes as well as the continuous decomposition, thereby enhancing the device stability under illumination in air. This finding reveals the kinetic degradation process of organic solar cells, establishes a correlation between the morphological properties and device performance, and further demonstrates the promising potential of Atums Green doping in organic solar cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Shape-tailored semiconductor dot-in-rods: optimizing CdS-shell growth for enhanced chiroptical properties via the rationalization of the role of temperature and time},

author = {J Hao and P Liu and Z Zhou and H Liu and W Chen and P M\"{u}ller-Buschbaum and J Cheng and K Wang and X W Sun and J-P Delville and M-H Delville},

url = {http://dx.doi.org/10.1039/D4NA01003E},

doi = {10.1039/D4NA01003E},

year  = {2025},

date = {2025-01-29},

journal = {Nanoscale Advances},

volume = {7},

number = {6},

pages = {1650-1662},

abstract = {Colloidal chemistry provides an assortment of synthetic tools for tuning the shape of semiconductor nanocrystals. To fully exploit the shape- and structure-dependent properties of semiconductor nanorods, high-precision control on growth and design is essential. However, achieving this precision is highly challenging due to the high temperatures (\>350 °C) and short reaction times (\<8 minutes) often required for these reactions. In this study, we performed the first investigation on the impact of temperature and time on the CdS-shell growth of CdSe/CdS quantum rods. Our findings demonstrate that temperature plays a pivotal role in achieving ultra-thin shell dot-in-rods, which are crucial for enhancing chiroptical properties. The two-step process proposed here explains the shell growth of CdSe/CdS dot-in-rods (DRs). It involves finely-tuned isotropic shell growth in the first stage, followed by anisotropic length growth along the [0001] rod axis in the second step. This approach has two advantages: a systematic control of the shell thickness for different aspect ratios (ARs) and batch monodispersity. These DRs, with an ultra-thin CdS shell and a high AR, after modification with l/d cysteine molecules, exhibit significant enhancement of their ligand-induced chirality, with circular dichroism (CD) g-factor values as high as 10−3.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Beta-Lactoglobulin for Water-Based and Tunable Nanostructure Templating of Printed Titania Thin Films: The Influence of pH Value and Protein Concentration},

author = {L F Huber and K Sun and M A Reus and C L Weindl and J E Heger and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1002/admi.202400929},

doi = {https://doi.org/10.1002/admi.202400929},

issn = {2196-7350},

year  = {2025},

date = {2025-01-26},

journal = {Advanced Materials Interfaces},

volume = {n/a},

number = {n/a},

pages = {2400929},

abstract = {Abstract An environmentally friendly as well as scalable synthesis route of nanostructured titania thin films is of interest for many state-of-the-art devices, from solar cells to battery materials. Beta-lactoglobulin (\ss-lg) enables water-based and tunable titania thin film templating, allowing for different domain sizes, porosities, and morphologies. When printed with a slot-die coater, the titania films can be tailored to specific applications with simple changes to the solution chemistry. Films printed at acidic pH conditions form significantly different final morphologies than films printed at a neutral pH value. The protein concentration plays a more limited role in the final nanostructure. With in situ grazing incidence small-angle/wide-angle X-ray scattering (GISAXS/GIWAXS), the structure formation is followed with an excellent time resolution during the printing process. From the GISAXS measurements, the size evolution of the titania clusters is understood, showing significant differences for different pH values. Crystal phases and corresponding crystal orientations are investigated with GIWAXS. The combination of a water-based titania synthesis with the scalable film deposition via slot die coating makes the presented results interesting for potential environmentally friendly mass production of nanostructured titania films.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Buried Interface Modulation Using Self-Assembled Monolayer and Ionic Liquid Hybrids for High-Performance Perovskite and Perovskite/CuInGaSe2 Tandem Photovoltaics},

author = {Z Feng and X Liu and T Tian and Z Zhu and R Jiang and J Li and Y Yuan and J Gong and G Gao and J Tong and Y Peng and S Bai and F Huang and X Xiao and P M\"{u}ller-Buschbaum and Y-B Cheng and T Bu},

url = {https://doi.org/10.1002/adma.202412692},

doi = {https://doi.org/10.1002/adma.202412692},

issn = {0935-9648},

year  = {2025},

date = {2025-01-06},

journal = {Advanced Materials},

volume = {n/a},

number = {n/a},

pages = {2412692},

abstract = {Abstract Effective modifications for the buried interface between self-assembled monolayers (SAMs) and perovskites are vital for the development of efficient, stable inverted perovskite solar cells (PSCs) and their tandem photovoltaics. Herein, an ionic-liquid-SAM hybrid strategy is developed to synergistically optimize the uniformity of SAMs and the crystallization of perovskites above. Specifically, an ionic liquid of 1-butyl-3-methyl-1H-imidazol-3-iumbis((trifluoromethyl)sulfonyl)amide (BMIMTFSI) is incorporated into the SAM solution, enabling reduced surface roughness, improved wettability, and a more evenly distributed surface potential of the SAM film. Leveraging this optimized substrate, a favorable growth of high-quality perovskite crystals is achieved. Furthermore, the introduced functional ions readily bond with the perovskites, effectively passivating undesirable cation or halide vacancies of the perovskite near the buried interface. Remarkably, high power conversion efficiencies (PCEs) of 25.68% and 22.53% are obtained for normal-bandgap (≈1.55 eV) and wide-bandgap (WBG) (≈1.66 eV) PSCs along with improved operational stability. Additionally, a champion PCE of 19.50% is achieved for semitransparent WBG PSCs, further delivering an impressive PCE of 28.34% for integrated four-terminal tandem photovoltaics when combined with CuInGaSe2 solar cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Hybrid-Size Quantum Dots in Hole Transport Layer Depress Dark Current Density of Short-Wave Infrared Photodetectors},

author = {S Chen and H Zhong and X Wang and G Pan and H Tang and F Fang and J Wu and W Wang and L Xu and J Tang and J Hao and K Zheng and D Wu and Z Tang and L Zhang and L Cao and P M\"{u}ller-Buschbaum and K Wang and W Chen},

url = {https://doi.org/10.1021/acsphotonics.4c01864},

doi = {10.1021/acsphotonics.4c01864},

year  = {2025},

date = {2025-01-02},

journal = {ACS Photonics},

abstract = {PbS quantum dots (QDs) are promising materials for low-cost short-wave infrared (SWIR) photodetection and imaging applications, owing to their unique optical properties and tunable bandgap. High-performance photodiodes rely on thiol-treated small PbS QDs as the hole transport layer (HTL) due to their suitable band alignment, but they face challenges such as crack formation, which increases dark currents. We develop a crack-free HTL by mixing small-size and large-size QDs. Grazing incidence small-angle X-ray scattering data confirms that the hybrid-size QD HTL is more homogeneous and denser than that made from monosize QDs. Photophysical studies show optimized charge carrier dynamics and energy transfer in the hybrid-size QDs, compared to monosize QDs. The devices based on the hybrid-size QD HTL exhibit a significantly reduced dark current density (392 nA/cm2). Additionally, they show high device performance, including a responsivity of 0.65 A/W, detectivity of 2.4 × 1012 Jones, and an external quantum efficiency of 65% in the SWIR region, paving the way for high-performance QD-based SWIR photodetectors.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Revealing the Effect of Solvent Additive Selectivity on Morphology and Formation Kinetics in Printed Non-fullerene Organic Solar Cells at Ambient Conditions},

author = {J Zhang and Z Li and X Jiang and L Xie and G Pan and A Buyan-Arivjikh and T Baier and S Tu and L Li and M Schwartzkopf and S K Vayalil and S V Roth and Z Ge and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1002/aenm.202404724},

doi = {https://doi.org/10.1002/aenm.202404724},

issn = {1614-6832},

year  = {2024},

date = {2024-12-23},

journal = {Advanced Energy Materials},

volume = {n/a},

number = {n/a},

pages = {2404724},

abstract = {Abstract Solvent additives enable the efficient modification of the morphology to improve the power conversion efficiency (PCE) of organic solar cells. However, the impact of solvent additive selectivity on the film morphology and formation kinetics is still unclarified. Herein, this work investigates two solvent additives, 1-chloronaphthalene (1-CN) and tetralin, characterized by their varying selectivity for the polymer donor (PBDB-T-2F) and the non-fullerene small molecule acceptor (BTP-C3-4F). Specifically, 1-CN exhibits superior solubility for BTP-C3-4F over PBDB-T-2F, whereas tetralin shows the opposite trend. The blend films with and without solvent additives are fabricated with the slot-die coating at ambient conditions. Both solvent additives can promote larger phase separation and increase the size of crystals of the selectively dissolved component. In situ grazing-incidence wide-angle X-ray scattering and UV?vis absorption spectra during printing unveil two distinct kinetic processes induced by 1-CN and tetralin, leading to large-sized crystals. 1-CN can prolong the liquid-solid phase separation to provide sufficient time for the BTP-C3-4F crystal growth but suppress the crystal growth of PBDB-T-2F. Tetralin can swell PBDB-T-2F and break down BTP-C3-4F crystals at the same time. Upon thermal annealing, the oversized crystals triggered by both solvent additives can be optimized to an appropriate size, resulting in an enhanced PCE.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {UV Irradiation as a Versatile Low-Temperature Strategy for Fabricating Templated Mesoporous Titania Films},

author = {G Pan and S Yin and L F Huber and Z Li and T Tian and L V Spanier and H Zhong and T Guan and C R Ehgartner and N H\"{u}sing and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1002/smll.202409856},

doi = {https://doi.org/10.1002/smll.202409856},

issn = {1613-6810},

year  = {2024},

date = {2024-12-17},

journal = {Small},

volume = {n/a},

number = {n/a},

pages = {2409856},

abstract = {Abstract Mesoporous titania thin films offer promising applications in sensors, batteries, and solar cells. The traditional soft templating methods rely on high-temperature calcination, which is energy-intensive, incompatible with thermosensitive flexible substrates, and destructive for titania structures. This work demonstrates UV irradiation as a versatile low-temperature and energy-saving alternative for mesoporous crystalline titania fabrication. Grazing incidence wide-angle X-ray scattering analysis reveals a three-stage crystallization process with increasing UV irradiation time supported by photoluminescence data. UV-irradiation-derived samples exhibit crystallinity and crystal size comparable to that of calcination. Integration with block copolymer templated sol?gel synthesis enables the creation of various morphologies, including cylindrical, ordered spherical, and hybrid structures. Characterizations via scanning electron microscopy and grazing incidence small-angle X-ray scattering confirm the homogeneity of morphology in the resulting films. The resulting films maintain similar optical properties despite morphological differences, as demonstrated by photoluminescence and UV?vis measurements. The versatility of UV irradiation extends to different titanium precursors, underscoring it as a flexible and efficient method for mesoporous titania thin film fabrication at low temperatures.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Sputter-deposited TiOx thin film as a buried interface modification layer for efficient and stable perovskite solar cells},

author = {X Jiang and J Zeng and K Sun and Z Li and Z Xu and G Pan and R Guo and S Liang and Y Bulut and B Sochor and M Schwartzkopf and K A Reck and T Strunskus and F Faupel and S V Roth and B Xu and P M\"{u}ller-Buschbaum},

url = {https://www.sciencedirect.com/science/article/pii/S2211285524011121},

doi = {https://doi.org/10.1016/j.nanoen.2024.110360},

issn = {2211-2855},

year  = {2024},

date = {2024-12-15},

journal = {Nano Energy},

volume = {132},

pages = {110360},

abstract = {Despite perovskite solar cells (PSCs) based on a SnO2 hole-blocking layer (HBL) are achieving excellent performance, the non-perfect buried interface between the SnO2 HBL and the perovskite layer is still an obstacle in achieving further improvement in power conversion efficiency (PCE) and stability. The poor morphology with numerous defects and the energy level mismatch at the buried interface constrain the open circuit voltage and cause instability. Herein, a sputter-deposited TiOx thin film is used as a buried interface modification layer to address the aforementioned issues. Utilizing in situ grazing-incidence small-angle X-ray scattering (GISAXS) during the sputter deposition, we monitor and unveil the growth process of the TiOx thin film, identifying a 10 nm thickness optimum. The defects at the buried interface are passivated through tuning the growth, leading to a suppressed non-radiative recombination and improved PCE (from 22.19 % to 23.93 %). The evolution of the device performance and the degradation process of PSCs using operando grazing-incidence wide-angle X-ray scattering (GIWAXS) under the protocol ISOS-L-1I explains the enhanced stability introduced by the buried interface modification via a sputter-deposited TiOx thin layer. The perovskite decomposition process and the detrimental formation of PbI2 are both slowed down by the TiOx thin layer.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Electrostatic Tailoring of Freestanding Polymeric Films for Multifunctional Thermoelectrics, Hydrogels, and Actuators},

author = {S Tu and T Tian and J Zhang and S Liang and G Pan and X Ma and L Liu and R A Fischer and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsnano.4c12502},

doi = {10.1021/acsnano.4c12502},

issn = {1936-0851},

year  = {2024},

date = {2024-12-09},

journal = {ACS Nano},

abstract = {Organic conducting polymer poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) has garnered enormous attention in organic electronics due to its low-cost solution processability, highly tunable conductivity, superior mechanical flexibility, and good biocompatibility together with excellent atmospheric stability. Nevertheless, limited electrical properties and unfavorable water instability of pristine PEDOT:PSS film impede its further implementation in a broad spectrum of practical applications. In this work, the successful tailoring of the intrinsic electrostatic interaction within PEDOT:PSS and consequent optimized electrical properties are enabled by a simple yet effective ionic salt post-treatment strategy. The choice of zinc di[bis(trifluoromethylsulfonyl)imide] (Zn(TFSI)2) not only endows the post-treated PEDOT:PSS film with high electrical properties but also other compelling characteristics, including superior water stability, excellent mechanical flexibility, and fast humidity responsiveness. Multidimensional characterizations are conducted to gain in-depth insights into the mechanisms underlying such improved performance, ranging from intermolecular interactions, polymer conformations, and doping levels to microstructural characteristics. Benefiting from these versatile properties, the as-prepared freestanding Zn(TFSI)2-post-treated PEDOT:PSS films can serve as promising candidates for high-performance polymeric materials integrated into multifunctional flexible electronics, including thermoelectric power generators, conductive hydrogels, and humidity-responsive actuators. This study demonstrates a facile methodology for the exploration of multifunctional conducting polymers, whose implications can extend across a wide range of next-generation wearable devices, bioelectronics, and soft robotics.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Ion-Transport Kinetics and Interface Stability Augmentation of Zinc Anodes Based on Fluorinated Covalent Organic Framework Thin Films},

author = {D Lei and W Shang and L Cheng and Poonam and W Kaiser and P Banerjee and S Tu and O Henrotte and J Zhang and A Gagliardi and J Jinschek and E Cort\'{e}s and P M\"{u}ller-Buschbaum and A S Bandarenka and M Z Hussain and R A Fischer},

url = {https://doi.org/10.1002/aenm.202403030},

doi = {https://doi.org/10.1002/aenm.202403030},

issn = {1614-6832},

year  = {2024},

date = {2024-12-01},

journal = {Advanced Energy Materials},

volume = {14},

number = {46},

pages = {2403030},

abstract = {Abstract Zinc (Zn) emerges as an ideal anode for aqueous-based energy storage devices because of its safety, non-toxicity, and cost-effectiveness. However, the reversibility of zinc anodes is constrained by unchecked dendrite proliferation and parasitic side reactions. To minimize these adverse effects, a highly oriented, crystalline 2D porous fluorinated covalent organic framework (denoted as TpBD-2F) thin film is in situ synthesized on the Zn anode as a protective layer. The zincophilic and hydrophobic TpBD-2F provides numerous 1D fluorinated nanochannels, which facilitate the hopping/transfer of Zn2+ and repel H2O infiltration, thus regulating Zn2+ flux and inhibiting interfacial corrosion. The resulting TpBD-2F protective film enabled stable plating/stripping in symmetric cells for over 1200 h at 2 mA cm?2. Furthermore, assembled full cells (Zn-ion capacitors) deliver an ultra-long cycling life of over 100 000 cycles at a current density of 5 A g?1, outperforming nearly all reported porous crystalline materials.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Drop-Cast Hybrid Poly(styrene)-b-Poly(ethylene oxide) Metal Salt Films: Solvent Evaporation and Crystallinity-Dependent Evolution of Film Morphology},

author = {Y Li and N Li and S Tu and Y Alon and Z Li and M Betker and D Sun and A Kurmanbay and W Chen and S Liang and S Shi and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1002/smll.202406279},

doi = {https://doi.org/10.1002/smll.202406279},

issn = {1613-6810},

year  = {2024},

date = {2024-12-01},

journal = {Small},

volume = {20},

number = {51},

pages = {2406279},

abstract = {Abstract Morphology templates of solution?based diblock copolymer (DBC) films with loading metal salts are widely applied in photocatalysts, photovoltaics, and sensors due to their adjustable characteristics based on surface (de?)wetting and microphase separation. The present work investigates the morphologies of drop?cast hybrid films based on poly(styrene)?b?poly(ethylene oxide) (PS?b?PEO) and the metal salts titanium isopropoxide (TTIP) and zinc acetate dehydrate (ZAD) in comparison to the pure DBC. By utilizing scanning electron microscopy, grazing?incidence small? and wide?angle X-ray scattering, and differential scanning calorimetry, we find that the resulting film morphologies depend not only on the presence of metal salts but also on solvent evaporation and crystalline formation. At 20 °C, additional TTIP and ZAD in the polymer template cause the morphology to change from packed globular structures to separated wormlike structures attributed to the changed polymer environment. Furthermore, additional tetrahydrofuran causes irregular structures at the precursor film part and the overlapped wormlike structures to transition into close?packed globular structures at the cap film parts of the pure DBC. In contrast, at 50 °C, the globular structures transit to fingerprint patterns due to the thermal behavior of the crystallizable PEO blocks, and the metal salt additives suppress crystalline structure formation in the PEO domains.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Deciphering Structure and Charge Carrier Behavior in Reduced-Dimensional Perovskites},

author = {K Sun and R Guo and S Liu and D Guo and X Jiang and L F Huber and Y Liang and M A Reus and Z Li and T Guan and J Zhou and M Schwartzkopf and S D Stranks and F Deschler and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1002/adfm.202411153},

doi = {https://doi.org/10.1002/adfm.202411153},

issn = {1616-301X},

year  = {2024},

date = {2024-12-01},

journal = {Advanced Functional Materials},

volume = {34},

number = {52},

pages = {2411153},

abstract = {Abstract Reduced-dimensional perovskites (RDPs) have advanced perovskite optoelectronic devices due to their tunable energy landscape, structure, and orientation. However, the origin of structural and photophysical property changes when moving from low-dimensional to high-dimensional RDPs remains to be understood. This study systematically reveals structural and photophysical properties of slot-die-coated Dion-Jacobson (DJ) and Ruddlesden-Popper (RP) RDPs with different dimensionalities. RP RDPs with lower dimensionality (n = 2) exhibit a dominant n = 2 phase, preferential out-of-plane orientation, and longer charge carrier lifetime compared with DJ RDPs. In addition, the formation kinetics of RDPs with higher dimensionality (n = 4) are unraveled by in situ X-ray scattering, showing the favorable formation of the lower-n phase in RP RDPs. The formation of these lower-n phases is thermodynamically and stoichiometrically favored, while these phases are likely in the form of an ?intermediate phase? which bridges the 3D-like and lower-n phases in DJ RDPs. DJ RDPs with higher dimensionality demonstrate comparable phase purity, preferential orientation, spatially vertical phase homogeneity, and longer charge carrier lifetime. As such, DJ-based perovskite solar cells (PSCs) (n = 4) demonstrate better photostability under operational conditions than RP-based PSCs. Thus, the work paves the way for the utilization of RDPs to upscale PSCs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Regulating phase homogeneity by self-assembled molecules for enhanced efficiency and stability of inverted perovskite solar cells},

author = {X Wang and J Li and R Guo and X Yin and R Luo and D Guo and K Ji and L Dai and H Liang and X Jia and J Chen and Z Jia and Z Shi and S Liu and Y Wang and Q Zhou and T Wang and G Pan and P M\"{u}ller-Buschbaum and S D Stranks and Y Hou},

url = {https://doi.org/10.1038/s41566-024-01531-x},

doi = {10.1038/s41566-024-01531-x},

issn = {1749-4893},

year  = {2024},

date = {2024-12-01},

journal = {Nature Photonics},

volume = {18},

number = {12},

pages = {1269-1275},

abstract = {Heterogeneity in transporting interfaces and perovskites poses a substantial challenge in improving the efficiency of perovskite solar cells from small to large scales, a key barrier to their commercial use. Here we find that the amorphous phases of self-assembling molecules (SAMs) can realize a more homogeneous perovskite growth. Hyperspectral analysis confirms a narrower and blueshifted photoluminescence peak distribution in perovskite/amorphous SAMs. Additionally, fluence-dependent time-resolved photoluminescence reveals a reduced trap-assisted recombination rate of 0.5 × 106 s−1 in amorphous-SAM-based perovskite films. This improvement translates to p\textendashi\textendashn structured perovskite solar cells achieving an efficiency of 25.20% (certified at 24.35%) over a one-square-centimetre area. These cells maintain nearly 100% efficiency after 600 h of 1-sun maximum power point tracking under the ISOS-L-1 protocol, and retain 90% of their initial efficiency after 1,000 h, as evaluated by the ISOS-T-2 protocol.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Converting Perovskite Nanocrystals to PbS Quantum Dots Toward Short-Wave Infrared Photodetectors},

author = {W Zhang and F Fang and H Zhong and L Huang and H Tang and X Chen and J Hao and L Zhang and L Cao and J Tang and K Zheng and P M\"{u}ller-Buschbaum and W Chen},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.202402740},

doi = {https://doi.org/10.1002/adom.202402740},

issn = {2195-1071},

year  = {2024},

date = {2024-11-29},

journal = {Advanced Optical Materials},

volume = {n/a},

number = {n/a},

pages = {2402740},

abstract = {Abstract PbS quantum dots (QDs) are particularly promising in low-cost short-wave infrared (SWIR) photodetection and imaging applications. Herein, a novel method is introduced defined as the perovskite conversion method (PCM) fabricating PbS QDs by using perovskite nanocrystals (PeNCs) as the lead precursor. The elemental substitution mechanism for PbS QDs from PeNCs is proposed, and it is confirmed that PCM-QDs are exhibiting a smaller trap density due to a natural perovskite passivated surface condition compared to QDs prepared via conventional hot injection method (HIM). Grazing-incidence small-angle X-ray scattering (GISAXS) results indicate that a short-range disorder of the QDs can lead to a long-range disorder configuration in the inner structure of PCM-QD superlattice, which leads to a compact configuration in the QD solid film facilitating charge carrier transport in devices. In a photoconductor-typed SWIR photodetector (PD) comparison, PCM-QD PDs exhibit a high responsivity of 468 A W−1 and detectivities of 2.1 × 1012 Jones, which are almost three times higher than the values in HIM-QDs PDs. Moreover, PCM-QD PDs further show a higher response speed and one magnitude order higher loss frequency than PCM-QD PDs. PCM is promising in the fabrication of high-quality QDs for advanced optoelectronic applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Homogeneous coverage of the low-dimensional perovskite passivation layer for formamidinium\textendashcaesium perovskite solar modules},

author = {J Li and C Jin and R Jiang and J Su and T Tian and C Yin and J Meng and Z Kou and S Bai and P M\"{u}ller-Buschbaum and F Huang and L Mai and Y-B Cheng and T Bu},

url = {https://doi.org/10.1038/s41560-024-01667-8},

doi = {10.1038/s41560-024-01667-8},

issn = {2058-7546},

year  = {2024},

date = {2024-11-12},

journal = {Nature Energy},

abstract = {The formation of a homogeneous passivation layer based on phase-pure two-dimensional (2D) perovskites is a challenge for perovskite solar cells, especially when upscaling the devices to modules. Here we reveal a chain-length-dependent and halide-related phase separation problem of 2D perovskite growing on top of three-dimensional perovskites. We demonstrate that a homogeneous 2D perovskite passivation layer can be formed upon treatment of the perovskite layer with formamidinium bromide in long-chain ( \>10) alkylamine ligand salts. We achieve champion active-area efficiencies of 25.61%, 24.62% and 23.60% for antisolvent-free processed small- (0.14 cm2) and large-size (1.04 cm2) devices and mini-modules (13.44 cm2), respectively. This passivation strategy is compatible with printing technology, enabling champion aperture-area efficiencies of 18.90% and 17.59% for fully slot-die printed large solar modules with areas of 310 cm2 and 802 cm2, respectively, demonstrating the feasibility of the upscaling manufacturing.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A small amount of sodium difluoro(oxalate)borate additive induces anion-derived interphases for sodium-ion batteries},

author = {Q Qiu and T Zheng and L Huang and T Xu and L Pan and W Sun and H Tian and W Zhang and Q Yu and Y Liang and Y Yan and J Yuan and P M\"{u}ller-Buschbaum and L Xia},

url = {https://www.sciencedirect.com/science/article/pii/S2405829724006846},

doi = {https://doi.org/10.1016/j.ensm.2024.103858},

issn = {2405-8297},

year  = {2024},

date = {2024-11-01},

journal = {Energy Storage Materials},

volume = {73},

pages = {103858},

abstract = {In sodium-ion batteries, the properties of the electrode-electrolyte interphases (EEIs) layer formed on the electrode surface, dominate the Na+ de-solvation process and Na+ (de)intercalation behavior, thereby influencing the battery performance. Currently, both high-concentration electrolytes and localized high-concentration electrolytes facilitate the formation of anion-derived and inorganic-rich interfacial chemistry, leading to excellent electrochemical performance. However, the expensive lithium salt and/or fluorinated diluent imposes a major concern. Herein, a small amount additive of 0.5 wt% sodium difluoro(oxalate)borate (NaDFOB) with the electron-rich property is introduced into 1 mol L\textendash1 NaClO4/propylene carbonate electrolyte to construct a robust inorganic-rich EEIs via an anion preferential adsorption-decomposition mechanism. Theoretical calculations and experimental results reveal that the DFOB\textendash anion has a lower adsorption energy than the other components, which will be preferentially adsorbed in the inner Helmholtz plane (IHP) with the closer proximity to two electrode surfaces and thus being firstly decomposed to form inorganic-rich interphases, thereby effectively suppressing side reactions. Consequently, both Na-ion half-cells and full-cells using this electrolyte deliver excellent cycling performance. This strategy that regulates the interphase chemistry on the electrode surface through an anion preferential adsorption-decomposition strategy, provides a promising avenue for developing long-term cycling sodium-ion batteries.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Multipoint Anionic Bridge: Asymmetric Solvation Structure Improves the Stability of Lithium-Ion Batteries},

