Publications

@article{nokey,

title = {A low-cost and high-energy aqueous potassium-ion battery},

author = {R L Streng and T Steeger and A Senyshyn and S Abel and P Schneider and C Benning and B M Naranjo and D Gryc and M Z Hussain and O Lieleg and M Elsner and A S Bandarenka and K Cicvari\'{c}},

url = {https://www.sciencedirect.com/science/article/pii/S2095495625001871},

doi = {https://doi.org/10.1016/j.jechem.2025.02.039},

issn = {2095-4956},

year  = {2025},

date = {2025-07-01},

journal = {Journal of Energy Chemistry},

volume = {106},

pages = {523-531},

abstract = {To address challenges related to the intermittency of renewable energy sources, aqueous potassium-ion batteries (AKIBs) are a promising and sustainable alternative to conventional systems for large-scale energy storage. To enable their practical application, maximizing energy density and longevity while minimizing production and material costs is a key goal. In this work, we propose an AKIB consisting only of abundant and cost-efficient materials, which delivers a high energy density of more than 70 Wh kg−1. We combine simple strategies to stabilize the Mn-rich Prussian blue analog cathode by Fe-doping, improving the crystallinity, and tuning the electrolyte composition without employing expensive water-in-salt electrolytes. Using a mixed 2.5 M Ca(NO3)2 + 1.5 M KNO3 electrolyte, we assemble a novel AKIB with a Fe-doped manganese hexacyanoferrate cathode and an organic poly(naphthalene-4-formyl-ethylenediamine) anode. Besides a high energy density, the full cell delivers a specific capacity of approximately 60 mA h g−1, a power density of 5000 W kg−1, and 80% capacity retention after 600 cycles.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Defect Imide Double Antiperovskites AE5AsPn(NH)2 (AE=Ca, Sr; Pn=Sb, Bi) as Potential Solar Cell Absorber Materials},

author = {T G Chau and D Han and F Wolf and S S Rudel and Y Yao and H Oberhofer and T Bein and H Ebert and W Schnick},

url = {https://doi.org/10.1002/anie.202500768},

doi = {https://doi.org/10.1002/anie.202500768},

issn = {1433-7851},

year  = {2025},

date = {2025-04-17},

journal = {Angewandte Chemie International Edition},

volume = {64},

number = {17},

pages = {e202500768},

abstract = {Abstract An abundance of oxide, halide and chalcogenide perovskites have been explored, demonstrating outstanding properties, while the emerging nitride perovskites are extremely rare due to their challenging synthesis requirements. By inverting the ion type in the perovskite structure, the corresponding antiperovskite structure is obtained. Among them, ternary antiperovskite nitrides X3AN (X=Ba, Sr, Ca, Mg; A=As, Sb) have recently been identified as exhibiting excellent optoelectronic properties. To explore the unrealized composition space of nitride perovskites, the ammonothermal method was applied, yielding three new layered quaternary imide-based defect-antiperovskites, namely AE5AsPn(NH)2 (AE=Ca, Sr; Pn=Sb, Bi). These new compounds feature distorted square-pyramidal coordination around the imide-group (Ca5NH). Layers with Ca2+ vacancies are found with an alternating As3? and Pn3? (Pn3?=Sb3?, Bi3?) coordination along the A-site, forming a two-dimensional (2D) structure. All three AE5AsPn(NH)2 compounds show suitable direct band gaps within the visible light spectrum. Density functional theory calculations reveal favorable band dispersion, as well as transport and optical properties, especially along the out-of-plane direction, demonstrating their 3D character of electronic transport. The narrow tunable direct band gaps and favorable charge carrier properties make AE5AsPn(NH)2 promising candidates for solar cell absorber materials.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Controlling the Morphology and Electrochemical Properties of Electrodeposited Nickel Hexacyanoferrate},

author = {T Steeger and R L Streng and A Senyshyn and V Dyadkin and X Lamprecht and R List and A S Bandarenka},