author = {T Zheng and T Xu and J Xiong and W Xie and M Wu and Y Yu and Z Xu and Y Liang and C Liao and X Dong and Y Xia and Y J Cheng and Y Xia and P M\"{u}ller-Buschbaum},

doi = {10.1002/advs.202410329},

issn = {2198-3844},

year  = {2024},

date = {2024-10-30},

journal = {Adv Sci (Weinh)},

pages = {e2410329},

abstract = {In this study, a novel concept of multipoint anionic bridge (MAB) is proposed and proved, which utilizes anions with different sites to connect with the asymmetric solvation structure (ASS). Compared to usual solvation structures, this study utilizes the multifunctional groups of difluoro(oxalate)borate anion (ODFB(-)), which can connect with Li(+). By tailoring the concentration, the anion serves as a bridge between different solvated structures. The electrolyte is investigated through in situ techniques and simulations to draw correlations between different solvation structures and reaction pathways. The proposed design demonstrates remarkable high-temperature performance on both the anode and cathode sides, enabling stable cycling of LCO||graphite (0.5 Ah, 1.0 C) pouch cell for over 200 cycles at 80 °C and facilitating Li||MCMB and Li||LFP cells to deliver stable performance for 200 cycles at 100 °C. This work paves the way for the development of high-performance electrolyte systems by designing and using new multipoint anions to construct ASSs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {From generation to collection \textendash impact of deposition temperature on charge carrier dynamics of high-performance vacuum-processed organic solar cells},

author = {R A Pacalaj and Y Dong and I Ramirez and R C I Mackenzie and S M Hosseini and E Bittrich and J E Heger and P Kaienburg and S Mukherjee and J Wu and M Riede and H Ade and P M\"{u}ller-Buschbaum and M Pfeiffer and J R Durrant},

url = {http://dx.doi.org/10.1039/D4EE03623A},

doi = {10.1039/D4EE03623A},

issn = {1754-5692},

year  = {2024},

date = {2024-10-23},

journal = {Energy \& Environmental Science},

volume = {17},

number = {23},

pages = {9215-9232},

abstract = {Vacuum-processed organic solar cells (VP-OSCs) possess many advantages for scalability. However, as the academic community focusses on high performing solution-processed OSCs, detailed studies about the relation between morphology and device characteristics in VP-OSCs are rare. Here, we present a study on a model donor/fullerene VP-OSC system deposited at different substrate temperatures. Substrate heating results in increases in current density and fill factor (FF). Changes in morphology are characterised by grazing-incidence wide-angle scattering (GIWAXS) and resonant soft X-ray scattering (RSoXS). The increase in the degree of crystallinity and preferential orientation of the donor molecule in heated samples results in enhanced absorption increasing current density. The exciton and charge separation efficiency were studied by transient absorption and photoluminescence quenching and only showed minor differences. To study the FF differences, charge transport and non-geminate recombination are studied by optoelectronic measurements and device simulations. The charge carrier kinetics are governed by a large density of trap states. While the energetic disorder and non-geminate recombination under open circuit conditions remain largely unchanged, the increased effective mobility and lower transport disorder observed in photocurrent transients explain the increased collection efficiency for heated devices. We relate this to the increased donor phase purity. Our results suggest that charge recombination and transport are governed by different aspects of disorder related to amorphous and crystalline donor phases. Quantitative comparison with high FF solution-processed OSCs reveals that the low mobility limits FF. Finally, drift-diffusion simulations give an outlook for possible performance increases through further optimisation of the deposition control.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A chronicle of titanium niobium oxide materials for high‐performance lithium‐ion batteries: From laboratory to industry},

author = {C Peng and S Liang and Y Yu and L Cao and Y Chao and X Liu and K Guo and P M\"{u}ller-Buschbaum and Y-J Cheng and C Wang},

doi = {10.1002/cnl2.177},

year  = {2024},

date = {2024-10-21},

journal = {Carbon Neutralization},

volume = {3},

abstract = {Titanium niobium oxide (TiNb x O 2 + 2.5 x ) is emerging as a promising electrode material for rechargeable lithium‐ion batteries (LIBs) due to its exceptional safety characteristics, high electrochemical properties (e.g., cycling stability and rate performance), and eco‐friendliness. However, several intrinsic critical drawbacks, such as relatively low electrical conductivity, significantly hinder its practical applications. Developing reliable strategies is crucial to accelerating the practical use of TiNb x O 2 + 2.5 x ‐based materials in LIBs, especially high‐power LIBs. Here, we provide a chronicle review of the research progress on TiNb x O 2 + 2.5 x ‐based anodes from the early 1950s to the present, which is classified into early stage (before 2008), emerging stage (2008\textendash2012), explosive stage (2013\textendash2017), commercialization (2018), steady development (2018\textendash2022), and new breakthrough stage (since 2022). In each stage, the advancements in the fundamental science and application of the TiNb x O 2 + 2.5 x ‐based anodes are reviewed, and the corresponding developing trends of TiNb x O 2 + 2.5 x ‐based anodes are summarized. Moreover, several future research directions to propel the practical use of TiNb x O 2 + 2.5 x anodes are suggested based on reviewing the history. This review is expected to pave the way for developing the fabrication and application of high‐performance TiNb x O 2 + 2.5 x ‐based anodes for LIBs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Micrometer-Thin Nanocellulose Foils for 3D Organic Electronics},

author = {M Betker and T Erichlandwehr and B Sochor and E Erbes and A Kurmanbay and Y Alon and Y Li and I Fernandez-Cuesta and P M\"{u}ller-Buschbaum and S A Techert and L D S\"{o}derberg and S V Roth},

url = {https://doi.org/10.1002/adfm.202403952},

doi = {https://doi.org/10.1002/adfm.202403952},

issn = {1616-301X},

year  = {2024},

date = {2024-10-01},

journal = {Advanced Functional Materials},

volume = {34},

number = {40},

pages = {2403952},

abstract = {Abstract Cellulose is a natural polymer with great properties such as high optical transparency and mechanical strength, flexibility, and biodegradability. Hence, cellulose-based foils are suitable for the replacement of synthetic polymers as substrate materials in organic electronics. This article reports the fabrication of ultrathin, free-standing cellulose foils by spraying aqueous 2,2,6,6-tetramethylpiperidine-1-oxyl-nanocellulose (TEMPO) fibrils ink layer-by-layer on a hot substrate using a movable spray nozzle. The resulting foils are only 2 ± 1 µm in thickness with an average basis weight of 1.9 g m?2, which ranges in the same scale as the world's thinnest paper. The suitability of these ultra-thin nanocellulose foils as a sustainable substrate material for organic electronic applications is demonstrated by testing the foils resistance against organic solvents. Furthermore, silver nanowires (AgNWs) and the blend poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) are integrated into the foils, and the foils are molded into 3D paper structures in order to create conductive, paper-based building blocks for organic electronics.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Stabilizing efficient wide-bandgap perovskite in perovskite-organic tandem solar cells},

author = {X Guo and Z Jia and S Liu and R Guo and F Jiang and Y Shi and Z Dong and R Luo and Y-D Wang and Z Shi and J Li and J Chen and L K Lee and P M\"{u}ller-Buschbaum and D S Ginger and D J Paterson and Y Hou},

url = {https://doi.org/10.1016/j.joule.2024.06.009},

doi = {10.1016/j.joule.2024.06.009},

issn = {2542-4785},

year  = {2024},

date = {2024-09-18},

journal = {Joule},

volume = {8},

number = {9},

pages = {2554-2569},

abstract = {Iodide and bromide integration facilitate bandgap tunability in wide-bandgap perovskites, yet high concentrations of bromide lead to halide phase segregation, adversely affecting the efficiency and stability of solar cell devices. In this work, 2-amino-4,5-imidazoledicarbonitrile (AIDCN), with highly polarized charge distribution and compact molecular configuration, is incorporated into a 1.86 eV wide-bandgap perovskite to effectively suppress photoinduced iodine escape and phase segregation. Hyperspectral photoluminescence microscopy reveals that AIDCN mitigates phase segregation under continuous laser exposure. Concurrent in situ grazing-incidence wide-angle X-ray scattering and X-ray fluorescence measurements further validate suppressed iodine escape, evidenced by a notable slowing down of lattice shrinkage and a well-maintained overall chemical composition of the perovskite under continuous illumination. Applying this approach, we achieve a power conversion efficiency (PCE) of 18.52% in 1.86 eV wide-bandgap perovskite solar cells. By integrating this perovskite subcell with the PM6:BTP-eC9 organic subcell, the tandem attains a maximum PCE of 25.13%, with a certified stabilized PCE of 23.40%.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Achieving the Inhibition of Aluminum Corrosion by Dual-Salt Electrolytes for Sodium-Ion Batteries},

author = {L Huang and Q Qiu and M Yang and H Li and J Zhu and W Zhang and S Wang and L Xia and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.4c10970},

doi = {10.1021/acsami.4c10970},

issn = {1944-8244},

year  = {2024},

date = {2024-09-04},

journal = {ACS Applied Materials \& Interfaces},

volume = {16},

number = {35},

pages = {46392-46400},

abstract = {Sodium bis(fluorosulfonyl)imide (NaFSI) electrolytes are renowned for their superior physicochemical and electrochemical properties, making them ideal for high-performance sodium-ion batteries (SIBs). However, severe oxidative dissolution of aluminum current collectors (commonly known as Al corrosion) in NaFSI-based electrolytes occurs at high potentials. To address this challenge, aiming to understand the Al corrosion mechanism and develop strategies to inhibit corrosion, we propose dual-salt electrolytes using 0.8 mol L\textendash1 (M) NaFSI and 0.2 M of a second fluorine-containing sodium salt dissolved in EC/PC solutions (1:1, v/v) to construct an insoluble deposits layer on the Al. Dual-salt electrolytes adopting a second sodium salt capable of passivating the Al collector have been extensively investigated through various techniques, such as cyclic voltammetry, scanning electron microscopy, chronoamperometry, X-ray photoelectron spectroscopy, and charge\textendashdischarge tests. Our findings demonstrate that introducing sodium difluoro(oxalato)borate (NaDFOB) into the NaFSI electrolytes inhibits Al corrosion, which is attributed to the formation of insoluble deposits of Al\textendashF (AlF3) and B\textendashF containing polymers. Moreover, the capacity retention of Na||Na3V2(PO4)3 (NVP) cells using the NaFSI-NaDFOB dual-salt electrolyte reaches 99.2% along with a Coulombic efficiency over 99.3% at a 1 C rate after 200 cycles. This research provides a practical solution for passivating Al collectors in SIBs with NaFSI electrolytes and promotes the development of sodium batteries with long calendar lifetimes.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Factors Shaping the Morphology in Sol-Gel Derived Mesoporous Zinc Titanate Films: Unveiling the Role of Precursor Competition and Concentration},

author = {Y Li and N Li and C Harder and S Yin and Y Bulut and A Vagias and P M Schneider and W Chen and S V Roth and A S Bandarenka and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/admi.202400215},

doi = {https://doi.org/10.1002/admi.202400215},

issn = {2196-7350},

year  = {2024},

date = {2024-09-04},

journal = {Advanced Materials Interfaces},

volume = {11},

number = {34},

pages = {2400215},

abstract = {Abstract Zinc titanate films with mesoporous structures have widespread applications ranging from sensors to supercapacitors and bio-devices owing to their photoelectric properties and specific surface area. The present work investigates the morphology of mesoporous zinc titanate films obtained by calcination of hybrid thin films containing polymer templates and precursor mixtures of zinc acetate dihydrate (ZAD) and titanium isopropoxide (TTIP). ZnO and TiO2 films are fabricated for reference. The influences of hydrochloric acid contents (HCl), the ratios of ZAD and TTIP, and the solution concentrations on the film morphologies are studied. The amphiphilic diblock copolymer, polystyrene-block-polyethylene oxide (PS-b-PEO), plays the role of a structure directing template, as it self-assembles into micelles in a solvent-acid mixture of N, N-dimethylformamide (DMF) and HCl. Thin films are prepared with spin-coating and subsequent calcination. Adjusting the ratio of TTIP and ZAD leads to the structure evolution from order to disorder in a film. It depends on the hydrolysis and condensation processes of the precursors, providing different time-to-growth processes to control the film morphologies. An increase in solution concentration enhances the surface coverage. As probed with grazing-incidence small-angle X-ray scattering, the inner structures are larger than the surface structures seen in scanning electron microscopy.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Ammonium Sulfate to Modulate Crystallization for High-Performance Rigid and Flexible Perovskite Solar Cells},

author = {Y Zou and Q Song and J Zhou and S Yin and Y Li and F C Apfelbeck and T Zheng and M-K Fung and C Mu and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1002/smll.202401456},

doi = {https://doi.org/10.1002/smll.202401456},

issn = {1613-6810},

year  = {2024},

date = {2024-09-01},

journal = {Small},

volume = {20},

number = {36},

pages = {2401456},

abstract = {Abstract Perovskite solar cells (PSCs) are attracting widespread research and attention as highly promising candidates in the field of electronic photovoltaics owing to their exceptional power conversion efficiency (PCE). However, rigid or flexible PSCs still face challenges in preparing full-coverage and low-defect perovskite films, as well as achieving highly reproducible and highly stable devices. Herein, a multifunctional additive 2-aminoethyl hydrogen sulfate (AES) is designed to regulate the film crystallization and thereby form flat and pinhole-free perovskite films. It is found that the introduction of AES can effectively passivate defects, restrain charge carrier recombination, and then achieve a higher fill factor. As seen with grazing incidence wide-angle X-ray scattering (GIWAXS), this approach does not affect the crystal orientation distribution. It is observed that AES addition shows a universality across different perovskite components since the PCE is improved up to 20.7% for FA0.97MA0.03Pb(I0.97Br0.03)3-AES, 22.85% for Cs0.05FA0.95PbI3-AES, 22.23% for FAPbI2.7Br0.3-AES, and 23.32% for FAPI-AES rigid devices. Remarkably, the non-encapsulated flexible Cs0.05 (FA0.85MA0.15)0.95Pb(I0.85Br0.15)3 device with AES additive delivers a PCE of 20.1% and maintains over 97% of its initial efficiency under ambient conditions (25 ± 5% relative humidity) over 2280 h of aging.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Suppressed Degradation Process of Green-Solvent Based Organic Solar Cells Through ZnO Modification With Sulfhydryl Derivatives},

author = {Z Li and Y Li and J Zhang and R Guo and K Sun and X Jiang and P Wang and S Tu and M Schwartzkopf and Z Li and C-Q Ma and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202402920},

doi = {https://doi.org/10.1002/aenm.202402920},

issn = {1614-6832},

year  = {2024},

date = {2024-08-29},

journal = {Advanced Energy Materials},

volume = {n/a},

number = {n/a},

pages = {2402920},

abstract = {Abstract The interface of organic solar cells plays a crucial role in device performance and stability. Several investigations demonstrated that the interface will affect the morphology and microstructure of the active layer, which is important for device performance. Here, several mercaptan derivatives are explored in green-solvent based organic solar cells (PBDB-TF-T1: BTP-4F-12) as effective stabilization modifiers on ZnO. Operando grazing-incidence wide/small-angle X-ray scattering (GIWAXS/GISAXS) provides a deep understanding of the degradation process during operation. The degradation process is driven by a compression of the molecule stacking as well as a decrease in the donor crystallinity, besides the known decomposition of the acceptor at the interface. Solar cell degradation comprises three stages, where an unexpected component from the acceptor appears in the second stage, simultaneously with a shapely shrinking micro-structure. Furthermore, the interface modifier pentaerythritol tetrakis(3-mercapto-propionate) (PETMP) stabilizes the crystallinity of the donor as well as suppresses the decomposition of the acceptor, thus improving the device stability. The modification effect is caused by the interaction between Zn and S from the sulfhydryl groups of the mercaptan derivatives. Thus, studies of changes in the active layer morphology extend the knowledge from ex situ characterizations, broadening the understanding of the degradation mechanisms.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Synergic Surface Modifications of PbS Quantum Dots by Sodium Acetate in Solid-State Ligand Exchange toward Short-Wave Infrared Photodetectors},

author = {X Wang and Z Song and H Tang and Y Li and H Zhong and J Wu and W Wang and S Chen and W Zhang and F Fang and J Hao and D Wu and P M\"{u}ller-Buschbaum and L Cao and Z Tang and J Tang and L Zhang and K Wang and W Chen},

url = {https://doi.org/10.1021/acsami.4c05201},

doi = {10.1021/acsami.4c05201},

issn = {1944-8244},

year  = {2024},

date = {2024-08-21},

journal = {ACS Applied Materials \& Interfaces},

volume = {16},

number = {33},

pages = {44164-44173},

abstract = {PbS quantum dots (QDs) are promising for short-wave infrared (SWIR) photodetection and imaging. Solid-state ligand exchange (SSLE) is a low-fabrication-threshold QD solid fabrication method. However, QD treatment by SSLE remains challenging in seeking refined surface passivation to achieve the desired device performance. This work investigates using NaAc in the ligand exchange process to enhance the film morphology and electronic coupling configuration of QD solids. By implementing various film and photodetector device characterization studies, we confirm that adding NaAc with a prominent adding ratio of 20 wt % NaAc with tetrabutylammonium iodide (TBAI) in the SSLE leads to an improved film morphology, reduced surface roughness, and decreased trap states in the QD solid films. Moreover, compared to the devices without NaAc treatment, those fabricated with NaAc-treated QD solids exhibit an enhanced performance, including lower dark current density (\<100 nA/cm2), faster response speed, higher responsivity, detectivity, and external quantum efficiency (EQE reaching 25%). The discoveries can be insightful in developing efficient, low-cost, and low-fabrication-threshold QD SWIR detection and imager applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Multifunctional Umbrella: In Situ Interface Film Forming on the High-Voltage LiCoO(2) Cathode by a Tiny Amount of Nanoporous Polymer Additives for High-Energy-Density Li-Ion Batteries},

author = {R Qi and M Yang and T Zheng and X Liu and Y Xia and Y J Cheng and P M\"{u}ller-Buschbaum},

doi = {10.1002/smll.202312087},

issn = {1613-6810},

year  = {2024},

date = {2024-08-20},

journal = {Small},

volume = {20},

number = {31},

pages = {e2312087},

abstract = {The LiCoO(2) (LCO) cathode is foreseen for extensive commercial applications owing to its high specific capacity and stability. Therefore, there is considerable interest in further enhancing its specific capacity by increasing the charging voltage. However, single-crystal LCO suffers from a significant capacity degradation when charged to 4.5 V due to the irreversible phase transition and unstable structure. Herein, an ultra-small amount (0.5% wt. in the electrode) of multi-functional PIM-1 (a polymer with intrinsic microporosity) additive is utilized to prepare a kind of binder-free electrode. PIM-1 modulates the solvation structure of LiPF(6) due to its unique structure, which helps to form a stable, robust, and inorganic-rich cathod-eelectrolyte interphase (CEI) film on the surface of LCO at a high voltage of 4.5 V. This reduces the irreversible phase transition of LCO, thereby enhancing the cyclic stability and improving the rate performance, providing new perspectives for the electrodes fabrication and improving LCO-based high-energy-density cathodes.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Influence of the Polymer Binder Composition on the Charge Transfer Resistance, Morphology, and Crystallinity of LiFePO4 Electrodes Revealed by Electrochemical Impedance Spectroscopy and Grazing Incidence Small- and Wide-Angle X-ray Scattering},

author = {F C Apfelbeck and J E Heger and T Zheng and T Guan and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/smsc.202400154},

doi = {https://doi.org/10.1002/smsc.202400154},

year  = {2024},

date = {2024-08-10},

journal = {Small Science},

volume = {4},

number = {10},

pages = {2400154},

abstract = {Electrode materials for application in lithium-ion batteries are commonly probed by X-ray diffraction (XRD) to investigate their crystalline structure. Grazing incidence wide-angle X-ray scattering (GIWAXS) is an extension to XRD since in-plane structures are also accessible. Additionally, with grazing incidence small-angle X-ray scattering (GISAXS), morphological information on the nanoscale can be revealed. In this work, the nanostructure of battery electrodes, which consist of lithium iron phosphate (LiFePO4) as active material, carbon black (CB) as conducting agent, and the polymeric binders polyvinylidenefluoride (PVDF) and poly((trifluoromethane) sulfonimide lithium styrene) (PSTFSILi) is studied by performing GISAXS and GIWAXS. The chemical nature of the binder is tuned by blending PVDF and PSTFSILi. Specifically, a series of LiFePO4 electrodes with polymer blends of the common, non-conducting PVDF and the single-ion conducting PSTFSILi with different weight ratios as binders is investigated to understand the influence of the binder on the structure of the electrode in detail. Scanning electron microscopy (SEM) and electrochemical impedance spectroscopy (EIS) complement these studies to correlate the morphology and structure with the electrochemical behavior. It is found that LiFePO4 crystallites do not exhibit any preferred orientation with respect to the substrate, irrespective of the binder composition, but their size depends on the binder composition.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Nanometer-Thick ITIC Bulk Heterojunction Films as Non-Fullerene Acceptors in Organic Solar Cells},

author = {T-Y Huang and A P Le Brun and B Sochor and C-M Wu and Y Bulut and P M\"{u}ller-Buschbaum and S V Roth and Y-L Yang},

url = {https://doi.org/10.1021/acsanm.4c02865},

doi = {10.1021/acsanm.4c02865},

year  = {2024},

date = {2024-08-09},

journal = {ACS Applied Nano Materials},

volume = {7},

number = {15},

pages = {17588-17595},

abstract = {The nanomorphology of bulk heterojunctions (BHJs) plays a critical role in determining the performance of non-fullerene organic solar cells (OSCs). Thermal annealing is commonly used to reorganize the donor and acceptor phases within the BHJs. In this study, we investigate the vertical morphology of BHJ blend films incorporating the poly[(5,6-difluoro-2,1,3-benzothiadiazol-4,7-diyl)-alt-(3,3‴-di(2-octyldodecyl)-2,2′;5′,2″;5″,2‴-quaterthiophen-5,5‴-diyl)] (PffBT4T-2OD) polymer as the donor and 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2′,3′-d′]-s-indaceno[1,2-b:5,6-b′]dithiophene (ITIC) as the acceptor. Neutron reflectivity patterns and scattering length density profiles reveal that the surface of the BHJ films became diffuse when the annealing temperature was above 150 °C. We further find that mitigated agglomeration of PffBT4T-2OD side chains exhibits minimal impact on morphology post-annealing. Instead, ITIC molecules trigger aggregations, accompanied by interface diffusion and increased film roughness. X-ray scattering confirms a 5-fold increase in aggregated ITIC nanodomains after annealing. Our findings highlight that unstable ITIC phases dominate the BHJ morphology of thin films, leading to the thermal instability of OSCs. This study enhances our understanding of the BHJ morphology and offers insights into improving the performance of energy conversion devices.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {High-Power Impulse Magnetron Sputter Deposition of Ag on Self-Assembled Au Nanoparticle Arrays at Low-Temperature Dewetting Conditions},

author = {T Guan and S Liang and Y Kang and E Pensa and D Li and W Liang and Z Liang and Y Bulut and K A Reck and T Xiao and R Guo and J Drewes and T Strunskus and M Schwartzkopf and F Faupel and S V Roth and E Cort\'{e}s and L Jiang and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.4c10726},

doi = {10.1021/acsami.4c10726},

issn = {1944-8244},

year  = {2024},

date = {2024-07-31},

journal = {ACS Applied Materials \& Interfaces},

volume = {16},

number = {30},

pages = {40286-40296},

abstract = {Plasmons have facilitated diverse analytical applications due to the boosting signal detectability by hot spots. In practical applications, it is crucial to fabricate straightforward, large-scale, and reproducible plasmonic substrates. Dewetting treatment, via applying direct thermal annealing of metal films, has been used as a straightforward method in the fabrication of such plasmonic nanostructures. However, tailoring the evolution of the dewetting process of metal films poses considerable experimental complexities, mainly due to nanoscale structure formation. Here, we use grazing-incidence small- and wide-angle X-ray scattering for the in situ investigation of the high-power impulse magnetron sputter deposition of Ag on self-assembled Au nanoparticle arrays at low-temperature dewetting conditions. This approach allows us to examine both the direct formation of binary Au/Ag nanostructure and the consequential impact of the dewetting process on the spatial arrangement of the bimetallic nanoparticles. It is observed that the dewetting at 100 °C is sufficient to favor the establishment of a homogenized structural configuration of bimetallic nanostructures, which is beneficial for localized surface plasmon resonances (LSPRs). The fabricated metal nanostructures show potential application for the surface-enhanced Raman scattering (SERS) detection of rhodamine 6G molecules. As SERS platform, bimetallic nanostructures formed with dewetting conditions turn out to be superior to those without dewetting conditions. The method in this work is envisioned as a facile strategy for the fabrication of plasmonic nanostructures.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Hole Localization in Bulk and 2D Lead-Halide Perovskites Studied by Time-Resolved Infrared Spectroscopy},

author = {D Sandner and K Sun and A Stadlbauer and M W Heindl and Q Y Tan and M Nuber and C Soci and R Kienberger and P M\"{u}ller-Buschbaum and F Deschler and H Iglev},

url = {https://doi.org/10.1021/jacs.4c02958},

doi = {10.1021/jacs.4c02958},

issn = {0002-7863},

year  = {2024},

date = {2024-07-24},

journal = {Journal of the American Chemical Society},

volume = {146},

number = {29},

pages = {19852-19862},

abstract = {Scattering and localization dynamics of charge carriers in the soft lattice of lead-halide perovskites impact polaron formation and recombination, which are key mechanisms of material function in optoelectronic devices. In this study, we probe the photoinduced lattice and carrier dynamics in perovskite thin films (CsFAPbX3},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Efficient Workflows for Detecting Li Depositions in Lithium-Ion Batteries},

author = {T Waldmann and C Hogrefe and M Fl\"{u}gel and I Pivarn\'{i}kov\'{a} and C Weisenberger and E Delz and M Bolsinger and L Boveleth and N Paul and M Kasper and M Feinauer and R Sch\"{a}fer and K Bischof and T Danner and V Knoblauch and P M\"{u}ller-Buschbaum and R Gilles and A Latz and M H\"{o}lzle and M Wohlfahrt-Mehrens},

url = {https://dx.doi.org/10.1149/1945-7111/ad5ef8},

doi = {10.1149/1945-7111/ad5ef8},

issn = {1945-7111 

0013-4651},

year  = {2024},

date = {2024-07-15},

journal = {Journal of The Electrochemical Society},

volume = {171},

number = {7},

pages = {070526},

abstract = {Lithium deposition on anode surfaces can lead to fast capacity degradation and decreased safety properties of Li-ion cells. To avoid the critical aging mechanism of lithium deposition, its detection is essential. We present workflows for the efficient detection of Li deposition on electrode and cell level. The workflows are based on a variety of complementary advanced physico-chemical methods which were validated against each other for both graphite and graphite/Si electrodes: Electrochemical analysis, scanning electron microscopy, glow discharge-optical emission spectroscopy and neutron depth profiling, ex situ optical microscopy, in situ optical microscopy of cross-sectioned full cells, measurements in 3-electrode full cells, as well as 3D microstructurally resolved simulations. General considerations for workflows for analysis of battery cells and materials are discussed. The efficiency can be increased by parallel or serial execution of methods, stop criteria, and design of experiments planning. An important point in case of investigation of Li depositions are rest times during which Li can re-intercalate into the anode or react with electrolyte. Three workflows are presented to solve the questions on the occurrence of lithium deposition in an aged cell, the positions of lithium deposition in a cell, and operating conditions which avoid lithium depositions in a cell.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Insulator Polymer Matrix Construction on All-Small-Molecule Photoactive Blend Towards Extrapolated 15000 Hour T80 Stable Devices},

author = {R Ma and X Jiang and T A Dela Pe\~{n}a and W Gao and J Wu and M Li and S V Roth and P M\"{u}ller-Buschbaum and G Li},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.202405005},

doi = {https://doi.org/10.1002/adma.202405005},

issn = {0935-9648},

year  = {2024},

date = {2024-07-11},

journal = {Advanced Materials},

volume = {36},

number = {35},

pages = {2405005},

abstract = {Abstract To boost the stability of all-small-molecule (ASM) organic photovoltaic (OPV) blends, an insulator polymer called styrene-ethylene-butylene-styrene (SEBS) as morphology stabilizer is applied into the host system of small molecules BM-ClEH:BO-4Cl. Minor addition of SEBS (1 mg/ml in host solution) provides a significantly enhanced T80 value of 15000 hours (extrapolated), surpassing doping-free (0 mg/ml) and heavy doping (10 mg/ml) counterparts (900 hours, 30 hours). The material reproducibility and cost-effectiveness of the active layer will not be affected by this industrially available polymer, where the power conversion efficiency (PCE) can be well maintained at 15.02%, which is still a decent value for non-halogen solvent-treated ASM OPV. Morphological and photophysical characterizations clearly demonstrate SEBS's pivotal effect on suppressing the degradation of donor molecules and blend film's crystallization/aggregation reorganization, which protects the exciton dynamics effectively. This work pays meaningful attention to the ASM system stability, performs a smart strategy to suppress the film morphology degradation, and releases a comprehensive understanding of the mechanism of device performance reduction.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Homogenizing The Low-Dimensional Phases for Stable 2D-3D Tin Perovskite Solar Cells},

author = {Z Kang and K Wang and L Zhang and Y Yang and J Wu and Y Tong and P Yan and Y Chen and H Qi and K Sun and P M\"{u}ller-Buschbaum and X Zhang and J Shang and H Wang},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/smll.202402028},

doi = {https://doi.org/10.1002/smll.202402028},

issn = {1613-6810},

year  = {2024},

date = {2024-07-06},

journal = {Small},

volume = {20},

number = {43},

pages = {2402028},

abstract = {Abstract 2D-3D tin-based perovskites are considered as promising candidates for achieving efficient lead-free perovskite solar cells (PSCs). However, the existence of multiple low-dimensional phases formed during the film preparation hinders the efficient transport of charge carriers. In addition, the non-homogeneous distribution of low-dimensional phases leads to lattice distortion and increases the defect density, which are undesirable for the stability of tin-based PSCs. Here, mixed spacer cations [diethylamine (DEA+) and phenethylamine (PEA+)] are introduced into tin perovskite films to modulate the distribution of the 2D phases. It is found that compared to the film with only PEA+, the combination of DEA+ and PEA+ favors the formation of homogeneous low-dimensional perovskite phases with three octahedral monolayers (n = 3), especially near the bottom interface between perovskite and hole transport layer. The homogenization of 2D phases help improve the film quality with reduced lattice distortion and released strain. With these merits, the tin PSC shows significantly improved stability with 94% of its initial efficiency retained after storing in a nitrogen atmosphere for over 4600 h, and over 80% efficiency maintained after continuous illumination for 400 h.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Operando Study Insights into Lithiation/Delithiation Processes in a Poly(ethylene oxide) Electrolyte of All-Solid-State Lithium Batteries by Grazing-Incidence X-ray Scattering},

author = {Y Liang and T Zheng and K Sun and Z Xu and T Guan and F C Apfelbeck and P Ding and I D Sharp and Y Cheng and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.4c01661},

doi = {10.1021/acsami.4c01661},

issn = {1944-8244},

year  = {2024},

date = {2024-07-03},

journal = {ACS Applied Materials \& Interfaces},

volume = {16},

number = {26},

pages = {33307-33315},

abstract = {Poly(ethylene oxide) (PEO)-based composite electrolytes (PCEs) are considered as promising candidates for next-generation lithium-metal batteries (LMBs) due to their high safety, easy fabrication, and good electrochemical stability. Here, we utilize operando grazing-incidence small-angle and wide-angle X-ray scattering to probe the correlation of electrochemically induced changes and the buried morphology and crystalline structure of the PCE. Results show that the two irreversible reactions, PEO-Li+ reduction and TFSI\textendash decomposition, cause changes in the crystalline structure, array orientation, and morphology of the PCE. In addition, the reversible Li plating/stripping process alters the inner morphology, especially the PEO-LiTFSI domain radius and distance between PEO-LiTFSI domains, rather than causing crystalline structure and orientation changes. This work provides a new path to monitor a working battery in real time and to a detailed understanding of the Li+ diffusion mechanism, which is essential for developing highly transferable and interface-stable PCE-based LMBs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Smart Electrolytes for Lithium Batteries with Reversible Thermal Protection at High Temperatures},

author = {Q Yu and W Sun and S Wang and Q Qiu and W Zhang and H Tian and L Xia and P M\"{u}ller-Buschbaum},

url = {https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/batt.202400339},

doi = {https://doi.org/10.1002/batt.202400339},

year  = {2024},

date = {2024-06-19},

journal = {Batteries \& Supercaps},

volume = {n/a},

number = {n/a},

pages = {e202400339},

abstract = {Abstract Battery safety is a multifaceted concern, with thermal runaway standing out as a primary issue. In this work, we introduce a novel temperature-responsive, self-protection electrolyte governed by the phase separation dynamics of poly (butyl methacrylate) (PBMA) in lithium salt/tetraglyme (G4) blends. This innovation effectively mitigates the risks associated with thermal runaway in lithium batteries. Our electrolyte exhibits a temperature-responsive-recovery characteristic, imparting intelligent capabilities to lithium batteries. At temperatures of \>105 °C, the electrolyte transitions from a homogeneous phase to a segregated state, comprising a PBMA-rich phase with low conductivity and a high conductivity phase containing dissolved lithium salt in G4. The deposition of the PBMA-rich phase on the electrode surface obstructs the ion transport, thereby averting a thermal runaway. Subsequently, upon returning to room temperature of 25 °C, the electrolyte reverts to its homogeneous, highly conductive state, with battery capacity resuming at approximately 94 %. Thus, our electrolyte offers a robust, reversible, smart self-protection for batteries. Additionally, it demonstrates exceptional cycling performance at room temperature. Our findings open new avenues for thermo-reversible and self-protective electrolytes, advancing the safe and widespread adoption of lithium-ion batteries.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Chiral perovskite-CdSe/ZnS QDs composites with high circularly polarized luminescence performance achieved through additive-solvent engineering},

author = {H Zhu and Q Wang and W Chen and K Sun and H Zhong and T Ye and Z Wang and W Zhang and P M\"{u}ller-Buschbaum and X W Sun and D Wu and K Wang},

url = {https://doi.org/10.1063/5.0200692},

doi = {10.1063/5.0200692},

issn = {0021-9606},

year  = {2024},

date = {2024-06-17},

journal = {The Journal of Chemical Physics},

volume = {160},

number = {23},

abstract = {Chiral perovskite materials are being extensively studied as one of the most promising candidates for circularly polarized luminescence (CPL)-related applications. Balancing chirality and photoluminescence (PL) properties is of great importance for enhancing the value of the dissymmetry factor (glum), and a higher glum value indicates better CPL. Chiral perovskite/quantum dot (QD) composites emerge as an effective strategy for overcoming the dilemma that achieving strong chirality and PL in chiral perovskite while at the same time achieving high glum in this composite is very crucial. Here, we choose diphenyl sulfoxide (DPSO) as an additive in the precursor solution of chiral perovskite to regulate the lattice distortion. How structural variation affects the chiral optoelectronic properties of the chiral perovskite has been further investigated. We find that chiral perovskite/CdSe\textendashZnS QD composites with strong CPL have been achieved, and the calculated maximum |glum| of the composites increased over one order of magnitude after solvent-additive modulation (1.55 × 10−3 for R-DMF/QDs, 1.58 × 10−2 for R-NMP-DPSO/QDs, −2.63 × 10−3 for S-DMF/QDs, and −2.65 × 10−2 for S-NMP-DPSO/QDs), even at room temperature. Our findings suggest that solvent-additive modulation can effectively regulate the lattice distortion of chiral perovskite, enhancing the value of glum for chiral perovskite/CdSe\textendashZnS QD composites.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Autonomous self-healing hybrid energy harvester based on the combination of triboelectric nanogenerator and quantum dot solar cell},

author = {T Xiao and S Tu and T Tian and W Chen and W Cao and S Liang and R Guo and L Liu and Y Li and T Guan and H Liu and K Wang and M Schwartzkopf and R A Fischer and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://www.sciencedirect.com/science/article/pii/S2211285524003033},

doi = {https://doi.org/10.1016/j.nanoen.2024.109555},

issn = {2211-2855},

year  = {2024},

date = {2024-06-15},

urldate = {2024-06-15},

journal = {Nano Energy},

volume = {125},

pages = {109555},

abstract = {Realization of multi-source energy harvesting with one single device would maximize power output. Thus, it is emerging as a promising strategy towards renewable energy generation and has attracted worldwide attention in the past decades. Capable of capturing mechanical energy that is ubiquitous in the ambient environment, triboelectric nanogenerator (TENG) has been considered a novel yet effective source towards next-generation energy harvesting. In this work, a flexible hybrid energy harvester (HEH) is developed via the rational integration of autonomous self-healing TENG and high bending-stable lead sulfide quantum dot (PbS QD) solar cell, enabling independent electricity generation by two different mechanisms. The single-electrode mode TENG component with self-healing is realized by a polydimethylsiloxane/Triton X-100 (PDMS/TX100) mixture as the dielectric layer and the shared gold (Au) electrode, which generates 0.39 µA of output current (Iout), 24.6 V of output voltages (Vout), 15.4 nC of transfer charges (Qsc), and 7.80 mW m−2 of output power peak density. The thin-film solar cell component is based on a PbS QD layer as the light absorber with a planar structure fabricated under low-cost and compatible conditions, achieving 22.8 mA cm−2 of short-circuit current density (Jsc) and 4.92% of power conversion efficiency (PCE). As a proof of concept, an electronic watch is successfully powered by harnessing ambient mechanical and solar energy with a hybridized energy cell. This approach will offer more opportunities to construct a versatile platform towards remote monitoring and smart home systems.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Surface Passivation with Tailoring Organic Potassium Salt for Efficient FAPbI3 Perovskite Solar Cells and Modules},

author = {S Zhang and T Tian and J Li and Z Su and C Jin and J Su and W Li and Y Yuan and J Tong and Y Peng and S Bai and P M\"{u}ller-Buschbaum and F Huang and Y-B Cheng and T Bu},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202401945},

doi = {https://doi.org/10.1002/adfm.202401945},

issn = {1616-301X},

year  = {2024},

date = {2024-06-03},

journal = {Advanced Functional Materials},

volume = {34},

number = {36},

pages = {2401945},

abstract = {Abstract Passivating surface defects on perovskite films with tailored functional materials has emerged as one of the most effective strategies for achieving high-performance perovskite solar cells (PSCs). Among existing material selections, potassium salts stand out for their effective passivation of defects surrounding perovskite grain boundaries. However, the widely used potassium salts are inorganic and only soluble in highly polar solvents, which limits their practical application for surface passivation. Herein, a novel organic potassium salt (KCFSO), with multiple organic functional groups and good solubility in low polar isopropanol, is reported to function as a post-treatment agent for perovskite. Combined with experimental results and theoretical calculations, the formed multiple intermolecular interactions between KCFSO and perovskite are revealed to play a vital role in determining the defect passivation effect. Thus, the KCFSO-modified film shows a more uniform surface potential distribution, dramatically decreased defect density, and improved charge transfer, leading to a champion power conversion efficiency (PCE) of 25.11%, and good stability for the derived PSCs. As a demonstration of scalability, the centimeter-sized PSCs and 5 cm × 5 cm mini-modules also demonstrate impressive PCEs of 24.17% and 20.18%, respectively. These findings provide insights into passivator design principles to achieve efficient and stable perovskite photovoltaics.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Direct linearly polarized electroluminescence from perovskite nanoplatelet superlattices},

author = {J Ye and A Ren and L Dai and T K Baikie and R Guo and D Pal and S Gorgon and J E Heger and J Huang and Y Sun and R Arul and G Grimaldi and K Zhang and J Shamsi and Y-T Huang and H Wang and J Wu and A F Koenderink and L Torrente Murciano and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum and J J Baumberg and S D Stranks and N C Greenham and L Polavarapu and W Zhang and A Rao and R L Z Hoye},

url = {https://doi.org/10.1038/s41566-024-01398-y},

doi = {10.1038/s41566-024-01398-y},

issn = {1749-4893},

year  = {2024},

date = {2024-06-01},

journal = {Nature Photonics},

volume = {18},

number = {6},

pages = {586-594},

abstract = {Polarized light is critical for a wide range of applications, but is usually generated by filtering unpolarized light, which leads to substantial energy losses and requires additional optics. Here we demonstrate the direct emission of linearly polarized light from light-emitting diodes made of CsPbI3 perovskite nanoplatelet superlattices. The use of solvents with different vapour pressures enables the self-assembly of the nanoplatelets with fine control over their orientation (either face-up or edge-up) and therefore their transition dipole moment. As a result of the highly uniform alignment of the nanoplatelets, as well as their strong quantum and dielectric confinement, large exciton fine-structure splitting is achieved at the film level, leading to pure red light-emitting diodes with linearly polarized electroluminescence exhibiting a high degree of polarization of 74.4% without any photonic structures. This work demonstrates the potential of perovskite nanoplatelets as a promising source of linearly polarized light, opening up the development of next-generation three-dimensional displays and optical communications from a highly versatile, solution-processable system.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Directional Charge Carrier Management Enabled by Orderly Arranged Perovskite Heterodomain with Defined Size for Self-Powered Photodetectors},

author = {Y Bao and M Li and H Jin and X Wang and J Zeng and Y Feng and W Hui and D Wang and L Gu and J Zhang and Y Hua and X Wang and B Xu and W Chen and Z Wu and P M\"{u}ller-Buschbaum and L Song},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202404697},

doi = {https://doi.org/10.1002/adfm.202404697},

issn = {1616-301X},

year  = {2024},

date = {2024-05-20},

journal = {Advanced Functional Materials},

volume = {34},

number = {44},

pages = {2404697},

abstract = {Abstract Perovskite planar heterojunction is reported to promote charge-carrier separation at the interface due to the introduced built-in potential, leading to improved charge-carrier harvesting. However, the possible diffusion of charge carriers along the film lateral will increase their travel distance to respective electrodes, resulting in increased recombination probabilities. Constructing independent transport channels for positive and negative charge carriers individually is an efficient way to optimize the transport in the perovskite layer and thereby to achieve enhanced device performance. Here, a solution-based strategy is proposed to fabricate lateral bulk heterojunction (BHJ) by arranging methylammonium-based and formamidinium-based perovskites alternately in an ordered array with controllable domains. The structure of perovskite heterodomain directs charge carrier transport along the film normal and limits in-plane charge carrier diffusion. Moreover, the ordered perovskite array is found to greatly increase light harvesting. Consequently, the self-powered photodetector based on the perovskite heterodomain with a thickness of only 250 nm achieves a specific detectivity exceeding 1 × 1014 Jones for weak light over the whole visible light spectrum. This work provides guidance toward the fabrication of perovskite lateral BHJ using solution processing, meeting the requirements not only for charge-carrier manipulation but also for light management.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Poly(sobrerol methacrylate) Colloidal Inks Sprayed onto Cellulose Nanofibril Thin Films for Anticounterfeiting Applications},

author = {C Harder and M Betker and A E Alexakis and Y Bulut and B Sochor and L D S\"{o}derberg and E Malmstr\"{o}m and P M\"{u}ller-Buschbaum and S V Roth},

url = {https://doi.org/10.1021/acsanm.4c01302},

doi = {10.1021/acsanm.4c01302},

year  = {2024},

date = {2024-05-10},

journal = {ACS Applied Nano Materials},

volume = {7},

number = {9},

pages = {10840-10851},

abstract = {The colloidal layer formation on porous materials is a crucial step for printing and applying functional coatings, which can be used to fabricate anticounterfeiting paper. The deposition of colloidal layers and subsequent thermal treatment allows for modifying the hydrophilicity of the surface of a material. In the present work, wood-based colloidal inks are applied by spray deposition on spray-deposited porous cellulose nanofibrils (CNF) films. The surface modification by thermal annealing of the fabricated colloid-cellulose hybrid thin films is investigated in terms of layering and hydrophobicity. The polymer colloids in the inks are core\textendashshell nanoparticles with different sizes and glass transition temperatures (Tg), thus enabling different and low thermal treatment temperatures. The ratio between the core polymers, poly(sobrerol methacrylate) (PSobMA), and poly(-butyl methacrylate) (PBMA) determines the Tg and hence allows for tailoring of the Tg. The layer formation of the colloidal inks on the porous CNF layer depends on the imbibition properties of the CNF layer which is determined by their morphology. The water adhesion of the CNF layer decreases due to the deposition of the colloids and thermal treatment except for the colloids with a size smaller than the void size of the porous CNF film. In this case, the colloids are imbibed into the CNF layer when Tg of the colloids is reached and the polymer chains transit in a mobile phase. Tailored aggregate and nanoscale-embedded hybrid structures are achieved depending on the colloid properties. The imbibition of these colloids into the porous CNF films is verified with grazing incidence small-angle X-ray scattering. This study shows a route for tuning the nanoscale structure and macroscopic physicochemical properties useful for anticounterfeiting paper.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Long-Lasting Hydrogen Evolution and Efficient Dew Harvest Realized via Electrospinning Polyvinylidene Fluoride Membrane on Hybrid Hydrogels},

author = {J Yu and M Chen and N Hu and W Wang and L Lei and H Fan and P M\"{u}ller-Buschbaum and Q Zhong},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/smsc.202400046},

doi = {https://doi.org/10.1002/smsc.202400046},

year  = {2024},

date = {2024-05-08},

journal = {Small Science},

volume = {4},

number = {7},

pages = {2400046},

abstract = {Long-lasting hydrogen evolution and efficient dew harvest is realized via electrospinning a polyvinylidene fluoride (PVDF) membrane on hybrid hydrogels embedded with photocatalytic g-C3N4/Pt nanosheets. Due to the hindrance of water evaporation by the hydrophobic PVDF membrane, the drying process of the hybrid hydrogels significantly slows down. Hence, the g-C3N4/Pt nanosheets can continue working on photocatalytic splitting of the water molecules in the hydrogels. When the thickness of the PVDF membrane is 48 μm, the hydrogen evolution rate can reach 2,543 μmol h−1 g−1, which is 38% more than that of the hybrid hydrogel without covering. Therefore, the hybrid hydrogels covered with PVDF membrane are able to work with high efficiency for 12 h, sufficient for hydrogen evolution during the daytime. In addition, the hydrophobic PVDF membrane and hydrophilic hydrogels construct a Janus structure and induce a fast transport of water molecules from the hydrophobic to hydrophilic side. It is beneficial for the rapid collection of dew in the morning. Based on the long-lasting hydrogen evolution and efficient dew harvest, the present hybrid hydrogels covered with PVDF membrane are very suitable for the environment rich in solar resource and lack of water supply, such as desert or prairie.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Enhanced Hydrogen Evolution in Porous and Hybrid g-C3N4/Pt-PVDF Electrospun Membranes via Piezoelectricity from Water Flow Energy},

author = {M Chen and N Hu and W Wang and L Lei and H Fan and P M\"{u}ller-Buschbaum and Q Zhong},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202402477},

doi = {https://doi.org/10.1002/adfm.202402477},

issn = {1616-301X},

year  = {2024},

date = {2024-05-06},

journal = {Advanced Functional Materials},

volume = {34},

number = {38},

pages = {2402477},

abstract = {Abstract Inspired from seaweed swayed by waves, the enhanced hydrogen evolution is realized in porous and hybrid g-C3N4/Pt-PVDF electrospun membranes via piezoelectricity from water flow energy. The membranes are fabricated by dispersing g-C3N4/Pt into the mixed solution of PVDF and PEO, followed by electrospinning and selective removal of PEO. By changing the PEO amount, the pore size in nanofibers is adjusted. Due to the hydrogen bonding between g-C3N4/Pt and PVDF, the β phase of PVDF is increased, beneficial for the piezoelectricity performance. When the electrospun membranes are exposed to water flow, an additional potential field is triggered due to the deformation of PVDF. It not only eases the photogeneration of charge carriers from g-C3N4/Pt but also hinders their recombination. The prolonged lifetime significantly improves the photocatalytic water splitting of g-C3N4/Pt under visible light. The hydrogen evolution in the electrospun membranes (PVDF to PEO = 4:1) is profoundly improved to 9 278 µmol h−1 g−1, almost doubled to the pure g-C3N4/Pt nanosheets (5 220 µmol h−1 g−1). Therefore, the seaweed-inspired electrospun membrane is a promising strategy for the efficiently photocatalytic water splitting via g-C3N4 in an aqueous environment, such as a natural sea and lake, by the piezoelectricity gained from the water flow energy.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Enhanced UV protection in silk fibroin based electrospun fabrics realized via orientation induced high efficiency of azobenzene isomerization},

author = {K Liu and P Zhang and P M\"{u}ller-Buschbaum and Q Zhong},

url = {https://www.sciencedirect.com/science/article/pii/S0141813024024437},

doi = {https://doi.org/10.1016/j.ijbiomac.2024.131638},

issn = {0141-8130},

year  = {2024},

date = {2024-05-02},

urldate = {2024-05-02},

journal = {International Journal of Biological Macromolecules},

volume = {268},

pages = {131638},

abstract = {Due to the poor UV protection capability, natural silk fabrics not only suffer from easy damage by sunshine but also induce possible sunburn in the human body. Efficient azobenzene isomerization and enhanced UV shielding are realized by replacing the natural silk with natural protein silk fibroin (SF) and electrospinning together with light-responsive copolymer P(MEO2-co-OEG300-co-AHMA). Compared to a solution cast film, the absorption peak intensity at 355 nm is 60 % higher in UV\textendashVis spectra of the electropsun SF/P(MEO2-co-OEG300-co-AHMA) fabrics. This improvement is related to the highly oriented chains, inducing more space and higher efficiency for azobenzene isomerization. Only exposure to visible light for 20 min, the absorption peak corresponding to the trans- state at 355 nm recovers to 92.5 % in the electrospun fabrics, which is at least 100 % faster than that in the solution cast film (50 min). It is related to the zip effect of the isomerization in the oriented chain structure. Thus, not only the absorption of UV radiation, but also the isomerization rate is enhanced. Based on these unique absorption and recovery capabilities, the SF based electrospun fabrics can be used to replace the natural silk fabrics for UV shielding in summer, especially for cyclic use.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A multi-dimensional tactile perception system based on triboelectric sensors: Towards intelligent sorting without seeing},

author = {T Xiao and Z Bing and Y Wu and W Chen and Z Zhou and F Fang and S Liang and R Guo and S Tu and G Pan and T Guan and K Wang and X W Sun and K Huang and A Knoll and Z L Wang and P M\"{u}ller-Buschbaum},

url = {https://www.sciencedirect.com/science/article/pii/S2211285524001460},

doi = {https://doi.org/10.1016/j.nanoen.2024.109398},

issn = {2211-2855},

year  = {2024},

date = {2024-05-01},

urldate = {2024-05-01},

journal = {Nano Energy},

volume = {123},

pages = {109398},

abstract = {Tactile perception systems as the medium between the ambient environment and robotics lie in the heart of modern artificial intelligence. By providing different electronic readouts under various circumstances, they can give easily captured information for post-processing. However, for applications of most reported tactile perception systems, external location assistances are still needed. Here, as inspired by the platypus’ sixth sense, we developed a new kind of tactile perception system based on triboelectric sensors with the additional function from quantum rods. This terminal can be used as a single-electrode mode triboelectric nanogenerator for both location detection and vertical force sensing with high sensitivity and fast response. Moreover, by adding CdSe/CdS quantum rods into an imprinted polydimethylsiloxane film, different lateral stretching levels can be perceived by a modified luminescence. Supported by the machine learning technology, the as-fabricated tactile perception system finally obtains an excellent recognition accuracy among 18 different objects of 98.5% on a micro-controller unit platform, which provides an easy pathway in smart home robotics for intelligent sorting.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Modular slot-die coater for in situ grazing-incidence x-ray scattering experiments on thin films},

author = {M A Reus and T Baier and C G Lindenmeir and A F Weinzierl and A Buyan-Arivjikh and S A Wegener and D P Kosbahn and L K Reb and J Rubeck and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1063/5.0204673},

doi = {10.1063/5.0204673},

issn = {0034-6748},

year  = {2024},

date = {2024-04-01},

journal = {Review of Scientific Instruments},

volume = {95},

number = {4},

abstract = {Multimodal in situ experiments during slot-die coating of thin films pioneer the way to kinetic studies on thin-film formation. They establish a powerful tool to understand and optimize the formation and properties of thin-film devices, e.g., solar cells, sensors, or LED films. Thin-film research benefits from time-resolved grazing-incidence wide- and small-angle x-ray scattering (GIWAXS/GISAXS) with a sub-second resolution to reveal the evolution of crystal structure, texture, and morphology during the deposition process. Simultaneously investigating optical properties by in situ photoluminescence measurements complements in-depth kinetic studies focusing on a comprehensive understanding of the triangular interdependency of processing, structure, and function for a roll-to-roll compatible, scalable thin-film deposition process. Here, we introduce a modular slot-die coater specially designed for in situ GIWAXS/GISAXS measurements and applicable to various ink systems. With a design for quick assembly, the slot-die coater permits the reproducible and comparable fabrication of thin films in the lab and at the synchrotron using the very same hardware components, as demonstrated in this work by experiments performed at Deutsches Elektronen-Synchrotron (DESY). Simultaneous to GIWAXS/GISAXS, photoluminescence measurements probe optoelectronic properties in situ during thin-film formation. An environmental chamber allows to control the atmosphere inside the coater. Modular construction and lightweight design make the coater mobile, easy to transport, quickly extendable, and adaptable to new beamline environments.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Triple-junction solar cells with cyanate in ultrawide-bandgap perovskites},

author = {S Liu and Y Lu and C Yu and J Li and R Luo and R Guo and H Liang and X Jia and X Guo and Y-D Wang and Q Zhou and X Wang and S Yang and M Sui and P M\"{u}ller-Buschbaum and Y Hou},

url = {https://doi.org/10.1038/s41586-024-07226-1},

doi = {10.1038/s41586-024-07226-1},

issn = {1476-4687},

year  = {2024},

date = {2024-04-01},

journal = {Nature},

volume = {628},

number = {8007},

pages = {306-312},

abstract = {Perovskite bandgap tuning without quality loss makes perovskites unique among solar absorbers, offering promising avenues for tandem solar cells1,2. However, minimizing the voltage loss when their bandgap is increased to above 1.90 eV for triple-junction tandem use is challenging3\textendash5. Here we present a previously unknown pseudohalide, cyanate (OCN−), with a comparable effective ionic radius (1.97 r{A}) to bromide (1.95 r{A}) as a bromide substitute. Electron microscopy and X-ray scattering confirm OCN incorporation into the perovskite lattice. This contributes to notable lattice distortion, ranging from 90.5° to 96.6°, a uniform iodide\textendashbromide distribution and consistent microstrain. Owing to these effects, OCN-based perovskite exhibits enhanced defect formation energy and substantially decreased non-radiative recombination. We achieved an inverted perovskite (1.93 eV) single-junction device with an open-circuit voltage (VOC) of 1.422 V, a VOC × FF (fill factor) product exceeding 80% of the Shockley\textendashQueisser limit and stable performance under maximum power point tracking, culminating in a 27.62% efficiency (27.10% certified efficiency) perovskite\textendashperovskite\textendashsilicon triple-junction solar cell with 1 cm2 aperture area.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Reversible and Photochromic Peony-Shaped Hairpin Prepared from Electrospun Hybrid Nanofibers for Visualized Solar UV Radiation Detector},

author = {N Ding and N Hu and J Zhang and H Xu and L Meng and X Cai and P M\"{u}ller-Buschbaum and D Qi and Q Zhong},

url = {https://doi.org/10.1021/acsanm.4c00748},

doi = {10.1021/acsanm.4c00748},

year  = {2024},

date = {2024-03-22},

urldate = {2024-03-22},

journal = {ACS Applied Nano Materials},

volume = {7},

number = {7},

pages = {8140-8150},

abstract = {Because of the detrimental effects of excessive exposure to solar ultraviolet radiation (UVR) on human skin health, wearable UVR detectors have attracted more and more attention. Inspired by the artwork “Tian-tsui hair pin with flora decoration” from the Palace Museum, a reversible and photochromic peony-shaped hairpin is designed to realize the visualized detection of solar UV radiation. It is prepared via electrospinning a mixed solution containing thermoplastic polyurethanes (TPUs) and Zn-MOF@WO3 onto microfiber nonwoven fabrics (MFNFs). Because of the enhanced UV responsive and photochromic capability from Zn-MOF@WO3 as well the excellent flexibility from TPUs and MFNFs, the obtained hairpin presents an excellent photoresponsive and wearable performance. When exposed to UV radiation from sunshine, the hairpin switches from white to light blue and finally to blue with radiation time. The colors light blue and blue can be used to indicate the UV radiation doses for the synthesis of vitamin D and the induction of erythema, respectively. With the assistance of oxygen in air, the hairpin recovers to its original state after being maintained in a dark atmosphere for 12 h. Even after six cycles of exposure to UV radiation and recovery in the dark, the photochromic performance almost remains unchanged. Only a minor reduction of 5% is observed. As a traditional wearable headdress in China, the peony-shaped hairpin prepared from the hybrid nanofibers not only presents oriental elegance but also is suitable for cyclical use in the daytime to monitor UV radiation for skin health management.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Influence of thermal annealing on microstructure, energetic landscape and device performance of P3HT:PCBM-based organic solar cells},

author = {S Alam and C E Petoukhoff and J P Jurado and H Aldosari and X Jiang and T V\'{a}ry and H A Nasser and A Dahman and W Althobaiti and S P G Lopez and W Alsufyani and P M\"{u}ller-Buschbaum and V N\'{a}da\v{z}dy and H Hoppe and F Laquai},

url = {https://dx.doi.org/10.1088/2515-7655/ad2498},

doi = {10.1088/2515-7655/ad2498},

issn = {2515-7655},

year  = {2024},

date = {2024-03-14},

journal = {Journal of Physics: Energy},

volume = {6},

number = {2},

pages = {025013},

abstract = {Thermal annealing alters the morphology of organic donor-acceptor bulk-heterojunction thin films used in organic solar cells. Here, we studied the influence of thermal annealing on blends of amorphous regio-random (RRa) and semi-crystalline regio-regular (RR) poly (3-hexylthiophene) (P3HT) and the fullerene derivative [6,6]-phenyl-C60-butyric acid methyl ester. Since the P3HT:PCBM blend is one of the most studied in the OPV community, the existing research provides a solid foundation for us to compare and benchmark our innovative characterization techniques that have been previously under-utilized to investigate bulk heterojunction organic thin films. Here, we combine advanced novel microscopies and spectroscopies, including polarized light microscopy, photo-deflection spectroscopy, hyperspectral photoluminescence imaging, and energy resolved-electrochemical impedance spectroscopy, with structural characterization techniques, including grazing-incidence wide-angle x-ray scattering, grazing-incidence x-ray diffraction, and Raman spectroscopy, in order to reveal the impact of thermal annealing on the microstructural crystallinity and morphology of the photoactive layer in organic solar cells. Coupled transfer matrix and drift-diffusion simulations were used to study the impact of the density of states on the solar cells’ device performance parameters, namely the short-circuit current (J SC), open circuit voltage (V OC), fill factor (FF), and power conversion efficiency (PCE).},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Triethylsilane introduced precursor engineering towards efficient and stable perovskite solar cells},

author = {Y Huang and W Zhou and H Zhong and W Chen and G Yu and W Zhang and S Wang and Y Sui and X Yang and Y Zhuang and J Tang and L Cao and P M\"{u}ller-Buschbaum and A Aierken and P Han and Z Tang},

url = {https://www.sciencedirect.com/science/article/pii/S2590049823001091},

doi = {https://doi.org/10.1016/j.mtadv.2023.100449},

issn = {2590-0498},

year  = {2024},

date = {2024-03-01},

journal = {Materials Today Advances},

volume = {21},

pages = {100449},

abstract = {Perovskite solar cells (PSCs) are believed to be optimistic for commercial deployment soon since the power conversion efficiency of PSCs presently reaches up to 26.10 % due to the intensive efforts these years. The two-step method is comparatively more suitable for scalable perovskite films, where lead halides and ammonium salts are prepared in separate precursors and deposited sequentially. Therefore, the reactivity between these two precursors governs the quality of final perovskite films and the intrinsic non-radiative recombination (NRR) at the perovskite's interfaces. Herein, we empowered both types of precursors, one by one and then simultaneously, with triethylsilane (TES) to investigate its effect on the (FAPbI3)1-x (MAPbBr3)x perovskite's morphological and optoelectronic properties. TES, with ethyl moieties and metalloid center, in ammonium salts delivers homogeneous perovskites' crystals and inhibits the NRR of perovskite films by reducing the defects and trap states. As a result, the optimized devices exhibit not only improved device performance (particularly for the increased fill factors and open circuit voltages) but also enhanced stabilities.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Humidity Stable Thermoelectric Hybrid Materials Toward a Self-Powered Triple Sensing System},

author = {S Tu and T Tian and T Xiao and X Yao and S Shen and Y Wu and Y Liu and Z Bing and K Huang and A Knoll and S Yin and S Liang and J E Heger and G Pan and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202316088},

doi = {https://doi.org/10.1002/adfm.202316088},

issn = {1616-301X},

year  = {2024},

date = {2024-02-14},

journal = {Advanced Functional Materials},

volume = {34},

number = {25},

pages = {2316088},

abstract = {Abstract Highly sensitive and humidity-resistive detection of the most common physical stimuli is of primary importance for practical application in real-time monitoring. Here, a simple yet effective strategy is reported to achieve a highly humidity-stable hybrid composite that enables simultaneous and accurate pressure and temperature sensing in a single sensor. The improved electronic performance is due to the enhanced planarity of poly (3,-4ethylenedioxythiophene) (PEDOT) and charge transfer between PEDOT:polystyrene sulfonate (PEDOT:PSS) and multi-walled carbon nanotubes (CNTs) by strong π\textendashπ interaction. The preferred electronic pathway induced by a robust morphology in the hybrid composite is responsible for the high humidity stability. This study also demonstrates that the sensor has tremendous potential for intelligent object identification with a high level of 97.78% accuracy. Together with the position-detection capability of a triboelectric nanogenerator (TENG), advantages for potential industrial applications of the triple sensing system in terms of intelligent classification without seeing are foreseen.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {INSIGHT: in situ heuristic tool for the efficient reduction of grazing-incidence X-ray scattering data},

author = {M A Reus and L K Reb and D P Kosbahn and S V Roth and P Muller-Buschbaum},

url = {https://doi.org/10.1107/S1600576723011159},

doi = {doi:10.1107/S1600576723011159},

issn = {1600-5767},

year  = {2024},

date = {2024-02-12},

journal = {Journal of Applied Crystallography},

volume = {57},

number = {2},

pages = {509-528},

abstract = {INSIGHT is a Python-based software tool for processing and reducing 2D grazing-incidence wide- and small-angle X-ray scattering (GIWAXS/GISAXS) data. It offers the geometric transformation of the 2D GIWAXS/GISAXS detector image to reciprocal space, including vectorized and parallelized pixel-wise intensity correction calculations. An explicit focus on efficient data management and batch processing enables full control of large time-resolved synchrotron and laboratory data sets for a detailed analysis of kinetic GIWAXS/GISAXS studies of thin films. It processes data acquired with arbitrarily rotated detectors and performs vertical, horizontal, azimuthal and radial cuts in reciprocal space. It further allows crystallographic indexing and GIWAXS pattern simulation, and provides various plotting and export functionalities. Customized scripting offers a one-step solution to reduce, process, analyze and export findings of large in situ and operando data sets.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {“T-shaped” Carbazole Alkylammonium Cation Passivation in Perovskite Solar Cells},

author = {Z Shi and R Guo and R Luo and X Wang and J Ma and J Feng and X Niu and E Alvianto and Z Jia and X Guo and H Liang and J Chen and Z Li and K Sun and X Jiang and Y Wu and P M\"{u}ller-Buschbaum and W Hu and Y Hou},

url = {https://doi.org/10.1021/acsenergylett.3c02357},

doi = {10.1021/acsenergylett.3c02357},

year  = {2024},

date = {2024-02-09},

journal = {ACS Energy Letters},

volume = {9},

number = {2},

pages = {419-427},

abstract = {Incorporating alkylammonium cations atop the 3D perovskite enables effective defect passivation and significantly enhances the power conversion efficiency of perovskite solar cells. However, the diversity and durability of this passivation strategy have been limited to the ligand type and diffusion of ligands due to high reactivity. Here, we designed bulky “T-shaped” conjugated carbazole alkylammonium cations with inner π\textendashπ interaction and enlarged steric hindrance to minimize ligand diffusion while maintaining passivation effects. As verified by grazing incidence X-ray diffraction and transient absorption spectra, these “T-shaped” passivators could keep a stable intrinsic crystal phase on the perovskite surface after thermal aging. Additionally, the devices utilizing these organic semiconductor-based “T-shaped” ligands were relatively constant in series resistance and introduced higher hole mobility than the PEAI. Finally, the champion device using the “T-shaped” passivator achieved a maximum device efficiency of 25.1% with improved operational stability under 1 sun illumination.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Microstrain and Crystal Orientation Variation within Naked Triple-Cation Mixed Halide Perovskites under Heat, UV, and Visible Light Exposure},

author = {Y Zou and J Eichhorn and J Zhang and F C Apfelbeck and S Yin and L Wolz and C-C Chen and I D Sharp and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsenergylett.3c02617},

doi = {10.1021/acsenergylett.3c02617},

year  = {2024},

date = {2024-02-09},

journal = {ACS Energy Letters},

volume = {9},

number = {2},

pages = {388-399},

abstract = {The instability of perovskite absorbers under various environmental stressors is the most significant obstacle to widespread commercialization of perovskite solar cells. Herein, we study the evolution of crystal structure and microstrain present in naked triple-cation mixed CsMAFA-based perovskite films under heat, UV, and visible light (1 Sun) conditions by grazing-incidence wide-angle X-ray scattering (GIWAXS). We find that the microstrain is gradient distributed along the surface normal of the films, decreasing from the upper surface to regions deeper within the film. Moreover, heat, UV, and visible light treatments do not interfere with the crystalline orientations within annealed polycrystalline films. However, when subjected to heat, the naked perovskite films exhibit a rapid component decomposition, induced by phase separation and ion migration. Conversely, under exposure to UV and 1 Sun light soaking, the naked perovskite films undergo a self-optimization structure evolution during degradation and develop into smoother films with reduced surface potential fluctuations.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Precise Methylation Yields Acceptor with Hydrogen-Bonding Network for High-Efficiency and Thermally Stable Polymer Solar Cells},

author = {W Wei and C E Zhang and Z Chen and W Chen and G Ran and G Pan and W Zhang and P M\"{u}ller-Buschbaum and Z Bo and C Yang and Z Luo},

url = {https://doi.org/10.1002/anie.202315625},

doi = {https://doi.org/10.1002/anie.202315625},

issn = {1433-7851},

year  = {2024},

date = {2024-02-05},

journal = {Angewandte Chemie International Edition},

volume = {63},

number = {6},

pages = {e202315625},

abstract = {Abstract Utilizing intermolecular hydrogen-bonding interactions stands for an effective approach in advancing the efficiency and stability of small-molecule acceptors (SMAs) for polymer solar cells. Herein, we synthesized three SMAs (Qo1, Qo2, and Qo3) using indeno[1,2-b]quinoxalin-11-one (Qox) as the electron-deficient group, with the incorporation of a methylation strategy. Through crystallographic analysis, it is observed that two Qox-based methylated acceptors (Qo2 and Qo3) exhibit multiple hydrogen bond-assisted 3D network transport structures, in contrast to the 2D transport structure observed in gem-dichlorinated counterpart (Qo4). Notably, Qo2 exhibits multiple and stronger hydrogen-bonding interactions compared with Qo3. Consequently, PM6?:?Qo2 device realizes the highest power conversion efficiency (PCE) of 18.4?%, surpassing the efficiencies of devices based on Qo1 (15.8?%), Qo3 (16.7?%), and Qo4 (2.4?%). This remarkable PCE in PM6?:?Qo2 device can be primarily ascribed to the enhanced donor-acceptor miscibility, more favorable medium structure, and more efficient charge transfer and collection behavior. Moreover, the PM6?:?Qo2 device demonstrates exceptional thermal stability, retaining 82.8?% of its initial PCE after undergoing annealing at 65?°C for 250?hours. Our research showcases that precise methylation, particularly targeting the formation of intermolecular hydrogen-bonding interactions to tune crystal packing patterns, represents a promising strategy in the molecular design of efficient and stable SMAs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Synergistic Effect of Dual Phases to Improve Lithium Storage Properties of Nb2O5},

author = {Q Ji and W Chen and X Chen and X Wang and Q Dong and S Yin and Y Shen and P M\"{u}ller-Buschbaum and Y-J Cheng and Y Xia},

url = {https://doi.org/10.1021/acsami.3c17230},

doi = {10.1021/acsami.3c17230},

issn = {1944-8244},

year  = {2024},

date = {2024-02-01},

urldate = {2024-02-01},

journal = {ACS Applied Materials \& Interfaces},

volume = {16},

number = {6},

pages = {7232-7242},

abstract = {Niobium pentoxides (Nb2O5) present great potential as next-generation anode candidates due to exceptional lithium-ion intercalation kinetics, considerably high capacity, and reasonable redox potential. Although four phases of Nb2O5 including hexagonal, orthorhombic, tetragonal, and monoclinic polymorphs show diverse characteristics in electrochemical performance, stable lifetime, high specific capacity, and fast intercalation properties cannot be delivered simultaneously with a single phase. Herein, this issue is addressed by generating a homogeneous mixture of orthorhombic and monoclinic crystals at the nanoscale. Reversible lithium-ion intercalation/deintercalation of the monoclinic phase is achieved, and exceptional lithium storage sites are created at the interface of the two phases. As a result, electrochemical features of stable lifetime from the orthorhombic phase and high specific performance from the monoclinic phase are harmoniously combined. This dual-phase Nb2O5/C nanohybrids deliver as high as 380 mA h g\textendash1 (0.01\textendash3.0 V) and 184 mA h g\textendash1 (1.0\textendash3.0 V) after 200 cycles. The essential principle of property enhancement is further confirmed through in situ XRD measurements and DFT calculations. The dual-phase concept can be further applied on electrodes with multiphases to achieve high electrochemical performance.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Lead-Free Halide Perovskite Materials and Optoelectronic Devices: Progress and Prospective},

author = {I L\'{o}pez-Fern\'{a}ndez and D Valli and C-Y Wang and S Samanta and T Okamoto and Y-T Huang and K Sun and Y Liu and V S Chirvony and A Patra and J Zito and L De Trizio and D Gaur and H-T Sun and Z Xia and X Li and H Zeng and I Mora-Ser\'{o} and N Pradhan and J P Mart\'{i}nez-Pastor and P M\"{u}ller-Buschbaum and V Biju and T Debnath and M Saliba and E Debroye and R L Z Hoye and I Infante and L Manna and L Polavarapu},

url = {https://doi.org/10.1002/adfm.202307896},

doi = {https://doi.org/10.1002/adfm.202307896},

issn = {1616-301X},

year  = {2024},

date = {2024-02-01},

urldate = {2024-02-01},

journal = {Advanced Functional Materials},

volume = {34},

number = {6},

pages = {2307896},

abstract = {Abstract Halide perovskites, in the form of thin films and colloidal nanocrystals, have recently taken semiconductor optoelectronics research by storm, and have emerged as promising candidates for high-performance solar cells, light-emitting diodes (LEDs), lasers, photodetectors, and radiation detectors. The impressive optical and optoelectronic properties, along with the rapid increase in efficiencies of solar cells and LEDs, have greatly attracted researchers across many disciplines. However, most advances made so far in terms of preparation (colloidal nanocrystals and thin films), and the devices with highest efficiencies are based on Pb-based halide perovskites, which have raised concerns over their commercialization due to the toxicity of Pb. This has triggered the search for lower-toxicity Pb-free halide perovskites and has led to significant progress in the last few years. In this roadmap review, researchers of different expertise have joined together to summarize the latest progress, outstanding challenges, and future directions of Pb-free halide perovskite thin films and nanocrystals, regarding their synthesis, optical spectroscopy, and optoelectronic devices, to guide the researchers currently working in this area as well as those that will join the field in the future.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Multifunctional Buried Interface Modification Enables Efficient Tin Perovskite Solar Cells},

author = {Y Chen and H Qi and K Wang and Z Kang and G Pan and C R Everett and P M\"{u}ller-Buschbaum and Y Tong and H Wang},

url = {https://doi.org/10.1002/smtd.202300029},

doi = {https://doi.org/10.1002/smtd.202300029},

issn = {2366-9608},

year  = {2024},

date = {2024-02-01},

journal = {Small Methods},

volume = {8},

number = {2},

pages = {2300029},

abstract = {Abstract Tin perovskite solar cells (PSCs) are considered promising candidates to promote lead-free perovskite photovoltaics. However, their power conversion efficiency (PCE) is limited by the easy oxidation of Sn2+ and low quality of tin perovskite film. Herein, an ultra-thin 1-carboxymethyl-3-methylimidazolium chloride (ImAcCl) layer is used to modify the buried interface in tin PSCs, which can induce multifunctional improvements and remarkably enhance the PCE. The carboxylate group (C?O) and the hydrogen bond donor (N?H) in ImAcCl can interact with tin perovskites, thus significantly suppressing the oxidation of Sn2+ and reducing the trap density in perovskite films. The interfacial roughness is reduced, which contributes to a high-quality tin perovskite film with increased crystallinity and compactness. In addition, the buried interface modification can modulate the crystal dimensionality, favoring the formation of large bulk-like crystals instead of low-dimensional ones in tin perovskite films. Therefore, the charge carrier transport is effectively promoted and the charge carrier recombination is suppressed. Eventually, tin PSCs show a remarkably enhanced PCE from 10.12% to 12.08%. This work highlights the importance of buried interface engineering and provides an effective way to realize efficient tin PSCs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Trace Water in Lead Iodide Affecting Perovskite Crystal Nucleation Limits the Performance of Perovskite Solar Cells},

author = {R Guo and Q Xiong and A Ulatowski and S Li and Z Ding and T Xiao and S Liang and J E Heger and T Guan and X Jiang and K Sun and L K Reb and M A Reus and A Chumakov and M Schwartzkopf and M Yuan and Y Hou and S V Roth and L M Herz and P Gao and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1002/adma.202310237},

doi = {https://doi.org/10.1002/adma.202310237},

issn = {0935-9648},

year  = {2024},

date = {2024-02-01},

journal = {Advanced Materials},

volume = {36},

number = {7},

pages = {2310237},

abstract = {Abstract The experimental replicability of highly efficient perovskite solar cells (PSCs) is a persistent challenge faced by laboratories worldwide. Although trace impurities in raw materials can impact the experimental reproducibility of high-performance PSCs, the in situ study of how trace impurities affect perovskite film growth is never investigated. Here, light is shed on the impact of inevitable water contamination in lead iodide (PbI2) on the replicability of device performance, mainly depending on the synthesis methods of PbI2. Through synchrotron-based structure characterization, it is uncovered that even slight additions of water to PbI2 accelerate the crystallization process in the perovskite layer during annealing. However, this accelerated crystallization also results in an imbalance of charge-carrier mobilities, leading to a degradation in device performance and reduced longevity of the solar cells. It is also found that anhydrous PbI2 promotes a homogenous nucleation process and improves perovskite film growth. Finally, the PSCs achieve a remarkable certified power conversion efficiency of 24.3%. This breakthrough demonstrates the significance of understanding and precisely managing the water content in PbI2 to ensure the experimental replicability of high-efficiency PSCs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {In Situ Surface Reconstruction toward Planar Heterojunction for Efficient and Stable FAPbI3 Quantum Dot Solar Cells},

author = {M Li and Y Bao and W Hui and K Sun and L Gu and X Kang and D Wang and B Wang and H Deng and R Guo and Z Li and X Jiang and P M\"{u}ller-Buschbaum and L Song and W Huang},

url = {https://doi.org/10.1002/adma.202309890},

doi = {https://doi.org/10.1002/adma.202309890},

issn = {0935-9648},

year  = {2024},

date = {2024-02-01},

journal = {Advanced Materials},

volume = {36},

number = {6},

pages = {2309890},

abstract = {Abstract Pure-phase α-FAPbI3 quantum dots (QDs) are the focus of an increasing interest in photovoltaics due to their superior ambient stability, large absorption coefficient, and long charge-carrier lifetime. However, the trap states induced by the ligand-exchange process limit the photovoltaic performances. Here, a simple post treatment using methylamine thiocyanate is developed to reconstruct the FAPbI3-QD film surface, in which a MAPbI3 capping layer with a thickness of 6.2 nm is formed on the film top. This planar perovskite heterojunction leads to a reduced density of trap-states, a decreased band gap, and a facilitated charge carrier transport. As a result, a record high power conversion efficiency (PCE) of 16.23% with negligible hysteresis is achieved for the FAPbI3 QD solar cell, and it retains over 90% of the initial PCE after being stored in ambient environment for 1000 h.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Dendritic Copper Current Collectors as a Capacity Boosting Material for Polymer-Templated Si/Ge/C Anodes in Li-Ion Batteries},

author = {C L Weindl and C E Fajman and Z Xu and T Zheng and G E M\"{o}hl and N Chaulagain and K Shankar and R Gilles and T F F\"{a}ssler and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.3c15735},

doi = {10.1021/acsami.3c15735},

issn = {1944-8244},

year  = {2024},

date = {2024-01-17},

journal = {ACS Applied Materials \& Interfaces},

volume = {16},

number = {2},

pages = {2309-2318},

abstract = {Dendritic copper offers a highly effective method for synthesizing porous copper anodes due to its intricate branching structure. This morphology results in an elevated surface area-to-volume ratio, facilitating shortened electron pathways during aqueous and electrolyte permeation. Here, we demonstrate a procedure for a time- and cost-efficient synthesis routine of fern-like copper microstructures as a host for polymer-templated Si/Ge/C thin films. Dissolvable Zintl clusters and sol\textendashgel chemistry are used to synthesize nanoporous coating as the anode. Cyclic voltammetry (CV) with KOH as the electrolyte is used to estimate the surface area increase in the dendritic copper current collectors (CCs). Half cells are assembled and tested with battery-related techniques such as CV, galvanostatic cycling, and electrochemical impedance spectroscopy, showing a capacity increase in the dendritic copper cells. Energy-dispersive X-ray spectroscopy is used to estimate the removal of K in the bulk after oxidizing the Zintl phase K12Si8Ge9 in the polymer/precursor blend with SiCl4. Furthermore, scanning electron microscopy images are provided to depict the thin films after synthesis and track the degradation of the half cells after cycling, revealing that the morphological degradation through alloying/dealloying is reduced for the dendritic Cu CC anodes as compared with the bare reference. Finally, we highlight this time- and cost-efficient routine for synthesizing this capacity-boosting material for low-mobility and high-capacity anode coatings.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Nanogels Containing Gold Nanoparticles on Cotton Fabrics for Comfort Control via Localized Surface Plasmon Resonance},

author = {Z Zhu and D Qi and Z Yang and Y Wang and P M\"{u}ller-Buschbaum and Q Zhong},

url = {https://doi.org/10.1021/acsanm.3c05211},

doi = {10.1021/acsanm.3c05211},

year  = {2024},

date = {2024-01-12},

journal = {ACS Applied Nano Materials},

volume = {7},

number = {1},

pages = {1222-1232},

abstract = {The wearing comfort of fabrics is strongly related to moisture permeability and thermal insulation. To enhance comfort, the localized surface plasmon resonance (LSPR) effect is applied on cotton fabrics by densely packed hybrid nanogels containing gold nanoparticles on the surface. The nanogels are prepared by emulsion polymerization using di(ethylene glycol) methyl ether methacrylate (MEO2MA), (ethylene glycol) methyl ether methacrylate (OEGMA300), and ethylene glycol methacrylate (EGMA) as monomers. Because of the different transition temperatures of MEO2MA (25 °C) and OEGMA300 (60 °C), the obtained nanogels present a linear shrinkage behavior between 20 to 50 °C. Further treated with in situ reduction, gold nanoparticles (Au NPs) are embedded in the nanogels. After cross-linking the hybrid nanogels onto cotton fabrics and exposure to visible light irradiation (0.1029 W), the ratio of moisture permeability of the cotton fabrics cross-linked with hybrid nanogels (weight gain ratio, WGR of 8%) at 30 °C to that at 20 °C is 1.67. It is 45% better than that of cross-linked pure nanogels without any Au NPs. When the WGR is increased to 15%, the ratio is up to 2.18, thereby almost doubling that of the cross-linked pure nanogels. Such improvement is caused by the LSPR effect from the densely packed hybrid nanogels on the cotton fabric, which induces a more efficient photothermal conversion and prominent shrinkage of the hybrid nanogels. In addition, because the Au NPs can well absorb light irradiation, the cotton fabrics cross-linked with hybrid nanogels are able to efficiently shield the incident light and present a good capability of heat insulation. Therefore, the obtained cotton fabrics can adjust their comfort according to the external light conditions, well suited for outdoor scenarios such as running and hiking.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A Practical Approach Toward Highly Reproducible and High-Quality Perovskite Films Based on an Aging Treatment},

author = {Y Zou and X Bai and S Kahmann and L Dai and S Yuan and S Yin and J E Heger and M Schwartzkopf and S V Roth and C-C Chen and J Zhang and S D Stranks and R H Friend and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1002/adma.202307024},

doi = {https://doi.org/10.1002/adma.202307024},

issn = {0935-9648},

year  = {2024},

date = {2024-01-01},

journal = {Advanced Materials},

volume = {36},

number = {1},

pages = {2307024},

abstract = {Abstract Solution processing of hybrid perovskite semiconductors is a highly promising approach for the fabrication of cost-effective electronic and optoelectronic devices. However, challenges with this approach lie in overcoming the controllability of the perovskite film morphology and the reproducibility of device efficiencies. Here, a facile and practical aging treatment (AT) strategy is reported to modulate the perovskite crystal growth to produce sufficiently high-quality perovskite thin films with improved homogeneity and full-coverage morphology. The resulting AT-films exhibit fewer defects, faster charge carrier transfer/extraction, and suppressed non-radiative recombination compared with reference. The AT-devices achieve a noticeable improvement in the reproducibility, operational stability, and photovoltaic performance of devices, with the average efficiency increased by 16%. It also demonstrates the feasibility and scalability of AT strategy in optimizing the film morphology and device performance for other perovskite components including MAPbI3, (MAPbBr3)15(FAPbI3)85, and Cs0.05(MAPbBr3)0.17(FAPbI3)0.83. This method opens an effective avenue to improve the quality of perovskite films and photovoltaic devices in a scalable and reproducible manner.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Modulation of electronic and ionic conduction in mixed polymer conductors via additive engineering: Towards targeted applications under varying humidity},

author = {S Tu and T Tian and A Vagias and L F Huber and L Liu and S Liang and R A Fischer and S Bernstorff and P M\"{u}ller-Buschbaum},

url = {https://www.sciencedirect.com/science/article/pii/S1385894723057650},

doi = {https://doi.org/10.1016/j.cej.2023.147034},

issn = {1385-8947},

year  = {2023},

date = {2023-12-01},

journal = {Chemical Engineering Journal},

volume = {477},

pages = {147034},

abstract = {Polymer solids with mixed ion and electron transport hold great promise for next-generation organic electronics, and rational regulation of ionic/electronic contribution within these materials can enable a broadened spectrum of practical applications. However, a fundamental understanding of the conduction mechanisms and their correlations with morphological characteristics remains limited, especially under varying environmental humidity conditions. In the present work, simple additive engineering enables the effective regulation of electronic and ionic contribution in poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) based conductors, giving rising to ion- and/or electron-dominant conductions. As a demonstration, PEDOT:PSS films with different electrical characteristics are successfully applied for thermal energy harvesting, healthcare monitoring and human motion detection upon humidity exposure. Combining operando alternating current (AC) impedance spectroscopy and grazing incidence small-angle X-ray scattering at low and high humidity levels, additive-dependent charge transport mechanisms are elucidated, and correlations between morphological alterations and conductivity evolutions are revealed. This work achieves highly tailorable PEDOT:PSS conduction utilizing Zonyl, dimethyl sulfoxide (DMSO) and carbon nanotubes (CNTs) as additives with distinct humidity responses and gains an in-depth comprehension of underlying mechanisms, which are expected to pave the way for next-generation organic electronics.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Tailoring Low-Dimensional Perovskites Passivation for Efficient Two-Step-Processed FAPbI3 Solar Cells and Modules},

author = {F Ye and T Tian and J Su and R Jiang and J Li and C Jin and J Tong and S Bai and F Huang and P M\"{u}ller-Buschbaum and Y-B Cheng and T Bu},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202302775},

doi = {https://doi.org/10.1002/aenm.202302775},

issn = {1614-6832},

year  = {2023},

date = {2023-11-27},

journal = {Advanced Energy Materials},

volume = {n/a},

number = {n/a},

pages = {2302775},

abstract = {Abstract Converting PbI2 residues into low-dimensional perovskites through post-treatment with ammonium-based large cations can passivate 3D perovskites, thus has emerged as an effective strategy to improve the performance of perovskite solar cells (PSCs). Herein, a dramatically improved efficiency is demonstrated for PSCs based on a two-step-processed FAPbI3 perovskite via post-treatment with formamidinium (FA)-based benzamidine hydrochloride (PFACl), outperforming the commonly used methylamine (MA)-based benzylamine hydrochloride (PMACl). With an in-depth exploration of the crystal structures and morphology changes of the FAPbI3 perovskite upon the PFACl post-treatment, the preferential formation of 1D rather than 2D structures on the 3D perovskite film is identified. In contrast to the 2D counterpart, the more energetically favorable 1D structure enables a more effective elimination of PbI2 residues. As a consequence, the PFACl-induced 1D/3D perovskite film is endowed with smoother morphology, more uniform surface potential distribution, lower trap density, faster charge transfer, and better film stability than the PMACl-induced 2D/3D perovskite and control films, demonstrating champion efficiencies of 24.9% for a small-size PSC, 23.6% for a 1 cm2 large-size PSC, and 21.2% for a 5 × 5 cm2 mini-module, which is the highest among the perovskite solar mini-modules using the two-step deposition method.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Near-Infrared Organic Photodetectors toward Skin-Integrated Photoplethysmography-Electrocardiography Multimodal Sensing System},

author = {Z Lou and J Tao and B Wei and X Jiang and S Cheng and Z Wang and C Qin and R Liang and H Guo and L Zhu and P M\"{u}ller-Buschbaum and H-M Cheng and X Xu},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/advs.202304174},

doi = {https://doi.org/10.1002/advs.202304174},

issn = {2198-3844},

year  = {2023},

date = {2023-11-22},

journal = {Advanced Science},

volume = {n/a},

number = {n/a},

pages = {2304174},

abstract = {Abstract In the fast-evolving landscape of decentralized and personalized healthcare, the need for multimodal biosensing systems that integrate seamlessly with the human body is growing rapidly. This presents a significant challenge in devising ultraflexible configurations that can accommodate multiple sensors and designing high-performance sensing components that remain stable over long periods. To overcome these challenges, ultraflexible organic photodetectors (OPDs) that exhibit exceptional performance under near-infrared illumination while maintaining long-term stability are developed. These ultraflexible OPDs demonstrate a photoresponsivity of 0.53 A W−1 under 940 nm, shot-noise-limited specific detectivity of 3.4 × 1013 Jones, and cut-off response frequency beyond 1 MHz at −3 dB. As a result, the flexible photoplethysmography sensor boasts a high signal-to-noise ratio and stable peak-to-peak amplitude under hypoxic and hypoperfusion conditions, outperforming commercial finger pulse oximeters. This ensures precise extraction of blood oxygen saturation in dynamic working conditions. Ultraflexible OPDs are further integrated with conductive polymer electrodes on an ultrathin hydrogel substrate, allowing for direct interface with soft and dynamic skin. This skin-integrated sensing platform provides accurate measurement of photoelectric and biopotential signals in a time-synchronized manner, reproducing the functionality of conventional technologies without their inherent limitations.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Tailoring Low-Dimensional Phases for Improved Performance of 2D\textendash3D Tin Perovskite Solar Cells},

author = {Z Kang and Y Tong and K Wang and Y Chen and P Yan and G Pan and P M\"{u}ller-Buschbaum and L Zhang and Y Yang and J Wu and H Xie and S Liu and H Wang},

url = {https://doi.org/10.1021/acsmaterialslett.3c00929},

doi = {10.1021/acsmaterialslett.3c00929},

year  = {2023},

date = {2023-11-22},

journal = {ACS Materials Letters},

pages = {1-9},

abstract = {2D\textendash3D tin perovskites are considered as promising candidates for realizing efficient lead-free perovskite solar cells (PSCs). However, the ultrathin 2D phases could unfavorably affect charge transport and device performance. In the present work, we demonstrate that the introduction of D-homoserine lactone hydrochloride (D-HLH) can tailor the low-dimensional phases and improve the quality of 2D\textendash3D tin perovskite films. The functional group in D-HLH can interact with FA+ and I\textendash as well as Sn2+ in the precursor solution. These interactions not only affect the formation of tin perovskite film and favor the formation of thicker 2D phases but also decrease the defect density and suppress the nonradiative recombination. As a result, the efficiency of tin PSCs is significantly improved from 7.97 to 12.45%, and the stability of the device is also enhanced. This work provides a feasible strategy to regulate the low-dimensional phases in 2D\textendash3D tin PSCs toward realizing high efficiency.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Unraveling the Humidity Influence on the Electrical Properties of Ionic Liquid Posttreated Poly(3,4-ethylene dioxythiophene):Poly(styrenesulfonate) Films},

author = {A L Oechsle and T Sch\"{o}ner and C Geiger and S Tu and P Wang and R Cubitt and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acs.macromol.3c01842},

doi = {10.1021/acs.macromol.3c01842},

issn = {0024-9297},

year  = {2023},

date = {2023-11-14},

journal = {Macromolecules},

volume = {56},

number = {22},

pages = {9117-9126},

abstract = {The conductive polymer blend poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), popular for numerous organic applications, is investigated in terms of the influences that ionic liquid (IL) treatment and ambient humidity have on its conductivity properties. PEDOT:PSS thin films posttreated with different concentrations of the IL 1-ethyl-3-methylimidazolium dicyanamide (EMIM DCA) are exposed to different relative humidity (RH) steps from 0% RH up to 90% RH. Simultaneously, the film swelling and increase in the scattering length density (SLD), indicating a water uptake of the films, are monitored in situ with spectral reflectance (SR) and time-of-flight neutron reflectometry (ToF-NR). Additional in situ electrochemical impedance spectroscopy (EIS) shows that the pristine PEDOT:PSS has only an electronic conductivity, while for the IL-treated samples, an additional ionic conductivity contribution is observed. Upon humidity increase, the electronic conductivity of all PEDOT:PSS thin films decreases, while the ionic conductivity for IL posttreated thin films is enhanced by the intake of water molecules.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Decoding the Self-Assembly Plasmonic Interface Structure in a PbS Colloidal Quantum Dot Solid for a Photodetector},

author = {T Guan and W Chen and H Tang and D Li and X Wang and C L Weindl and Y Wang and Z Liang and S Liang and T Xiao and S Tu and S V Roth and L Jiang and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsnano.3c08526},

doi = {10.1021/acsnano.3c08526},

issn = {1936-0851},

year  = {2023},

date = {2023-11-10},

journal = {ACS Nano},

volume = {17},

number = {22},

pages = {23010-23019},

abstract = {Hybrid plasmonic nanostructures have gained enormous attention in a variety of optoelectronic devices due to their surface plasmon resonance properties. Self-assembled hybrid metal/quantum dot (QD) architectures offer a means of coupling the properties of plasmonics and QDs to photodetectors, thereby modifying their functionality. The arrangement and localization of hybrid nanostructures have an impact on exciton trapping and light harvesting. Here, we present a hybrid structure consisting of self-assembled gold nanospheres (Au NSs) embedded in a solid matrix of PbS QDs for mapping the interface structures and the motion of charge carriers. Grazing-incidence small-angle X-ray scattering is utilized to analyze the localization and spacing of the Au NSs within the hybrid structure. Furthermore, by correlating the morphology of the Au NSs in the hybrid structure with the corresponding differences observed in the performance of photodetectors, we are able to determine the impact of interface charge carrier dynamics in the coupling structure. From the perspective of architecture, our study provides insights into the performance improvement of optoelectronic devices.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Unraveling the Morphology-Function Correlation of Mesoporous ZnO Films upon Water Exposure},

author = {T Tian and S Tu and A Xu and S Yin and A L Oechsle and T Xiao and A Vagias and J Eichhorn and J Suo and Z Yang and S Bernstorff and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202311793},

doi = {https://doi.org/10.1002/adfm.202311793},

issn = {1616-301X},

year  = {2023},

date = {2023-11-05},

journal = {Advanced Functional Materials},

volume = {n/a},

number = {n/a},

pages = {2311793},

abstract = {Abstract Ubiquitous moisture in synthetic conditions and ambient environments can strongly influence the conductivity of ZnO semiconductors via the chemisorption and physisorption of water molecules on the ZnO surface. Such an intrinsically water-sensitive nature will become more evident in mesoporous ZnO films where a large surface area and active sites are created simultaneously. However, fundamental insights underlying water-mediated ZnO surface chemistry and electrical conductivity and the factors affecting them remain ambiguous due to the complexity of ZnO surfaces and the difficulties of in situ characterizations at multi-dimensions. Here, self-assembling diblock copolymers are exploited as structure-directing agents to achieve mesoporous ZnO thin films with highly tailorable structural characteristics ranging from nanomorphologies, over crystalline levels, to defect contents. As verified by theoretical calculations, the presence of oxygen vacancy will facilitate favorable water adsorption and subsequent dissociation on the polar ZnO surfaces. Upon humidity exposure with progressively increased levels, mesoporous ZnO films are revealed to follow an almost positive relationship between adsorption and electrical conductivity but show superior morphological stability. This work not only elucidates the water-governed ZnO surface chemistry but may also promote a comprehensive understanding of the morphology-function relationship on ZnO-based electronics.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Thermally-Induced Degradation in PM6:Y6-Based Bulk Heterojunction Organic Solar Cells},

author = {S Alam and H Aldosari and C E Petoukhoff and T V\'{a}ry and W Althobaiti and M Alqurashi and H Tang and J I Khan and V N\'{a}da\v{z}dy and P M\"{u}ller-Buschbaum and G C Welch and F Laquai},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202308076},

doi = {https://doi.org/10.1002/adfm.202308076},

issn = {1616-301X},

year  = {2023},

date = {2023-10-27},

journal = {Advanced Functional Materials},

volume = {n/a},

number = {n/a},

pages = {2308076},

abstract = {Abstract Thermally induced degradation of organic photovoltaic devices hinders the commercialization of this emerging PV technology. Thus, a precise understanding of the origin of thermal device instability, as well as identifying strategies to circumvent degradation is of utmost importance. Here, it investigates thermally-induced degradation of state-of-the-art PBDB-T-2F (PM6):BTP (Y6) bulk heterojunction solar cells at different temperatures and reveal changes of their optical properties, photophysics, and morphology. The open-circuit voltage and fill factor of thermally degraded devices are limited by dissociation and charge collection efficiency differences, while the short-circuit current density is only slightly affected. Energy-resolved electrochemical impedance spectroscopy measurements reveal that thermally degraded samples exhibit a higher energy barrier for the charge-transfer state to charge-separated state conversion. Furthermore, the field dependence of charge generation, recombination, and extraction are studied by time-delayed collection field and transient photocurrent and photovoltage experiments, indicating significant bimolecular recombination limits device performance. Finally, coupled optical-electrical device simulations are conducted to fit the devices’ current-voltage characteristics, enabling us to find useful correlations between optical and electrical properties of the active layers and device performance parameters.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Operando study of the influence of small molecule acceptors on the morphology induced device degradation of organic solar cells with different degrees of π\textendashπ stacking},

author = {X Jiang and A J Gillett and T Zheng and X Song and J E Heger and K Sun and L V Spanier and R Guo and S Liang and S Bernstorff and P M\"{u}ller-Buschbaum},

url = {http://dx.doi.org/10.1039/D3EE02527F},

doi = {10.1039/D3EE02527F},

issn = {1754-5692},

year  = {2023},

date = {2023-10-18},

journal = {Energy \& Environmental Science},

volume = {16},

number = {12},

pages = {5970-5981},

abstract = {Due to the development of efficient non-fullerene acceptors with excellent crystallinity and effective inter-mixing with donor polymers, the power conversion efficiencies (PCEs) of organic solar cells (OSCs) have reached levels suitable for commercial implementation. Nonetheless, the poor operational stability of these OSCs remains a significant bottleneck, limiting their practical application and necessitating immediate attention. In an effort to address this issue, in the present study, we investigate the active layers fabricated using four different acceptors (BTP4F, IT4CL, IT4F, and PC71BM) blended with a conjugated polymer donor (PBDBT-2F). The corresponding OSCs demonstrate distinctly different π\textendashπ stacking characteristics. We utilize operando experiments to examine the temporal evolution of the active layer morphology as the OSCs operate under AM 1.5 G light illumination. We discover that, after device operation, the active layer for all types of devices develops a finer structure with more isolated domains, particularly for larger-sized domains. In addition, the morphology of the middle-sized domains is more influenced at the initial operating stage of OSCs with relatively poor π\textendashπ stacking, resulting in a more severe performance decay of these devices. Moreover, the decrease in PCE is primarily attributed to a decrease in the fill factor (FF), with decay curves displaying a similar trend to the structural shrinkage. Notably, we observe that the stability of the active layer morphology in the device geometry is not optimal for well-intermixed donor\textendashacceptor systems with notable face-on crystallinity compared to slightly de-mixed donor\textendashacceptor systems with good π\textendashπ stacking. This behavior is consistent with the different degrees of resilience of device performance.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Insights into the effects of oriented crystallization on the performance of quasi-two-dimensional perovskite solar cells},

author = {R Jiang and T Tian and B Ke and Z Kou and P M\"{u}ller-Buschbaum and F Huang and Y-B Cheng and T Bu},

url = {https://www.sciencedirect.com/science/article/pii/S2949822823000448},

doi = {https://doi.org/10.1016/j.nxmate.2023.100044},

issn = {2949-8228},

year  = {2023},

date = {2023-10-11},

journal = {Next Materials},

volume = {1},

number = {4},

pages = {100044},

abstract = {Long-term operational stability is one of the key problems for the commercialization of the perovskite photovoltaics. During the past decade, a tremendous amount of work has aimed at addressing the stability issues of perovskite solar cells (PSCs). Among them, the intrinsic instability of the ionic crystal structure of perovskite materials is foremost where proper strategies are highly required to complete the crystallization. Reducing the dimensional structure of the photoactive three-dimensional (3D) perovskites by the introduction of a non-photoactive two-dimensional (2D) perovskite phase is a rising topic recently, which generates a quasi-2D perovskite for improving the corresponding device stability. However, the power conversion efficiency (PCE) of quasi-2D perovskite solar cells decreases unfortunately with the increase of the 2D contents, which obviously depends on the orientation of the crystals. In this review, we first review the effect of the crystal orientation on the performance of quasi-2D PSCs. Then, the growth mechanism of the preferred crystal orientation is discussed in detail. The research progress of the modulation strategies which are key segments for the preferred oriented growth of quasi-2D perovskite crystals is summarized emphatically. Finally, we identify some challenges and opportunities for chasing efficient quasi-2D PSCs in furthering our understanding of the above themes.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Ionic Liquid-Induced Inversion of the Humidity-Dependent Conductivity of Thin PEDOT:PSS Films},

author = {A L Oechsle and T Sch\"{o}ner and L Deville and T Xiao and T Tian and A Vagias and S Bernstorff and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.3c08208},

doi = {10.1021/acsami.3c08208},

issn = {1944-8244},

year  = {2023},

date = {2023-09-27},

journal = {ACS Applied Materials \& Interfaces},

volume = {15},

number = {40},

pages = {47682-47691},

abstract = {The humidity influence on the electronic and ionic resistance properties of thin post-treated poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) films is investigated. In particular, the resistance of these PEDOT:PSS films post-treated with three different concentrations (0, 0.05, and 0.35 M) of ethyl-3-methylimidazolium dicyanamide (EMIM DCA) is measured while being exposed to a defined humidity protocol. A resistance increase upon elevated humidity is observed for the 0 M reference sample, while the EMIM DCA post-treated samples demonstrate a reverse behavior. Simultaneously performed in situ grazing-incidence small-angle X-ray scattering (GISAXS) measurements evidence changes in the film morphology upon varying the humidity, namely, an increase in the PEDOT domain distances. This leads to a detriment in the interdomain hole transport, which causes a rise in the resistance, as observed for the 0 M reference sample. Finally, electrochemical impedance spectroscopy (EIS) measurements at different humidities reveal additional contributions of ionic charge carriers in the EMIM DCA post-treated PEDOT:PSS films. Therefrom, a model is proposed, which describes the hole and cation transport in different post-treated PEDOT:PSS films dependent on the ambient humidity.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Unraveling the modification effect at NiOx/perovskite interfaces for efficient and stable inverted perovskite solar cells},

author = {X Kang and D Wang and K Sun and X Dong and W Hui and B Wang and L Gu and M Li and Y Bao and J Zhang and R Guo and Z Li and X Jiang and P M\"{u}ller-Buschbaum and L Song},

url = {http://dx.doi.org/10.1039/D3TA05069F},

doi = {10.1039/D3TA05069F},

issn = {2050-7488},

year  = {2023},

date = {2023-09-26},

journal = {Journal of Materials Chemistry A},

volume = {11},

number = {42},

pages = {22982-22991},

abstract = {Due to low costs and high light transmittance, solution-processed NiOx nanocrystals as the hole transport layer (HTL) for inverted perovskite solar cells (PSCs) have attracted great attention recently. Nevertheless, the intrinsic defects (Ni vacancies) in the NiOx film and the I vacancies at the buried interface of the perovskite limit the performance of PSCs. Thus, in this work, iodine-substituted phenyl acids are used to modify the NiOx/perovskite layer interface. Our results show that the acid functional groups have strong coordination with Ni vacancies in the NiOx film, giving rise to a high conductivity of NiOx films and thereby an improved hole transport capacity. The para-iodine gives the molecule a larger dipole moment, leading to a better energy level alignment between NiOx and the perovskite and thereby a favorable hole transfer through the NiOx/perovskite interface. As a result, the PSC based on 4-iodophenylboronic acid yields a champion power conversion efficiency (PCE) of 22.91% and an improved fill factor of 86.18%. The non-encapsulated device maintains above 80% of its initial PCE after storing in N2 for 3000 h, under heating at 60 °C for 1000 h and in air with a relative humidity (RH) of 50\textendash70% for 1000 h.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Refining the Substrate Surface Morphology for Achieving Efficient Inverted Perovskite Solar Cells},

author = {R Guo and X Wang and X Jia and X Guo and J Li and Z Li and K Sun and X Jiang and E Alvianto and Z Shi and M Schwartzkopf and P M\"{u}ller-Buschbaum and Y Hou},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202302280},

doi = {https://doi.org/10.1002/aenm.202302280},

issn = {1614-6832},

year  = {2023},

date = {2023-09-25},

journal = {Advanced Energy Materials},

volume = {13},

number = {43},

pages = {2302280},

abstract = {Abstract Significant advancements in perovskite solar cells (PSCs) have been driven by the engineering of the interface between perovskite absorbers and charge transport layers. Inverted PSCs offer substantial potential with their high power conversion efficiency (PCE) and enhanced compatibility for tandem solar cell applications. Conventional hole transport materials like poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) and poly(triaryl amine) (PTAA) not only constrain the PSC efficiency but also elevate their fabrication costs. In the case of improving inverted structured PSCs according to the aforementioned concerns, utilizing self-assembled monolayers (SAMs) as hole-transporting layers has played a crucial role. However, the growth of self-assembled monolayers on the substrates still limits the performance and reproducibility of inverted structured PSCs. In this study, the authors delve into the growth model of SAMs on different surface morphologies. Moreover, it is found that the plasma treatment can effectively regulate the surface morphologies of substrates and achieve conformal growth of SAMs. This treatment improves the uniformity and suppresses non-radiative recombination at the interface, which leads to a PCE of 24.5% (stabilized at 23.5%) for inverted structured PSCs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Layer-By-Layer Printed Metal Hybrid (Cs:FA)PbI3 Perovskite Nanocrystal Solar Cells},

author = {M A Reus and A Krifa and Q A Akkerman and A Biewald and Z Xu and D P Kosbahn and C L Weindl and J Feldmann and A Hartschuh and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.202301008},

doi = {https://doi.org/10.1002/adom.202301008},

issn = {2195-1071},

year  = {2023},

date = {2023-09-01},

journal = {Advanced Optical Materials},

volume = {n/a},

number = {n/a},

pages = {2301008},

abstract = {Abstract Mixed halide perovskite nanocrystals in the form of cesium/formamidinium lead triiodide ((Cs:FA)PbI3) offer great potential for efficient and stable solar cells. To date, large-scale production with roll-to-roll compatible deposition methods remains difficult and requires detailed research on each involved processing step. Here, a proof-of-concept study about slot-die coating (printing) the active layer of (Cs:FA)PbI3-based nanocrystal solar cells is presented. Structural and morphological changes during ligand exchange of long-chain oleic acid and oleylamine by Pb(NO3)2, and top-layer FAI passivation are investigated. Ligand exchange improves the processability of the nanocrystal layer and enhances charge transport. It also changes texture from face-on toward edge-on orientation as grazing-incidence X-ray scattering studies indicate. Ligand exchange and FAI passivation redshift photoluminescence and prolong charge carrier lifetime in the printed nanocrystal films. The proof-of-concept feasibility of printing metal halide perovskite nanocrystal films for solar cells is shown by building 20 devices with a median power conversion efficiency of 6.39%.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Sprayed Hybrid Cellulose Nanofibril\textendashSilver Nanowire Transparent Electrodes for Organic Electronic Applications},

author = {M Betker and C Harder and E Erbes and J E Heger and A E Alexakis and B Sochor and Q Chen and M Schwartzkopf and V K\"{o}rstgens and P M\"{u}ller-Buschbaum and K Schneider and S A Techert and L D S\"{o}derberg and S V Roth},

url = {https://doi.org/10.1021/acsanm.3c02496},

doi = {10.1021/acsanm.3c02496},

year  = {2023},

date = {2023-07-07},

journal = {ACS Applied Nano Materials},

volume = {6},

number = {14},

pages = {13677-13688},

abstract = {In times of climate change and resource scarcity, researchers are aiming to find sustainable alternatives to synthetic polymers for the fabrication of biodegradable, eco-friendly, and, at the same time, high-performance materials. Nanocomposites have the ability to combine several favorable properties of different materials in a single device. Here, we evaluate the suitability of two kinds of inks containing silver nanowires for the fast, facile, and industrial-relevant fabrication of two different types of cellulose-based silver nanowire electrodes via layer-by-layer spray deposition only. The Type I electrode has a layered structure, which is composed of a network of silver nanowires sprayed on top of a cellulose nanofibrils layer, while the Type II electrode consists of a homogeneous mixture of silver nanowires and cellulose nanofibrils. A correlation between the surface structure, conductivity, and transparency of both types of electrodes is established. We use the Haacke figure of merit for transparent electrode materials to demonstrate the favorable influence of cellulose nanofibrils in the spray ink by identifying Type II as the electrode with the lowest sheet resistance (minimum 5 ± 0.04 Ω/sq), while at the same time having a lower surface roughness and shorter fabrication time than Type I. Finally, we prove the mechanical stability of the Type II electrode by bending tests and its long-time stability under ambient conditions. The results demonstrate that the mixed spray ink of silver nanowires and cellulose nanofibrils is perfectly suitable for the fast fabrication of highly conductive organic nanoelectronics on an industrial scale.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Film-formation dynamics coordinated by intermediate state engineering enables efficient thickness-insensitive organic solar cells},

author = {X Song and H Xu and X Jiang and S Gao and X Zhou and S Xu and J Li and J Yu and W Liu and W Zhu and P M\"{u}ller-Buschbaum},

url = {http://dx.doi.org/10.1039/D3EE01320K},

doi = {10.1039/D3EE01320K},

issn = {1754-5692},

year  = {2023},

date = {2023-06-20},

journal = {Energy \& Environmental Science},

volume = {16},

number = {8},

pages = {3441-3452},

abstract = {The severe carrier recombination and enormous trap density induced by the anisotropic aggregation state and ungovernable scale of phase separation not only constrain the photovoltaic performance, but also the operational reliability and thickness-tolerance, of organic solar cells (OSCs). Herein, by the delicate coordination of film-formation kinetics, we propose an intermediate state engineering (ISE) strategy to yield efficient, thickness-insensitive and robust OSCs. Using Y6 as a demonstration, inspired by its superior intermolecular interaction with the dithienothiophen[3.2-b]pyrrolobenzothiadiazole (BTP) core in the Y6 molecule, a 1,3,5-tribromobenzene (TBr) solid additive would trigger a distinct TBr:Y6 intermediate phase, which would facilitate self-aggregation behavior and prolong the aggregation kinetics during the drying process. Remarkably, this subtle modulation of BHJ morphology catalyzes inhibited energetic disorder, suppressed trap-assisted recombination and elevated carrier transport and collection capabilities, resulting in a considerable boost in power conversion efficiency (PCE) from 15.9% to 19.1% with an impressive improvement of 20.1% based on the PM6:L8-BO system. Benefitting from this superior manipulation facility, a champion PCE of 17.8% is harvested in a thickness of 300 nm after ISE treatment, representing one of the highest efficiencies in thick-film OSCs. Additionally, doctor-blade coated thick-film devices are fabricated to assess the commercialization potential of the ISE methodology, where a best PCE of 17.1% is yielded on an ISE device with a substantial improvement of 31.5% compared to that of a control device (13.0%). More critically, the ISE-treated device displayed a significantly enhanced T80 (80% degradation of initial value) lifetime from 106 h to 492 h under a continuous 1-sun illumination test.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Morphological Insights into the Degradation of Perovskite Solar Cells under Light and Humidity},

author = {K Sun and R Guo and Y Liang and J E Heger and S Liu and S Yin and M A Reus and L V Spanier and F Deschler and S Bernstorff and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.3c05671},

doi = {10.1021/acsami.3c05671},

issn = {1944-8244},

year  = {2023},

date = {2023-06-16},

journal = {ACS Applied Materials \& Interfaces},

volume = {15},

number = {25},

pages = {30342-30349},

abstract = {Perovskite solar cells (PSCs) have achieved competitive power conversion efficiencies compared with established solar cell technologies. However, their operational stability under different external stimuli is limited, and the underlying mechanisms are not fully understood. In particular, an understanding of degradation mechanisms from a morphology perspective during device operation is missing. Herein, we investigate the operational stability of PSCs with CsI bulk modification and a CsI-modified buried interface under AM 1.5G illumination and 75 ± 5% relative humidity, respectively, and concomitantly probe the morphology evolution with grazing-incidence small-angle X-ray scattering. We find that volume expansion within perovskite grains, induced by water incorporation, initiates the degradation of PSCs under light and humidity and leads to the degradation of device performance, in particular, the fill factor and short-circuit current. However, PSCs with modified buried interface degrade faster, which is ascribed to grain fragmentation and increased grain boundaries. In addition, we reveal a slight lattice expansion and PL redshifts in both PSCs after exposure to light and humidity. Our detailed insights from a buried microstructure perspective on the degradation mechanisms under light and humidity are essential for extending the operational stability of PSCs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Mass transport and charge transfer through an electrified interface between metallic lithium and solid-state electrolytes},

author = {L Katzenmeier and M G\"{o}\sswein and L Carstensen and J Sterzinger and M Ederer and P M\"{u}ller-Buschbaum and A Gagliardi and A S Bandarenka},

url = {https://doi.org/10.1038/s42004-023-00923-4},

doi = {10.1038/s42004-023-00923-4},

issn = {2399-3669},

year  = {2023},

date = {2023-06-15},

journal = {Communications Chemistry},

volume = {6},

number = {1},

pages = {124},

abstract = {All-solid-state Li-ion batteries are one of the most promising energy storage devices for future automotive applications as high energy density metallic Li anodes can be safely used. However, introducing solid-state electrolytes needs a better understanding of the forming electrified electrode/electrolyte interface to facilitate the charge and mass transport through it and design ever-high-performance batteries. This study investigates the interface between metallic lithium and solid-state electrolytes. Using spectroscopic ellipsometry, we detected the formation of the space charge depletion layers even in the presence of metallic Li. That is counterintuitive and has been a subject of intense debate in recent years. Using impedance measurements, we obtain key parameters characterizing these layers and, with the help of kinetic Monte Carlo simulations, construct a comprehensive model of the systems to gain insights into the mass transport and the underlying mechanisms of charge accumulation, which is crucial for developing high-performance solid-state batteries.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Synergistic Defect Passivation by Metformin Halides for Improving Perovskite Solar Cell Performance},

author = {H Dong and G Shen and Y Zou and Y Li and Z Lin and Q Cai and X Xu and Q Song and H Duan and P M\"{u}ller-Buschbaum and C Mu},

url = {https://doi.org/10.1021/acs.jpcc.3c02121},

doi = {10.1021/acs.jpcc.3c02121},

issn = {1932-7447},

year  = {2023},

date = {2023-06-14},

journal = {The Journal of Physical Chemistry C},

volume = {127},

number = {25},

pages = {11845-11853},

abstract = {Defect passivation plays a critical role in manufacturing high-performance perovskite solar cells (PSCs). Herein, engineered components of metformin halides are introduced to the bulk and surface of perovskite layers in PSCs to realize synergistic defect passivation. It is found that the bulk addition of metformin hydrochloride influences the orientation distribution of perovskite crystals and contributes to better perovskite films. Further, the modification of metformin iodide could treat residual defects on the surface of perovskite films. As a result, the synergistically passivated PSCs shows an improved power conversion efficiency (PCE), which increased from 19.36% to 22.17%, together with a higher short-circuit current and open-circuit voltage than those of the control device. Moreover, the as-treated PSCs exhibit excellent thermal and humidity stabilities, maintaining 95% of their initial PCE after being stored under air conditions for over 1000 h. This work provides a novel strategy to passivate perovskite defects and improve the PCE and stability of PSCs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A Novel Multi-Functional Thiophene-Based Organic Cation as Passivation, Crystalline Orientation, and Organic Spacer Agent for Low-Dimensional 3D/1D Perovskite Solar Cells},

author = {A Semerci and A Buyruk and S Emin and R Hooijer and D Kovacheva and P Mayer and M A Reus and D Bl\"{a}tte and M G\"{u}nther and N F Hartmann and S Lotfi and J P Hofmann and P M\"{u}ller-Buschbaum and T Bein and T Ameri},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.202300267},

doi = {https://doi.org/10.1002/adom.202300267},

issn = {2195-1071},

year  = {2023},

date = {2023-05-25},

journal = {Advanced Optical Materials},

volume = {11},

number = {16},

pages = {2300267},

abstract = {Abstract Recently, the mixed-dimensional (3D/2D or 3D/1D) perovskite solar cells using small organic spacers have attracted interest due to their outstanding long-term stability. Here, a new type of thiophene-based organic cation 2-(thiophene-2yl-)pyridine-1-ium iodide (ThPyI), which is used to fabricate mixed-dimensional 3D/1D perovskite solar cells, is presented. The ThPyI-based 1D perovskitoid is applied as a passivator on top of a 3D methyl ammonium lead iodide (MAPI) to fabricate surface-passivated 3D/1D perovskite films or added alone into the 3D perovskite precursor to generate bulk-passivated 3D MAPI. The 1D perovskitoid acts as a passivating agent at the grain boundaries of surface-passivated 3D/1D, which improves the power conversion efficiency (PCE) of the solar cells. Grazing incidence wide-angle X-ray scattering (GIWAXS) studies confirm that ThPyI triggers the preferential orientation of the bulk MAPI slabs, which is essential to enhance charge transport. Champion bulk-passivated 3D and surface-passivated 3D/1D devices yield 14.10% and 19.60% PCE, respectively. The bulk-passivated 3D offers favorable stability, with 84% PCE retained after 2000 h without encapsulation. This study brings a new perspective to the design of organic spacers having a different binding motif and a passivation strategy to mitigate the impact of defects in hybrid 3D/1D perovskite solar cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {When audience takes stage: Pseudo-localized-high-concentration electrolyte with lithium nitrate as the only salt enables lithium metal batteries with excellent temperature and cathode adaptability},

author = {T Zheng and B Zhu and J Xiong and T Xu and C Zhu and C Liao and S Yin and G Pan and Y Liang and X Shi and H Zhao and R Berger and Y-J Cheng and Y Xia and P M\"{u}ller-Buschbaum},

url = {https://www.sciencedirect.com/science/article/pii/S2405829723001617},

doi = {https://doi.org/10.1016/j.ensm.2023.102782},

issn = {2405-8297},

year  = {2023},

date = {2023-05-01},

journal = {Energy Storage Materials},

volume = {59},

pages = {102782},

abstract = {A new concept for pseudo-localized-high-concentration electrolytes (PLHCE) is developed using cheap and less corrosive lithium nitrate as the single lithium salt to improve the electrochemical performance of the lithium metal batteries with excellent temperature and cathode adaptability. Unlike conventional localized high-concentration electrolytes, a small number of the diluent molecules involved in the solvation structure by lithium nitrate and triethyl phosphate (TEP) promote the formation of an organic-inorganic composite solid electrolyte interface (SEI) layer. A good balance is achieved in terms of the mechanical properties of the SEI layer. A high coulombic efficiency of more than 98% for the Li||Cu cell and 1000 h of long-term cycling for the Li||Li cell is exhibited. Assisted with the PLHCE strategy, the Li||LFP cells display excellent performance at both room and high temperatures, and the Li||NCM523 cells with a high working voltage exhibit good electrochemical stability as well. Moreover, alternative solvents are selected as the pseudo-diluents, which proves the general applicability of the PLHCE approach. This work provides an innovative concept to use the solubility difference to manipulate the solvation structure, which paves a new but simple way to design advanced electrolytes for lithium secondary batteries.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {In-situ study of degradation in PTB7:PCBM films prepared with the binary solvent additive DPE:DIO},

author = {D M Schwaiger and W Lohstroh and M Wolf and C J Garvey and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/pol.20230072},

doi = {https://doi.org/10.1002/pol.20230072},

issn = {2642-4150},

year  = {2023},

date = {2023-04-27},

journal = {Journal of Polymer Science},

volume = {61},

number = {15},

pages = {1660-1674},

abstract = {Abstract Blend films of poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b]thiophenediyl]] (PTB7) in combination with 6,6-phenyl-C61-butyric-acid-methyl-ester (PCBM) are a model system for low bandgap organic photovoltaics. Typically, solvent additives are used to improve the power conversion efficiencies of the resulting devices but possibly also decrease the device stability. In this study, we use the binary solvent additive 1,8-diiodooctane:diphenylether (DIO:DPE) for PTB7:PCBM blend films and study how different film drying procedures influence the physical and chemical stability of the polymer blend. The strong influence of the drying procedure on the stability against photoinduced degradation of the PTB7:PCBM films, produced with solvent additives, is shown with data from UV\textendashvisible (UV\textendashvis), Fourier transform infrared (FTIR) and Raman spectroscopy. The addition of solvent additive molecules DIO:DPE to the PTB7:PCBM blend accelerates the degradation compared with the pristine blend. At higher annealing temperature a removal of the additives is bringing degradation back to the level of the pristine blend films, which is promising for photovoltaic applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Ionic liquids tailoring crystal orientation and electronic properties for stable perovskite solar cells},

author = {Y Zou and J Eichhorn and S Rieger and Y Zheng and S Yuan and L Wolz and L V Spanier and J E Heger and S Yin and C R Everett and L Dai and M Schwartzkopf and C Mu and S V Roth and I D Sharp and C-C Chen and J Feldmann and S D Stranks and P M\"{u}ller-Buschbaum},

url = {https://www.sciencedirect.com/science/article/pii/S2211285523002860},

doi = {https://doi.org/10.1016/j.nanoen.2023.108449},

issn = {2211-2855},

year  = {2023},

date = {2023-04-21},

journal = {Nano Energy},

volume = {112},

pages = {108449},

abstract = {The crystallization behavior of perovskite films has a profound influence on the resulting defect densities, charge carrier dynamics and photovoltaic performance. Herein, we introduce ionic liquids into the perovskite component to tailor the crystal growth of perovskite films from a disordered to a preferential corner-up orientation and accordingly increase the charge carrier mobility to accelerate electron transport and extraction. Using time-resolved measurements, we probe the charge carrier generation, transport and recombination behavior in these films and related devices. We find the ionic liquid-containing samples exhibit lower defects, faster charge carrier transport and suppressed non-radiative recombination, contributing to higher efficiency and fill factor. Via operando grazing-incidence small- and wide-angle X-ray scattering measurements, we observe a light-induced lattice compression and grain fragmentation in the control devices, whereas the ionic liquid-containing devices exhibit a slight light-induced crystal reconstitution and stronger tolerance against illumination. Under ambient conditions, the non-encapsulated device with the pyrrolidinium-based ionic compound (Pyr14BF4) maintains 97% of its initial efficiency after 4368 h.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Ionic liquids tailoring crystal orientation and electronic properties for stable perovskite solar cells},

author = {Y Zou and J Eichhorn and S Rieger and Y Zheng and S Yuan and L Wolz and L V Spanier and J E Heger and S Yin and C R Everett and L Dai and M Schwartzkopf and C Mu and S V Roth and I D Sharp and C-C Chen and J Feldmann and S D Stranks and P M\"{u}ller-Buschbaum},

url = {https://www.sciencedirect.com/science/article/pii/S2211285523002860},

doi = {https://doi.org/10.1016/j.nanoen.2023.108449},

issn = {2211-2855},

year  = {2023},

date = {2023-04-14},

journal = {Nano Energy},

volume = {112},

pages = {108449},

abstract = {The crystallization behavior of perovskite films has a profound influence on the resulting defect densities, charge carrier dynamics and photovoltaic performance. Herein, we introduce ionic liquids into the perovskite component to tailor the crystal growth of perovskite films from a disordered to a preferential corner-up orientation and accordingly increase the charge carrier mobility to accelerate electron transport and extraction. Using time-resolved measurements, we probe the charge carrier generation, transport and recombination behavior in these films and related devices. We find the ionic liquid-containing samples exhibit lower defects, faster charge carrier transport and suppressed non-radiative recombination, contributing to higher efficiency and fill factor. Via operando grazing-incidence small- and wide-angle X-ray scattering measurements, we observe a light-induced lattice compression and grain fragmentation in the control devices, whereas the ionic liquid-containing devices exhibit a slight light-induced crystal reconstitution and stronger tolerance against illumination. Under ambient conditions, the non-encapsulated device with the pyrrolidinium-based ionic compound (Pyr14BF4) maintains 97% of its initial efficiency after 4368 h.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Revealing the underlying solvent effect on film morphology in high-efficiency organic solar cells through combined ex situ and in situ observations},

author = {R Ma and X Jiang and J Fu and T Zhu and C Yan and K Wu and P M\"{u}ller-Buschbaum and G Li},

url = {http://dx.doi.org/10.1039/D3EE00294B},

doi = {10.1039/D3EE00294B},

issn = {1754-5692},

year  = {2023},

date = {2023-04-07},

journal = {Energy \& Environmental Science},

volume = {16},

number = {5},

pages = {2316-2326},

abstract = {The morphological features and the film formation processes in high-performance donor\textendashacceptor binary photovoltaic blends cast from three representative solvents are carefully investigated and analyzed. The PM6:L8-BO system shows a very significant efficiency change on varying the solvent from chloroform (CF) to chlorobenzene (CB) and o-xylene (XY), whereas the PM6:eC9 system shows limited influence of the solvent used. Ex situ characterization studies have revealed that CB and XY cause too-pronounced phase separation for PM6:L8-BO. In contrast, PM6:eC9 films display only slightly enhanced phase segregation in CB films and even better mixing in XY-processed films. The in situ observations further reveal that the PM6 aggregation-dominated stage during film formation is longer for the eC9 system than for L8-BO, effectively suppressing the separation of donors and acceptors. PM6 is found to be highly miscible with the acceptors when processed from XY. The ex situ analysis results correlate well with the device performance and are finely explained by the in situ and miscibility study. Furthermore, an excellent device efficiency of 19.10% (verified 18.77%) is achieved using a ternary design for XY-enabled organic solar cells (OSCs) with PTQ10, while the corresponding blade coating devices present an excellent PCE of 18.25%. Thereby, this work provides a clear understanding of film morphology formation and enables the realization of high-performance non-halogenated solvent-processed OSCs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Elucidating the Roles of Nafion/Solvent Formulations in Copper-Catalyzed CO2 Electrolysis},

author = {P Ding and H An and P Zellner and T Guan and J Gao and P M\"{u}ller-Buschbaum and B M Weckhuysen and W Van Der Stam and I D Sharp},

url = {https://doi.org/10.1021/acscatal.2c05235},

doi = {10.1021/acscatal.2c05235},

year  = {2023},

date = {2023-04-05},

journal = {ACS Catalysis},

pages = {5336-5347},

abstract = {Nafion ionomer, composed of hydrophobic perfluorocarbon backbones and hydrophilic sulfonic acid side chains, is the most widely used additive for preparing catalyst layers (CLs) for electrochemical CO2 reduction, but its impact on the performance of CO2 electrolysis remains poorly understood. Here, we systematically investigate the role of the catalyst ink formulation on CO2 electrolysis using commercial CuO nanoparticles as the model pre-catalyst. We find that the presence of Nafion is essential for achieving stable product distributions due to its ability to stabilize the catalyst morphology under reaction conditions. Moreover, the Nafion content and solvent composition (water/alcohol fraction) regulate the internal structure of Nafion coatings, as well as the catalyst morphology, thereby significantly impacting CO2 electrolysis performance, resulting in variations of C2+ product Faradaic efficiency (FE) by \>3×, with C2+ FE ranging from 17 to 54% on carbon paper substrates. Using a combination of ellipsometry and in situ Raman spectroscopy during CO2 reduction, we find that such selectivity differences stem from changes to the local reaction microenvironment. In particular, the combination of high water/alcohol ratios and low Nafion fractions in the catalyst ink results in stable and favorable microenvironments, increasing the local CO2/H2O concentration ratio and promoting high CO surface coverage to facilitate C2+ production in long-term CO2 electrolysis. Therefore, this work provides insights into the critical role of Nafion binders and underlines the importance of optimizing Nafion/solvent formulations as a means of enhancing the performance of electrochemical CO2 reduction systems.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Optical Properties of Slot-Die Coated Hybrid Colloid/Cellulose-Nanofibril Thin Films},

author = {C Harder and A E Alexakis and Y Bulut and S Xiong and B Sochor and G Pan and H Zhong and K Goordeyeva and M A Reus and V K\"{o}rstgens and A Jeromin and T F Keller and L D S\"{o}derberg and E Malmstr\"{o}m and P M\"{u}ller-Buschbaum and S V Roth},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.202203058},

doi = {https://doi.org/10.1002/adom.202203058},

issn = {2195-1071},

year  = {2023},

date = {2023-04-05},

journal = {Advanced Optical Materials},

volume = {n/a},

number = {n/a},

pages = {2203058},

abstract = {Abstract Correlating nanostructure and optical properties of thin hybrid films is the crucial ingredient for designing sustainable applications ranging from structural colors in anticounterfeiting to sensors. Here, the tailoring of the refractive index of hybrid cellulose nanofibril/water-dispersed colloidal ink thin films is presented. The authors apply scalable, layer-by-layer slot-die coating for preparing the cellulose nanofibril and hybrid thin films. Making use of the mobility of the polymer chains in the colloids upon annealing, the influence of the different colloid sizes and their glass transition temperature on the refractive index of the hybrid material is shown. The complex refractive indices of the thin films are characterized by spectroscopic ellipsometry and correlated to the different nanostructures of the thin films. The authors find that post-deposition annealing changes the colloidal nanostructure from particulate to agglomerates. Depending on the size of the colloids, imbibition of the colloids into the cellulose nanofibril template is observed. This scalable approach offers new avenues in structural color functional biomaterial hybrid layers.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Revealing Surface and Interface Evolution of Molybdenum Nitride as Carrier-Selective Contacts for Crystalline Silicon Solar Cells},

author = {Y Li and Y Li and J E Heger and J Zhou and T Guan and C R Everett and W Wei and Z Hong and Y Wu and X Jiang and S Yin and X Yang and D Li and C Jiang and B Sun and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.2c22781},

doi = {10.1021/acsami.2c22781},

issn = {1944-8244},

year  = {2023},

date = {2023-03-06},

journal = {ACS Applied Materials \& Interfaces},

volume = {15},

number = {10},

pages = {13753-13760},

abstract = {Molybdenum nitride (MoNx) was perceived as carrier-selective contacts (CSCs) for crystalline silicon (c-Si) solar cells due to having proper work functions and excellent conductivities. However, the poor passivation and non-Ohmic contact at the c-Si/MoNx interface endow an inferior hole selectivity. Here, the surface, interface, and bulk structures of MoNx films are systematically investigated by X-ray scattering, surface spectroscopy, and electron microscope analysis to reveal the carrier-selective features. Surface layers with the composition of MoO2.51N0.21 form upon air exposure, which induces the overestimated work function and explains the origin of inferior hole selectivities. The c-Si/MoNx interface is confirmed to adopt long-term stability, providing guidance for designing stable CSCs. A detailed evolution of the scattering length density, domain sizes, and crystallinity in the bulk phase is presented to elucidate its superior conductivity. These multiscale structural investigations offer a clear structure\textendashfunction correlation of MoNx films, providing key inspiration for developing excellent CSCs for c-Si solar cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Fully Methylammonium-Free Stable Formamidinium Lead Iodide Perovskite Solar Cells Processed under Humid Air Conditions},

author = {K Wang and J Huo and L Cao and P Yang and P M\"{u}ller-Buschbaum and Y Tong and H Wang},

url = {https://doi.org/10.1021/acsami.2c23134},

doi = {10.1021/acsami.2c23134},

issn = {1944-8244},

year  = {2023},

date = {2023-02-28},

journal = {ACS Applied Materials \& Interfaces},

volume = {15},

number = {10},

pages = {13353-13362},

abstract = {Fabricating perovskite solar cells (PSCs) in ambient air condition is beneficial for lowering the processing cost and boosting the commercialization. Formamidinium lead iodide (FAPbI3) is an attractive candidate for efficient PSCs; however, it easily suffers from degradation and phase transition in the presence of ambient moisture. Methylammonium (MA) cation is commonly incorporated to stabilize FAPbI3, whereas the residual MA tends to deteriorate the thermal and operational stability. Herein, we report a MA-free strategy to fabricate high-quality α-FAPbI3 films and inverted PSCs under open air conditions with a relative humidity (RH) of 60 ± 10%. The incorporation of phenylethylammonium iodide (PEAI) effectively inhibits the decomposition and phase transition of FAPbI3 during its crystallization in humid air. Accordingly, phase-pure α-FAPbI3 perovskite films with significantly reduced δ-FAPbI3 and PbI2 content are successfully obtained. In addition, introducing PEAI strongly enhances the crystallinity of FAPbI3 perovskite films, thereby yielding enlarged grain sizes and reduced grain boundaries. Defects at the grain boundaries and surface are further passivated by PEAI addition, so that the trap state density is significantly decreased. As a result, the non-radiative recombination is effectively suppressed and the charge carrier transport is promoted. The inverted device optimized with a suitable PEAI concentration exhibits an enhanced power conversion efficiency (PCE) of 17.83%, which significantly surpasses the control device (12.29% PCE). Moreover, the PEAI optimized FAPbI3 PSCs demonstrate strongly improved long-term stability, with nearly 97% PCE maintained after 27-day storage under ambient conditions. This work provides a feasible way to fabricate PSCs in ambient air for promoting their wide range of applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Shedding Light on the Moisture Stability of Halide Perovskite Thin Films},

author = {K Sun and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/ente.202201475},

doi = {https://doi.org/10.1002/ente.202201475},

issn = {2194-4288},

year  = {2023},

date = {2023-02-08},

journal = {Energy Technology},

volume = {n/a},

number = {n/a},

pages = {2201475},

abstract = {To date, remarkable progress has been achieved in the power conversion efficiency of perovskite solar cells (PSCs). Nevertheless, the instability and degradation of PSCs under external stimuli still shadow the prospectus of their commercialization. As a notorious culprit deteriorating the stability of PSCs, moisture-induced degradation is thereby an important aspect. Herein, a comprehensive review of moisture effects on the halide perovskite film, in particular the moisture-induced degradation mechanism and methods toward enhancing the stability, is discussed. In detail, the benefits for perovskite films having a certain amount of water incorporation are elucidated, and the underlying moisture-induced structural degradation and decomposition process of perovskites are summarized. Light is also shed on the methods to enhance the moisture stability of perovskites, particularly a 3D/2D heterostructure. Thereby, this review will enlighten the readers of understanding moisture-induced degradation and the development of stable perovskites.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Solvent Modulation of Chiral Perovskite Films Enables High Circularly Polarized Luminescence Performance from Chiral Perovskite/Quantum Dot Composites},

author = {H Zhu and Q Wang and K Sun and W Chen and J Tang and J Hao and Z Wang and J Sun and W C H Choy and P M\"{u}ller-Buschbaum and X W Sun and D Wu and K Wang},

url = {https://doi.org/10.1021/acsami.2c20716},

doi = {10.1021/acsami.2c20716},

issn = {1944-8244},

year  = {2023},

date = {2023-02-08},

journal = {ACS Applied Materials \& Interfaces},

volume = {15},

number = {7},

pages = {9978-9986},

abstract = {Materials with circularly polarized luminescence (CPL) activity are promising in many chiroptoelectronics fields, such as for biological probes, asymmetric photosynthesis, information storage, spintronic devices, and so on. Promoting the value of the dissymmetry factor (glum) for the CPL-active materials based on chiral perovskite draws increasing attention since a higher glum value indicates better CPL. In this work, we find that, after being treated with a facile solvent modulation strategy, the chirality of 2D chiral perovskite films has been enhanced a lot, which we attribute to an increased lattice distortion degree. By forming chiral perovskite/quantum dot (QD) composites, the CPL-active material is successfully obtained. The calculated maximum |glum| of these composites increased over 4 times after solvent modulation treatment (1.53 × 10\textendash3 for the pristine sample of R-DMF and 6.91 × 10\textendash3 for R-NMP) at room temperature. Moreover, the enhancement of the CPL intensity is ascribed to two aspects: one is the generation and transportation of spin-polarized charge carriers from chiral perovskite films to combine in the QD layer, and the other is the solvent modulation strategy to enlarge the lattice distortion of chiral perovskite films. This facile route provides an effective way to construct CPL-active materials. More importantly, this kind of composite material (chiral perovskite film/QD layer) can be easily applied for fabricating circularly polarized light-emitting diode devices for electroluminescence.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Ligand Chemistry of Inorganic Lead Halide Perovskite Nanocrystals},

author = {N Fiuza-Maneiro and K Sun and I L\'{o}pez-Fern\'{a}ndez and S G\'{o}mez-Gra\~{n}a and P M\"{u}ller-Buschbaum and L Polavarapu},

url = {https://doi.org/10.1021/acsenergylett.2c02363},

doi = {10.1021/acsenergylett.2c02363},

year  = {2023},

date = {2023-01-26},

journal = {ACS Energy Letters},

pages = {1152-1191},

abstract = {Lead halide perovskite nanocrystals (LHP NCs) have emerged as next-generation semiconductor materials with outstanding optical and optoelectronic properties. Because of the high surface-to-volume ratio, the optical and optoelectronic performance and the colloidal stability of LHP NCs largely depend on their surface chemistry, especially the ligands and surface termination. On one hand, the capping ligands improve the colloidal stability and luminescence; on the other hand the highly dynamic binding nature of ligands is detrimental to the colloidal stability and photoluminescence of LHP NCs. In addition, the surface functionalization with desired molecules induces new functionalities such as chirality, light harvesting, and triplet sensitization through energy/electron transfer or use as X-ray detectors. In this review, we present the current understanding of an atomic view of the surface chemistry of colloidal LHP NCs, including crystal termination, vacancies, and different types of capping ligands. Furthermore, we discuss the ligand-induced functionalities, including photocatalysis and chirality.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Superlattice deformation in quantum dot films on flexible substrates via uniaxial strain},

author = {J E Heger and W Chen and H Zhong and T Xiao and C Harder and F C Apfelbeck and A F Weinzierl and R Boldt and L Schraa and E Euchler and A K Sambale and K Schneider and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {http://dx.doi.org/10.1039/D2NH00548D},

doi = {10.1039/D2NH00548D},

issn = {2055-6756},

year  = {2023},

date = {2023-01-23},

journal = {Nanoscale Horizons},

volume = {8},

number = {3},

pages = {383-395},

abstract = {The superlattice in a quantum dot (QD) film on a flexible substrate deformed by uniaxial strain shows a phase transition in unit cell symmetry. With increasing uniaxial strain, the QD superlattice unit cell changes from tetragonal to cubic to tetragonal phase as measured with in situ grazing-incidence small-angle X-ray scattering (GISAXS). The respective changes in the optoelectronic coupling are probed with photoluminescence (PL) measurements. The PL emission intensity follows the phase transition due to the resulting changing inter-dot distances. The changes in PL intensity accompany a redshift in the emission spectrum, which agrees with the F\"{o}rster resonance energy transfer (FRET) theory. The results are essential for a fundamental understanding of the impact of strain on the performance of flexible devices based on QD films, such as wearable electronics and next-generation solar cells on flexible substrates.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {All-optical controlled-NOT logic gate achieving directional asymmetric transmission based on metasurface doublet},

author = {Y Huang and T Xiao and S Chen and Z Xie and J Zheng and J Zhu and Y Su and W Chen and K Liu and M Tang and P M\"{u}ller-Buschbaum and L Li},

url = {http://www.oejournal.org//article/doi/10.29026/oea.2023.220073},

doi = {10.29026/oea.2023.220073},

issn = {2096-4579},

year  = {2023},

date = {2023-01-18},

journal = {Opto-Electronic Advances},

pages = {220073-1-220073-9},

abstract = {Optical logic gates play important roles in all-optical logic circuits, which lie at the heart of the next-generation optical computing technology. However, the intrinsic contradiction between compactness and robustness hinders the development in this field. Here, we propose a simple design principle that can possess multiple-input-output states according to the incident circular polarization and direction based on the metasurface doublet, which enables controlled-NOT logic gates in infrared region. Therefore, the directional asymmetric electromagnetic transmission can be achieved. As a proof of concept, a spin-dependent Janus metasurface is designed and experimentally verified that four distinct images corresponding to four input states can be captured in the far-field. In addition, since the design method is derived from geometric optics, it can be easily applied to other spectra. We believe that the proposed metasurface doublet may empower many potential applications in chiral imaging, chiroptical spectroscopy and optical computing.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Film Formation Kinetics of Polymer Donor and Nonfullerene Acceptor Active Layers During Printing Out of 1,2,4-Trimethylbenzene in Ambient Conditions},

author = {X Jiang and S Grott and V K\"{o}rstgens and K S Wienhold and Z Li and J Zhang and C R Everett and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/solr.202201077},

doi = {https://doi.org/10.1002/solr.202201077},

issn = {2367-198X},

year  = {2023},

date = {2023-01-13},

journal = {Solar RRL},

volume = {7},

number = {6},

pages = {2201077},

abstract = {Slot-die coating is a promising upscaling fabrication method to promote commercialization in the field of organic solar cells. Herein, the nonfullerene active layer blend of a conjugated polymer PffBT4T-2OD and a small molecule acceptor EH-IDTBR, which is printed out of the nonhalogenated solvent 1,2,4-trimethylbenzene, is studied. The film formation kinetics of the active layer PffBT4T-2OD:EH-IDTBR is probed in terms of the temporal evolutions in morphology as well as molecular conformation and aggregation as revealed by in situ grazing-incidence small angle X-ray scattering and UV\textendashvis spectroscopy during the film printing process. A five-regime mesoscale domain growth process is observed in the active layer from the liquid state to the final dry state. The solvent evaporation-induced domain growth is accompanied with molecular stacking in a distinct J-type aggregation of the acceptor and a slight H-type aggregation of the donor molecules. The printed active layers exhibit an edge-on dominated PffBT4T-2OD and a face-on dominated EH-IDTBR crystallite structure. Compared to the neat PffBT4T-2OD and EH-IDTBR films, in the active layer, the crystallite structure deviates slightly in lattice spacing.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Control of the Crystallization and Phase Separation Kinetics in Sequential Blade-Coated Organic Solar Cells by Optimizing the Upper Layer Processing Solvent},

author = {Y Wang and J Xue and H Zhong and C R Everett and X Jiang and M A Reus and A Chumakov and S V Roth and M A Adedeji and N Jili and K Zhou and G Lu and Z Tang and G T Mola and P M\"{u}ller-Buschbaum and W Ma},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202203496},

doi = {https://doi.org/10.1002/aenm.202203496},

issn = {1614-6832},

year  = {2023},

date = {2023-01-01},

journal = {Advanced Energy Materials},

volume = {n/a},

number = {n/a},

pages = {2203496},

abstract = {Abstract Sequential deposition of the active layer in organic solar cells (OSCs) is favorable to circumvent the existing drawbacks associated with controlling the microstructure in bulk-heterojunction (BHJ) device fabrication. However, how the processing solvents impact on the morphology during sequential deposition processes is still poorly understood. Herein, high-efficiency OSCs are fabricated by a sequential blade coating (SBC) through optimization of the morphology evolution process induced by processing solvents. It is demonstrated that the device performance is highly dependent on the processing solvent of the upper layer. In situ morphology characterizations reveal that an obvious liquid\textendashsolid phase separation can be identified during the chlorobenzene processing of the D18 layer, corresponding to larger phase separation. During chloroform (CF) processing of the D18 layer, a proper aggregation rate of Y6 and favorable intermixing of lower and upper layers results in the enhanced crystallinity of the acceptor. This facilitates efficient exciton dissociation and charge transport with an inhibited charge recombination in the D18/CF-based devices, contributing to a superior performance of 17.23%. These results highlight the importance of the processing solvent for the upper layer in the SBC strategy and suggest the great potential of achieving optimized morphology and high-efficiency OSCs using the SBC strategy.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Antisolvent Additive Engineering for Boosting Performance and Stability of Graded Heterojunction Perovskite Solar Cells Using Amide-Functionalized Graphene Quantum Dots},

author = {E Khorshidi and B Rezaei and A Kavousighahfarokhi and J Hanisch and M A Reus and P M\"{u}ller-Buschbaum and T Ameri},

url = {https://doi.org/10.1021/acsami.2c12944},

doi = {10.1021/acsami.2c12944},

issn = {1944-8244},

year  = {2022},

date = {2022-11-29},

journal = {ACS Applied Materials \& Interfaces},

volume = {14},

number = {49},

pages = {54623-54634},

abstract = {Additive and antisolvent engineering strategies are outstandingly efficient in enhancing perovskite quality, photovoltaic performance, and stability of perovskite solar cells (PSCs). In this work, an effective approach is applied by coupling the antisolvent mixture and multi-functional additive procedures, which is recognized as antisolvent additive engineering (AAE). The graphene quantum dots functionalized with amide (AGQDs), which consists of carbonyl, amine, and long hydrophobic alkyl chain functional groups, are added to the antisolvent mixture of toluene (T) and hexane (H) as an efficient additive to form the CH3NH3PbI3 (MAPI):AGQDs graded heterojunction structure. A broad range of analytical techniques, including scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, space charge limited current, UV\textendashvisible spectroscopy, external quantum efficiency, and time-of-flight secondary ion mass spectrometry, are used to investigate the effect of AAE treatment with AGQDs on the quality of perovskite film and performance of the PSCs. Importantly, not only a uniform and dense perovskite film with hydrophobic property is obtained but also defects on the perovskite surface are significantly passivated by the interaction between AGQDs and uncoordinated Pb2+. As a result, an enhanced power conversion efficiency (PCE) of 19.10% is achieved for the champion PSCs treated with AGQD additive, compared to the PCE of 16.00% for untreated reference PSCs. In addition, the high-efficiency PSCs based on AGQDs show high stability and maintain 89% of their initial PCE after 960 h in ambient conditions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Tailored fabrication of quasi-isoporous and double layered α-Fe2O3 thin films and their application in photovoltaic devices},

author = {S Yin and Y Zou and M A Reus and X Jiang and S Tu and T Tian and R Qi and Z Xu and S Liang and Y Cheng and J E Heger and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://www.sciencedirect.com/science/article/pii/S1385894722056157},

doi = {https://doi.org/10.1016/j.cej.2022.140135},

issn = {1385-8947},

year  = {2022},

date = {2022-11-21},

journal = {Chemical Engineering Journal},

pages = {140135},

abstract = {A series of α-Fe2O3 thin films with distinct morphologies are prepared via a facile polystyrene-block-polyethylene oxide templated sol\textendashgel method. By tailoring the poor solvent contents and FeCl3-to-polymer weight ratio in the sol\textendashgel solutions, quasi-isoporous α-Fe2O3 thin films with different substructures and thicknesses are obtained. Via a thermal annealing post-treatment, double layered structures are induced by a synergistic dewetting and Oswald ripening effect. Special focus is set on the α-Fe2O3 thin films prepared with no annealing/annealing-medium FeCl3 concentration, as they possess uniform periodic structures, which is suitable to be used as hole blocking modification layer of perovskite solar cells (PSCs). An improved power conversion efficiency (PCE) is obtained when the double layered α-Fe2O3 thin film is applied as the hole blocking modification layer for PSCs. The improved PCE primarily originates from the increased VOC, which probably benefits from the synergistic effect of the suppressed charge carrier recombination at the interfaces, the enhanced light transmittance as well as the superior electron extraction capacity.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Mapping structure heterogeneities and visualizing moisture degradation of perovskite films with nano-focus WAXS},

author = {N Li and S Pratap and V K\"{o}rstgens and S Vema and L Song and S Liang and A Davydok and C Krywka and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1038/s41467-022-34426-y},

doi = {10.1038/s41467-022-34426-y},

issn = {2041-1723},

year  = {2022},

date = {2022-11-05},

journal = {Nature Communications},

volume = {13},

number = {1},

pages = {6701},

abstract = {Extensive attention has focused on the structure optimization of perovskites, whereas rare research has mapped the structure heterogeneity within mixed hybrid perovskite films. Overlooked aspects include material and structure variations as a function of depth. These depth-dependent local structure heterogeneities dictate their long-term stabilities and efficiencies. Here, we use a nano-focused wide-angle X-ray scattering method for the mapping of film heterogeneities over several micrometers across lateral and vertical directions. The relative variations of characteristic perovskite peak positions show that the top film region bears the tensile strain. Through a texture orientation map of the perovskite (100) peak, we find that the perovskite grains deposited by sequential spray-coating grow along the vertical direction. Moreover, we investigate the moisture-induced degradation products in the perovskite film, and the underlying mechanism for its structure-dependent degradation. The moisture degradation along the lateral direction primarily initiates at the perovskite-air interface and grain boundaries. The tensile strain on the top surface has a profound influence on the moisture degradation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Picosecond Charge-Transfer-State Dynamics in Wide Band Gap Polymer\textendashNon-Fullerene Small-Molecule Blend Films Investigated via Transient Infrared Spectroscopy},

author = {M Nuber and L V Spanier and S Roth and G N Vayssilov and R Kienberger and P M\"{u}ller-Buschbaum and H Iglev},

url = {https://doi.org/10.1021/acs.jpclett.2c02864},

doi = {10.1021/acs.jpclett.2c02864},

year  = {2022},

date = {2022-11-03},

journal = {The Journal of Physical Chemistry Letters},

pages = {10418-10423},

abstract = {Organic solar cells based on wide band gap polymers and nonfullerene small-molecule acceptors have demonstrated remarkably good device performances. Nevertheless, a thorough understanding of the charge-transfer process in these materials has not been achieved yet. In this study, we use Fano resonance signals caused by the interaction of broad electronic charge carrier absorption and the molecular vibrations of the electron acceptor molecule to monitor the charge-transfer state dynamics. In our time-resolved infrared spectroscopy experiments, we find that in the small-molecule acceptor, they have additional dynamics on the order of a few picoseconds. A change in the solvent used in thin film deposition, leading to different morphologies, influences this time further. We interpret our findings as the dynamics of the charge-transfer state at the interface of the electron donor and the electron- acceptor. The additional mid-infrared transient signal is generated in this state, as both electron and hole polarons can interact with small-molecule acceptor vibrational modes.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Improvement of the thermoelectric properties of PEDOT:PSS films via DMSO addition and DMSO/salt post-treatment resolved from a fundamental view},

author = {S Tu and T Tian and A Lena Oechsle and S Yin and X Jiang and W Cao and N Li and M A Scheel and L K Reb and S Hou and A S Bandarenka and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://www.sciencedirect.com/science/article/pii/S1385894721038742},

doi = {https://doi.org/10.1016/j.cej.2021.132295},

issn = {1385-8947},

year  = {2022},

date = {2022-09-06},

urldate = {2022-09-06},

journal = {Chemical Engineering Journal},

volume = {429},

pages = {132295},

abstract = {The combination of dimethyl sulfoxide (DMSO)-solvent doping and physical\textendashchemical DMSO/salt de-doping in a sequence has been used to improve the thermoelectric (TE) properties of poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) films. A high power factor of ca.105.2 µW m−1 K−2 has been achieved for the PEDOT:PSS film after post-treatment with 10 % sodium sulfite (Na2SO3) in the DMSO/salt mixture (v/v), outperforming sodium bicarbonate (NaHCO3). The initial DMSO-doping treatment induces a distinct phase separation by facilitating the aggregation of the PEDOT molecules. At the same time, the subsequent DMSO/salt de-doping post-treatment strengthens the selective removal of the surplus non-conductive PSS chains. Substantial alterations in the oxidation level, chain conformations, PEDOT crystallites and their preferential orientation are observed upon treatment on the molecular level. At the mesoscale level, the purification and densification of PEDOT-rich domains enable the realization of inter-grain coupling by the formation of the electronically well-percolated network. Thereby, both electrical conductivity and Seebeck coefficient are optimized.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {High-performance and Large-area Inverted Perovskite Solar Cells based on NiOx Films Enabled with A Novel Microstructure-Control Technology},

author = {G Shen and X Li and Y Zou and H Dong and D Zhu and Y Jiang and X R Ng and F Lin and P M\"{u}ller-Buschbaum and C Mu},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/eem2.12504},

doi = {https://doi.org/10.1002/eem2.12504},

year  = {2022},

date = {2022-08-26},

journal = {ENERGY \& ENVIRONMENTAL MATERIALS},

volume = {n/a},

number = {n/a},

pages = {e12504},

abstract = {Abstract The improvement in the efficiency of inverted perovskite solar cells (PSCs) is significantly limited by undesirable contact at the NiOX/perovskite interface. In this study, a novel microstructure-control technology is proposed for the fabrication of porous NiOX films using Pluronic P123 as the structure-directing agent and acetylacetone (AcAc) as the coordination agent. The synthesized porous NiOX films enhanced the hole extraction efficiency and reduced recombination defects at the NiOX/perovskite interface. Consequently, without any modification, the power conversion efficiency (PCE) of the PSC with MAPbI3 as the absorber layer improved from 16.50 to 19.08 %. Moreover, the PCE of the device composed of perovskite Cs0.05(MA0.15FA0.85)0.95Pb(I0.85Br0.15)3 improved from 17.49 to 21.42 %. Furthermore, the application of the fabricated porous NiOX on fluorine-doped tin oxide (FTO) substrates enabled the fabrication of large-area PSCs (1.2 cm2) with a PCE of 19.63 %. This study provides a novel strategy for improving the contact at the NiOX/perovskite interface for the fabrication of high-performance large-area perovskite solar cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {In Situ Observation of Morphological and Oxidation Level Degradation Processes within Ionic Liquid Post-treated PEDOT:PSS Thin Films upon Operation at High Temperatures},

author = {A L Oechsle and J E Heger and N Li and S Yin and S Bernstorff and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.2c05745},

doi = {10.1021/acsami.2c05745},

issn = {1944-8244},

year  = {2022},

date = {2022-07-13},

journal = {ACS Applied Materials \& Interfaces},

volume = {14},

number = {27},

pages = {30802-30811},

abstract = {Organic thermoelectric thin films are investigated in terms of their stability at elevated operating temperatures. Therefore, the electrical conductivity of ethyl-3-methylimidazolium dicyanamide (EMIM DCA) post-treated poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) thin films is measured over 4.5 h of heating at 50 or 100 °C for different EMIM DCA concentrations. The changes in the electrical performance are correlated with changes in the film morphology, as evidenced with in situ grazing-incidence small-angle X-ray scattering (GISAXS). Due to the overall increased PEDOT domain distances, the resulting impairment of the interdomain charge carrier transport directly correlates with the observed electrical conductivity decay. With in situ ultraviolet−visible (UV\textendashVis) measurements, a simultaneously occurring reduction of the PEDOT oxidation level is found to have an additional electrical conductivity lowering contribution due to the decrease of the charge carrier density. Finally, the observed morphology and oxidation level degradation is associated with the deterioration of the thermoelectric properties and hence a favorable operating temperature range is suggested for EMIM DCA post-treated PEDOT:PSS-based thermoelectrics.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {In Situ Observation of Morphological and Oxidation Level Degradation Processes within Ionic Liquid Post-treated PEDOT:PSS Thin Films upon Operation at High Temperatures},

author = {A L Oechsle and J E Heger and N Li and S Yin and S Bernstorff and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.2c05745},

doi = {10.1021/acsami.2c05745},

issn = {1944-8244},

year  = {2022},

date = {2022-06-27},

journal = {ACS Applied Materials \& Interfaces},

volume = {14},

number = {27},

pages = {30802-30811},

abstract = {Organic thermoelectric thin films are investigated in terms of their stability at elevated operating temperatures. Therefore, the electrical conductivity of ethyl-3-methylimidazolium dicyanamide (EMIM DCA) post-treated poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) thin films is measured over 4.5 h of heating at 50 or 100 °C for different EMIM DCA concentrations. The changes in the electrical performance are correlated with changes in the film morphology, as evidenced with in situ grazing-incidence small-angle X-ray scattering (GISAXS). Due to the overall increased PEDOT domain distances, the resulting impairment of the interdomain charge carrier transport directly correlates with the observed electrical conductivity decay. With in situ ultraviolet−visible (UV\textendashVis) measurements, a simultaneously occurring reduction of the PEDOT oxidation level is found to have an additional electrical conductivity lowering contribution due to the decrease of the charge carrier density. Finally, the observed morphology and oxidation level degradation is associated with the deterioration of the thermoelectric properties and hence a favorable operating temperature range is suggested for EMIM DCA post-treated PEDOT:PSS-based thermoelectrics.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Elucidating the Role of Antisolvents on the Surface Chemistry and Optoelectronic Properties of CsPbBrxI3-x Perovskite Nanocrystals},

author = {J Ye and Z Li and D J Kubicki and Y Zhang and L Dai and C Otero-Mart\'{i}nez and M A Reus and R Arul and K R Dudipala and Z Andaji-Garmaroudi and Y-T Huang and Z Li and Z Chen and P M\"{u}ller-Buschbaum and H-L Yip and S D Stranks and C P Grey and J J Baumberg and N C Greenham and L Polavarapu and A Rao and R L Z Hoye},

url = {https://doi.org/10.1021/jacs.2c02631},

doi = {10.1021/jacs.2c02631},

issn = {0002-7863},

year  = {2022},

date = {2022-06-27},

journal = {Journal of the American Chemical Society},

volume = {144},

number = {27},

pages = {12102-12115},

abstract = {Colloidal lead-halide perovskite nanocrystals (LHP NCs) have emerged over the past decade as leading candidates for efficient next-generation optoelectronic devices, but their properties and performance critically depend on how they are purified. While antisolvents are widely used for purification, a detailed understanding of how the polarity of the antisolvent influences the surface chemistry and composition of the NCs is missing in the field. Here, we fill this knowledge gap by studying the surface chemistry of purified CsPbBrxI3-x NCs as the model system, which in itself is considered a promising candidate for pure-red light-emitting diodes and top-cells for tandem photovoltaics. Interestingly, we find that as the polarity of the antisolvent increases (from methyl acetate to acetone to butanol), there is a blueshift in the photoluminescence (PL) peak of the NCs along with a decrease in PL quantum yield (PLQY). Through transmission electron microscopy and X-ray photoemission spectroscopy measurements, we find that these changes in PL properties arise from antisolvent-induced iodide removal, which leads to a change in halide composition and, thus, the bandgap. Using detailed nuclear magnetic resonance (NMR) and Fourier-transform infrared spectroscopy (FTIR) measurements along with density functional theory calculations, we propose that more polar antisolvents favor the detachment of the oleic acid and oleylamine ligands, which undergo amide condensation reactions, leading to the removal of iodide anions from the NC surface bound to these ligands. This work shows that careful selection of low-polarity antisolvents is a critical part of designing the synthesis of NCs to achieve high PLQYs with minimal defect-mediated phase segregation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Strong Induced Circular Dichroism in a Hybrid Lead-Halide Semiconductor Using Chiral Amino Acids for Crystallite Surface Functionalization},

author = {M W Heindl and T Kodalle and N Fehn and L K Reb and S Liu and C Harder and M Abdelsamie and L Eyre and I D Sharp and S V Roth and P M\"{u}ller-Buschbaum and A Kartouzian and C M Sutter-Fella and F Deschler},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.202200204},

doi = {https://doi.org/10.1002/adom.202200204},

issn = {2195-1071},

year  = {2022},

date = {2022-06-17},

journal = {Advanced Optical Materials},

volume = {n/a},

number = {n/a},

pages = {2200204},

abstract = {Abstract Chirality is a desired property in functional semiconductors for optoelectronic, catalytic, and spintronic applications. Here, introducing enantiomerically-pure 3-aminobutyric acid (3-ABA) into thin films of the 1D semiconductor dimethylammonium lead iodide (DMAPbI3) is found to result in strong circular dichroism (CD) in the optical absorption. X-ray diffraction and grazing incidence small angle X-ray scattering (GISAXS) are applied to gain molecular-scale insights into the chirality transfer mechanism, which is attributed to a chiral surface modification of DMAPbI3 crystallites. This study demonstrates that the CD signal strength can be controlled by the amino-acid content relative to the crystallite surface area. The CD intensity is tuned by the composition of the precursor solution and the spin-coating time, thereby achieving anisotropy factors (gabs) as high as 1.75 × 10\textendash2. Grazing incidence wide angle scattering reveals strong preferential ordering that can be suppressed via tailored synthesis conditions. Different contributions to the chiroptical properties are resolved by a detailed analysis of the CD signal utilizing an approach based on the Mueller matrix model. This report of a novel class of chiral hybrid semiconductors with precise control over their optical activity presents a promising approach for the design of circularly polarized light detectors and emitters.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Operando Study of Structure Degradation in Solid-State Dye-Sensitized Solar Cells with a TiO2 Photoanode Having Ordered Mesopore Arrays},

author = {N Li and R Guo and A L Oechsle and M A Reus and S Liang and L Song and K Wang and D Yang and F Allegretti and A Kumar and M Nuber and J Berger and S Bernstorff and H Iglev and J Hauer and R A Fischer and J V Barth and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/solr.202200373},

doi = {https://doi.org/10.1002/solr.202200373},

issn = {2367-198X},

year  = {2022},

date = {2022-05-31},

journal = {Solar RRL},

volume = {n/a},

number = {n/a},

pages = {2200373},

abstract = {Via operando grazing-incidence small-angle X-ray scattering, the degradation mechanisms of solid-state dye-sensitized solar cells (ssDSSCs) using two types of ordered mesoporous TiO2 scaffolds with different pore sizes, and an exemplary dye D205, are investigated. The temporal evolution of the inner morphology shows a strong impact on device performance. The photoinduced dye aggregation on the TiO2 surface leads to an increase in the domain radius but a decreased spatial order of the photoactive layer during the burn-in stage. This dye aggregation on the TiO2 surface causes the short-circuit current density loss, which plays a major role in the power conversion efficiency decay. Finally, it is found that a larger surface area in the small-pore sample yields a faster short-circuit current density decay as compared with the big-pore sample. Therefore, a control of dye aggregation and the pore size of TiO2 photoelectrodes is crucial for the stability of TiO2-based ssDSSCs.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Effect of Solvent Vapor Annealing on Diblock Copolymer-Templated Mesoporous Si/Ge/C Thin Films: Implications for Li-Ion Batteries},

author = {C L Weindl and C E Fajman and M A Giebel and K S Wienhold and S Yin and T Tian and C Geiger and L P Kreuzer and M Schwartzkopf and S V Roth and T F F\"{a}ssler and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsanm.2c01191},

doi = {10.1021/acsanm.2c01191},

year  = {2022},

date = {2022-05-17},

journal = {ACS Applied Nano Materials},

volume = {5},

number = {5},

pages = {7278-7287},

abstract = {Although amphiphilic diblock copolymer templating of inorganic materials such as TiO2 is already well investigated, sol\textendashgel synthesis routines for porous silicon and germanium are relatively rare. Therefore, especially in the field of Li-ion batteries, novel synthesis routines with the possibility to tune the silicon and germanium ratio and the morphology in the nanometer regime are of high interest. Here, we demonstrate a synthesis method that allows a change of morphology and elemental composition with minimal effort. We evidence a morphological transformation in the nanometer regime with real space (scanning electron microscopy) and complementary reciprocal space analysis methods (grazing-incidence small-angle X-ray scattering). Although energy-dispersive X-ray spectroscopy (EDS) reveals a considerable amount of oxygen in the thin film, crystalline Ge in the bulk is detected with powder X-ray diffraction (PXRD) and Raman spectroscopy. Due to the system’s simplicity, chemical mass production options such as roll-to-roll or slot-die printing can also be considered high-yield methods compared to standard synthesis routines.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Time-Resolved Orientation and Phase Analysis of Lead Halide Perovskite Film Annealing Probed by In Situ GIWAXS},

author = {M A Reus and L K Reb and A F Weinzierl and C L Weindl and R Guo and T Xiao and M Schwartzkopf and A Chumakov and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.202102722},

doi = {https://doi.org/10.1002/adom.202102722},

issn = {2195-1071},

year  = {2022},

date = {2022-04-03},

journal = {Advanced Optical Materials},

volume = {n/a},

number = {n/a},

pages = {2102722},

abstract = {Abstract Scalable thin-film deposition methods are increasingly important for hybrid lead halide perovskite thin films. Understanding the structure evolution during non-equilibrium processes helps to find suitable materials and processing parameters to produce films with well-performing optoelectronic properties. Here, spin-cast and slot-die coated bilayers of lead iodide (PbI2) and methylammonium iodide (MAI) are investigated by in situ grazing-incidence wide-angle X-ray scattering during the thermal annealing process, which converts the bilayer into methylammonium lead iodide (MAPI). Photoluminescence (PL) and UV/Vis measurements show increasing crystallinity during the annealing process and a slight PL red-shift of the spin-cast film, attributed to crystallite coalescence that is not prominent for the slot-die coated film. The disintegration of the solvent-precursor complex (MA)2(Pb3I8) ⋅ 2 DMSO and conversion into perovskite are followed in situ and differences in the morphology and time evolution are observed. In both, spin-cast and slot-die coated thin-films, the isotropic orientation is dominant, however, in the slot-die coated films, the perovskite crystallites have an additional face-on orientation ((110) parallel to substrate) that is not detected in spin-cast films. An Avrami model is applied for the perovskite crystal growth that indicates reduced dimensionality of the growth for the printed thin films.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Process-aid solid engineering triggers delicately modulation of Y-series non-fullerene acceptor for efficient organic solar cells},

author = {X Song and K Zhang and R Guo and K Sun and Z Zhou and S Huang and L Huber and M Reus and J Zhou and M Schwartzkopf and S V Roth and W Liu and Y Liu and W Zhu and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.202200907},

doi = {https://doi.org/10.1002/adma.202200907},

issn = {0935-9648},

year  = {2022},

date = {2022-03-22},

journal = {Advanced Materials},

volume = {n/a},

number = {n/a},

pages = {2200907},

abstract = {Abstract Volatile solids with symmetric π-backbone have been intensively implemented on manipulating the nanomorphology for improving the operability and stability of organic solar cells. However, due to the isotropic stacking, the announced solids with symmetric geometry cannot modify the microscopic phase separation and component distribution collaboratively, which would constrain the promotion of exciton splitting and charge collection efficiency. Inspired by the superiorities of asymmetric configuration, a novel process-aid solid (PAS) engineering is proposed. By coupling with BTP core unit in Y-series molecule, an asymmetric, volatile 1, 3-dibromo-5-chlorobenzene (DBCl) solid can induce the anisotropic dipole direction, elevated dipole moment, and interlaminar interaction spontaneously. Due to the synergetic effects on the favorable phase separation and desired component distribution, the PAS treated devices feature the evident improvement of exciton splitting, charge transport, and collection, accompanied by the suppressed trap-assisted recombination. Consequently, we achieve an impressive fill factor of 80.2% with maximum power conversion efficiency (PCE) of 18.5% in the PAS treated device. More strikingly, the PAS treated devices demonstrate a promising thickness-tolerance character, where a record PCE of 17.0% is yielded in PAS devices with a 300 nm thickness photoactive layer, which represents the highest PCE for thick-film OSCs. This article is protected by copyright. All rights reserved},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Hydrophobic Graphene Quantum Dots for Defect Passivation and Enhanced Moisture Stability of CH3NH3PbI3 Perovskite Solar Cells},

author = {E Khorshidi and B Rezaei and D Bl\"{a}tte and A Buyruk and M A Reus and J Hanisch and B B\"{o}ller and P M\"{u}ller-Buschbaum and T Ameri},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/solr.202200023},

doi = {https://doi.org/10.1002/solr.202200023},

issn = {2367-198X},

year  = {2022},

date = {2022-03-19},

journal = {Solar RRL},

volume = {n/a},

number = {n/a},

pages = {2200023},

abstract = {Passivating the defects and grain boundaries (GBs) of perovskite films at the interface by interface engineering is a promising route to achieve efficient and stable perovskite solar cells (PSCs). Herein, a new type of graphene, that is, hydrophobic graphene quantum dots (HGQDs) containing amide linkages, which consist of carbonyl and dodecyl amine groups, is successfully used as a bifunctional interface modifier to engineer the interface of the perovskite/hole transport layer. A comprehensive characterization including X-ray photoelectron spectroscopy, Fourier-transform photocurrent spectroscopy, Raman spectroscopy, photoluminescence spectroscopy, and space-charge-limited current measurements is performed to identify the underlying passivation mechanisms. It can be demonstrated that the HGQDs, due to the bifunctional groups containing N and O atoms, effectively passivate the uncoordinated Pb2+ ions at the perovskite film surface and GBs and consequently induce a lower trap state density. Moreover, HGQDs enhance the quality of the perovskite film which reduces the charge recombination at the interface. Therefore, the power conversion efficiency of PSCs treated with HGQDs is significantly increased from 16.00% to 18.30%, mainly based on the improved open-circuit voltage and fill factor. Importantly, the HGQDs featuring hydrophobicity due to alkyl chains significantly enhance moisture stability.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Revealing Donor\textendashAcceptor Interaction on the Printed Active Layer Morphology and the Formation Kinetics for Nonfullerene Organic Solar Cells at Ambient Conditions},

author = {X Jiang and P Chotard and K Luo and F Eckmann and S Tu and M A Reus and S Yin and J Reitenbach and C L Weindl and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/aenm.202103977},

doi = {https://doi.org/10.1002/aenm.202103977},

issn = {1614-6832},

year  = {2022},

date = {2022-02-27},

journal = {Advanced Energy Materials},

volume = {n/a},

number = {n/a},

pages = {2103977},

abstract = {Abstract Slot-die coating is a powerful method for upscaling the production of organic solar cells (OSCs) with low energy consumption print processes at ambient conditions. Herein, chlorobenzene (CB) and chloroform (CF) are compared as host solvents for printing films of the neat novel fused-ring unit based wide-bandgap donor polymer (PDTBT2T-FTBDT), the small molecule nonfullerene acceptor based on a fused ring with a benzothiadiazole core (BTP-4F) as well as the respective PDTBT2T-FTBDT:BTP-4F blend films at room temperature in air. Using CF printing of the PDTBT2T-FTBDT:BTP-4F active layer, OSCs with a high power conversion efficiency of up to 13.2% are reached in ambient conditions. In comparison to CB printed blend films, the active layer printed out of CF has a superior morphology, a smoother film surface and a more pronounced face-on orientation of the crystallites, which altogether result in an enhanced exciton dissociation, a superior charge transport, and suppressed nonradiative charge carrier recombination. Based on in situ studies of the slot-die coating process of PDTBT2T-FTBDT, BTP-4F, and PDTBT2T-FTBDT:BTP-4F films, the details of the film formation kinetics are clarified, which cause the superior behavior for CF compared to CB printing due to balancing the aggregation and crystallization of donor and acceptor.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Low-Temperature and Water-Based Biotemplating of Nanostructured Foam-Like Titania Films Using \ss-Lactoglobulin},

author = {J E Heger and W Chen and S Yin and N Li and V K\"{o}rstgens and C J Brett and W Ohm and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202113080},

doi = {https://doi.org/10.1002/adfm.202113080},

issn = {1616-301X},

year  = {2022},

date = {2022-02-17},

journal = {Advanced Functional Materials},

volume = {n/a},

number = {n/a},

pages = {2113080},

abstract = {Abstract Given the broad use of nanostructured crystalline titania films, an environmentally friendly and more sustainable synthesis route is highly desirable. Here, a water-based, low-temperature route is presented to synthesize nanostructured foam-like crystalline titania films. A pearl necklace-like nanostructure is introduced as tailored titania morphology via biotemplating with the use of the major bovine whey protein \ss-lactoglobulin (\ss-lg). It is shown that titania crystallization in a brookite-anatase mixed phase is promoted via spray deposition at a comparatively low temperature of 120 °C. The obtained crystallites have an average grain size of (4.2 ± 0.3) nm. In situ grazing incidence small-angle and wide-angle X-ray scattering (GISAXS/GIWAXS) are simultaneously performed to understand the kinetics of film formation and the templating role of \ss-lg during spray coating. In the \ss-lg:titania biohybrid composites, the crystal growth in semicrystalline titania clusters is sterically directed by the condensing \ss-lg biomatrix. Due to using spray coating, the green chemistry approach to titania-based functional films can be scaled up on a large scale, which can potentially be used in photocatalytic processes or systems related to energy application.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Solvent Tuning of the Active Layer Morphology of Non-Fullerene Based Organic Solar Cells},

author = {S Grott and A Kotobi and L K Reb and C L Weindl and R Guo and S Yin and K S Wienhold and W Chen and T Ameri and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/solr.202101084},

doi = {https://doi.org/10.1002/solr.202101084},

issn = {2367-198X},

year  = {2022},

date = {2022-02-12},

journal = {Solar RRL},

volume = {n/a},

number = {n/a},

pages = {2101084},

abstract = {Non-fullerene acceptor (NFA)-based organic solar cells have made tremendous progress in recent years. For the neat NFA system PBDB-T:ITIC, the film morphology and crystallinity are tailored by the choice of the solvent used for spin coating the active layers. Three different chlorinated solvents, chlorobenzene (CB), chloroform, and dichlorobenzene, are compared and the obtained active layer morphology is correlated with the optoelectronic properties and the device performance. The small domain sizes in the case of CB are most beneficial for the device performance, whereas the largest number or size of face-on PBDB-T crystallites is not causing the highest power conversion efficiencies (PCEs). In addition, when using CB, the number of edge-on crystallites is highest and the distances between neighboring domains are small. The smoothest blend films are realized with CB, which exhibit correlated roughness with their substrates and no large aggregates have formed in these blend films. Thus, CB offers the best way to balance the aggregation and crystallization kinetics in the active layer and enables the highest PCE values.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {The Influence of CsBr on Crystal Orientation and Optoelectronic Properties of MAPbI3-Based Solar Cells},

author = {Y Zou and S Yuan and A Buyruk and J Eichhorn and S Yin and M A Reus and T Xiao and S Pratap and S Liang and C L Weindl and W Chen and C Mu and I D Sharp and T Ameri and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.1c22184},

doi = {10.1021/acsami.1c22184},

issn = {1944-8244},

year  = {2022},

date = {2022-01-06},

urldate = {2022-01-06},

journal = {ACS Applied Materials \& Interfaces},

volume = {14},

pages = {2958},

abstract = {Crystal orientations are closely related to the behavior of photogenerated charge carriers and are vital for controlling the optoelectronic properties of perovskite solar cells. Herein, we propose a facile approach to reveal the effect of lattice plane orientation distribution on the charge carrier kinetics via constructing CsBr-doped mixed cation perovskite phases. With grazing-incidence wide-angle X-ray scattering measurements, we investigate the crystallographic properties of mixed perovskite films at the microscopic scale and reveal the effect of the extrinsic CsBr doping on the stacking behavior of the lattice planes. Combined with transient photocurrent, transient photovoltage, and space-charge-limited current measurements, the transport dynamics and recombination of the photogenerated charge carriers are characterized. It is demonstrated that CsBr compositional engineering can significantly affect the perovskite crystal structure in terms of the orientation distribution of crystal planes and passivation of trap-state densities, as well as simultaneously facilitate the photogenerated charge carrier transport across the absorber and its interfaces. This strategy provides unique insight into the underlying relationship between the stacking pattern of crystal planes, photogenerated charge carrier transport, and optoelectronic properties of solar cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {In Situ GISAXS Observation and Large Area Homogeneity Study of Slot-Die Printed PS-b-P4VP and PS-b-P4VP/FeCl3 Thin Films},

author = {S Yin and T Tian and C L Weindl and K S Wienhold and Q Ji and Y Cheng and Y Li and C M Papadakis and M Schwartzkopf and S V Roth and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsami.1c19797},

doi = {10.1021/acsami.1c19797},

issn = {1944-8244},

year  = {2022},

date = {2022-01-04},

urldate = {2022-01-04},

journal = {ACS Applied Materials \& Interfaces},

abstract = {Mesoporous hematite (α-Fe2O3) thin films with high surface-to-volume ratios show great potential as photoelectrodes or electrochemical electrodes in energy conversion and storage. In the present work, with the assistance of an up-scalable slot-die coating technique, locally highly ordered α-Fe2O3 thin films are successfully printed based on the amphiphilic diblock copolymer poly(styrene-b-4-vinylpyridine) (PS-b-P4VP) as a structure-directing agent. Pure PS-b-P4VP films are printed under the same conditions for comparison. The micellization of the diblock copolymer in solution, the film formation process of the printed thin films, the homogeneity of the dry films in the lateral and vertical direction as well as the morphological and compositional information on the calcined hybrid PS-b-P4VP/FeCl3 thin film are investigated. Because of convection during the solvent evaporation process, a similar dimple-type structure of vertically aligned cylindrical PS domains in a P4VP matrix developed for both printed PS-b-P4VP and hybrid PS-b-P4VP/FeCl3 thin films. The coordination effect between the Fe3+ ions and the vinylpyridine groups significantly affects the attachment ability of the P4VP chains to the silicon substrate. Accordingly, distinct feature sizes and homogeneity in the lateral direction, as well as the thicknesses in the perpendicular direction, are demonstrated in the two printed films. By removing the polymer template from the hybrid PS-b-P4VP/FeCl3 film at high temperature, a locally highly ordered mesoporous α-Fe2O3 film is obtained. Thus, a facile and up-scalable printing technique is presented for producing homogeneous mesoporous α-Fe2O3 thin films.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Morphology\textendashIonic Conductivity Relationship in Polymer\textendashTitania Hybrid Electrolytes for Lithium-Ion Batteries},

author = {S J Schaper and E Metwalli and M V Kaeppel and A Kriele and R Gilles and K N Raftopoulos and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1021/acsaem.1c03393},

doi = {10.1021/acsaem.1c03393},

year  = {2021},

date = {2021-12-14},

urldate = {2021-12-14},

journal = {ACS Applied Energy Materials},

volume = {4},

number = {12},

pages = {13438\textendash13443},

abstract = {The morphology and ionic conductivity of a high-molecular-weight polystyrene-block-poly(ethylene oxide) (PS-b-PEO) diblock copolymer (DBC) solid-state hybrid electrolyte, prepared entirely from solution, containing the lithium salt LiTFSI ([Li]/[EO] = 0.1) and titania (TiO2) nanoparticles (NP) were investigated at different temperatures. Structure investigation using small-angle X-ray scattering (SAXS) indicates a rupture of the DBC morphology upon increasing TiO2\textendashNP content, without a significant decrease in the ionic conductivity at high TiO2\textendashNP contents. A high number of unbound charge carriers in the hybrid DBC electrolyte, achieved by careful tuning of the materials’ ratios, is the most important contribution to a high ionic conductivity.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Biopolymer-Templated Deposition of Ordered and Polymorph Titanium Dioxide Thin Films for Improved Surface-Enhanced Raman Scattering Sensitivity},

author = {Q Chen and M Betker and C Harder and C J Brett and M Schwartzkopf and N M Ulrich and M E Toimil-Molares and C Trautmann and L D S\"{o}derberg and C L Weindl and V K\"{o}rstgens and P M\"{u}ller-Buschbaum and M Ma and S V Roth},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adfm.202108556},

doi = {https://doi.org/10.1002/adfm.202108556},

issn = {1616-301X},

year  = {2021},

date = {2021-10-27},

journal = {Adv. Funct. Mater.},

volume = {n/a},

number = {n/a},

pages = {2108556},

abstract = {Abstract Titanium dioxide (TiO2) is an excellent candidate material for semiconductor metal oxide-based substrates for surface-enhanced Raman scattering (SERS). Biotemplated fabrication of TiO2 thin films with a 3D network is a promising route for effectively transferring the morphology and ordering of the template into the TiO2 layer. The control over the crystallinity of TiO2 remains a challenge due to the low thermal stability of biopolymers. Here is reported a novel strategy of the cellulose nanofibril (CNF)-directed assembly of TiO2/CNF thin films with tailored morphology and crystallinity as SERS substrates. Polymorphous TiO2/CNF thin films with well-defined morphology are obtained by combining atomic layer deposition and thermal annealing. A high enhancement factor of 1.79 × 106 in terms of semiconductor metal oxide nanomaterial (SMON)-based SERS substrates is obtained from the annealed TiO2/CNF thin films with a TiO2 layer thickness of 10 nm fabricated on indium tin oxide (ITO), when probed by 4-mercaptobenzoic acid molecules. Common SERS probes down to 10 nm can be detected on these TiO2/CNF substrates, indicating superior sensitivity of TiO2/CNF thin films among SMON SERS substrates. This improvement in SERS sensitivity is realized through a cooperative modulation of the template morphology of the CNF network and the crystalline state of TiO2.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Degradation mechanisms of perovskite solar cells under vacuum and one atmosphere of nitrogen},

author = {R Guo and D Han and W Chen and L Dai and K Ji and Q Xiong and S Li and L K Reb and M A Scheel and S Pratap and N Li and S Yin and T Xiao and S Liang and A L Oechsle and C L Weindl and M Schwartzkopf and H Ebert and P Gao and K Wang and M Yuan and N C Greenham and S D Stranks and S V Roth and R H Friend and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1038/s41560-021-00912-8},

doi = {10.1038/s41560-021-00912-8},

issn = {2058-7546},

year  = {2021},

date = {2021-10-01},

urldate = {2021-10-01},

journal = {Nature Energy},

volume = {6},

number = {10},

pages = {977-986},

abstract = {Extensive studies have focused on improving the operational stability of perovskite solar cells, but few have surveyed the fundamental degradation mechanisms. One aspect overlooked in earlier works is the effect of the atmosphere on device performance during operation. Here we investigate the degradation mechanisms of perovskite solar cells operated under vacuum and under a nitrogen atmosphere using synchrotron radiation-based operando grazing-incidence X-ray scattering methods. Unlike the observations described in previous reports, we find that light-induced phase segregation, lattice shrinkage and morphology deformation occur under vacuum. Under nitrogen, only lattice shrinkage appears during the operation of solar cells, resulting in better device stability. The different behaviour under nitrogen is attributed to a larger energy barrier for lattice distortion and phase segregation. Finally, we find that the migration of excessive PbI2 to the interface between the perovskite and the hole transport layer degrades the performance of devices under vacuum or under nitrogen.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Stability of mixed-halide wide bandgap perovskite solar cells: Strategies and progress},

author = {L Tao and J Qiu and B Sun and X Wang and X Ran and L Song and W Shi and Q Zhong and P Li and H Zhang and Y Xia and P M\"{u}ller-Buschbaum and Y Chen},

url = {https://www.sciencedirect.com/science/article/pii/S2095495621001704},

doi = {https://doi.org/10.1016/j.jechem.2021.03.038},

issn = {2095-4956},

year  = {2021},

date = {2021-10-01},

journal = {Journal of Energy Chemistry},

volume = {61},

pages = {395-415},

abstract = {Benefiting from the superior optoelectronic properties and low-cost manufacturing techniques, mixed-halide wide bandgap (WBG) perovskite solar cells (PSCs) are currently considered as ideal top cells for fabricating multi-junction or tandem solar cells, which are designed to beyond the Shockley-Queisser (S-Q) limit of single-junction solar cells. However, the poor long-term operational stability of WBG PSCs limits their further employment and hinders the marketization of multi-junction or tandem solar cells. In this review, recent progresses on improving environmental stability of mixed-halide WBG PSCs through different strategies, including compositional engineering, additive engineering, interface engineering, and other strategies, are summarized. Then, the outlook and potential direction are discussed and explored to promote the further development of WBG PSCs and their applications in multi-junction or tandem solar cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating},

author = {S Pratap and F Babbe and N S Barchi and Z Yuan and T Luong and Z Haber and T-B Song and J L Slack and C V Stan and N Tamura and C M Sutter-Fella and P M\"{u}ller-Buschbaum},

url = {https://doi.org/10.1038/s41467-021-25898-5},

doi = {10.1038/s41467-021-25898-5},

issn = {2041-1723},

year  = {2021},

date = {2021-09-24},

journal = {Nature Communications},

volume = {12},

number = {1},

pages = {5624},

abstract = {Complex phenomena are prevalent during the formation of materials, which affect their processing-structure-function relationships. Thin films of methylammonium lead iodide (CH3NH3PbI3, MAPI) are processed by spin coating, antisolvent drop, and annealing of colloidal precursors. The structure and properties of transient and stable phases formed during the process are reported, and the mechanistic insights of the underlying transitions are revealed by combining in situ data from grazing-incidence wide-angle X-ray scattering and photoluminescence spectroscopy. Here, we report the detailed insights on the embryonic stages of organic-inorganic perovskite formation. The physicochemical evolution during the conversion proceeds in four steps: i) An instant nucleation of polydisperse MAPI nanocrystals on antisolvent drop, ii) the instantaneous partial conversion of metastable nanocrystals into orthorhombic solvent-complex by cluster coalescence, iii) the thermal decomposition (dissolution) of the stable solvent-complex into plumboiodide fragments upon evaporation of solvent from the complex and iv) the formation (recrystallization) of cubic MAPI crystals in thin film.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}