url = {https://doi.org/10.1002/celc.202500073},

doi = {https://doi.org/10.1002/celc.202500073},

issn = {2196-0216},

year  = {2025},

date = {2025-04-14},

journal = {ChemElectroChem},

volume = {n/a},

number = {n/a},

pages = {2500073},

abstract = {In recent years, Prussian blue analogs (PBAs) have gained significant attention due to their broad applicability. The synthesis routines of this material class have been shown to allow for great tunability by varying the corresponding parameters. The control of crystal phase, defect, and water content, as well as electrochemical properties, have been studied extensively for the state-of-the-art coprecipitation method. In turn, electrochemical deposition, which is particularly suited for thin-film production, remains mainly underexplored. This study investigates the effects of synthesis temperature, scan rate, precursor concentration, and supporting electrolyte pH on nickel hexacyanoferrate (NiHCF) films electrodeposited onto a high surface area carbon-based substrate via cyclic voltammetry. Electrochemical analysis and morphological characterization reveal that higher deposition temperatures increase cation-specific capacity, influence NiHCF coverage, and promote larger, more crystalline structures. Scan rate, precursor concentration, and pH variations further demonstrate the correlation between deposition parameters, crystallite size, and NiHCF structure. These findings highlight the tunability of electrodeposited PBAs for tailored electrochemical performance and morphology.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Non-Precious Metal Catalysts with Gradient Oxidative Dual Sites Boost Bimolecular Activation for Catalytic Oxidation Reactions},

author = {Y Wang and T Lan and L Han and E Pensa and Y Shen and X Li and Z Xu and X Chen and M Wang and X Xue and Y Li and M Xie and E Cort\'{e}s and D Zhang},

url = {https://doi.org/10.1002/anie.202506018},

doi = {https://doi.org/10.1002/anie.202506018},

issn = {1433-7851},

year  = {2025},

date = {2025-04-09},

journal = {Angewandte Chemie International Edition},

volume = {n/a},

number = {n/a},

pages = {e202506018},

abstract = {Abstract Catalytic oxidation emerges as a highly promising and cost-effective approach for eliminating gaseous pollutants, greenhouse gases, and volatile organic compounds (VOCs) from industrial exhaust streams. However, achieving the simultaneous activation of O2 and substrate molecules at low temperatures using non-precious metal catalysts remains a significant challenge. In this study, we introduce gradient oxidative Cu─O─Ti/Cu─O─Cu dual sites that enhance bimolecular activation for catalytic oxidation reactions. The catalyst, Ti-doped CuO, is synthesized on a TiO2 support through the immobilization of Cu2? on NO3?-grafted TiO2, followed by thermal treatment. The resulting gradient oxidative Cu─O─Ti/Cu─O─Cu sites exhibit exceptional catalytic oxidation activity for NH3 and various VOCs at low temperatures, matching the performance of precious metal-based catalysts. Notably, during NH? oxidation, Cu─O─Ti sites enhance the activation of both O? and NH?. HNO intermediates formed on Cu─O─Ti sites react with NH intermediates on neighboring Cu─O─Cu sites?producing N? and H?O via an imide mechanism?which effectively lowers the reaction barrier for catalytic NH? oxidation. As such, dual sites in non-precious metal catalysts show promising results for advancing future catalytic oxidation technologies.},

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 = {Locking in Color: Stable RGB Perovskite Nanocrystal Films via UV Cross-Linking},

author = {P Ganswindt and I Tepfenhart and A Singldinger and A Abfalterer and L Spies and E Kostyurina and M Stadler and B Nickel and A S Urban},

url = {https://doi.org/10.1002/adom.202500166},

doi = {https://doi.org/10.1002/adom.202500166},

issn = {2195-1071},

year  = {2025},

date = {2025-04-07},

journal = {Advanced Optical Materials},

volume = {n/a},

number = {n/a},

pages = {2500166},

abstract = {Abstract Perovskite nanocrystals have positioned themselves at the forefront of next-generation emitter applications due to their extraordinary optoelectronic properties, which include widely tunable narrow emission spectra and low-cost syntheses. However, stability issues and halide ion exchange inhibit the realization of heterostructures, severely limiting their applicability and decelerating their commercialization. Here, a block copolymer templated halide perovskite nanocrystal synthesis with a post-synthetic treatment is combined with UV-C light to obtain ultra-stable thin film emitters. The UV light induces cross-linking between the polymer strands, thereby rendering them insoluble to the organic solvent and nearly impervious to halide ion diffusion while retaining the nanocrystals? optical properties. This method enabled the fabrication of an all-perovskite nanocrystal white light-emitting thin film. The resulting films feature narrow linewidths (\<95 meV) for each RGB emission peak. Additionally, the color temperature of the ?white? light can be tuned with a color gamut approximating the Rec. 2020 standard. These RGB-emissive phosphor films can be combined with commercial UV or blue LED backlights to create the next-generation high-efficiency, high-quality phosphor-converted white LEDs or color displays.},

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 = {DNA origami signal amplification in lateral flow immunoassays},

author = {H Ij\"{a}s and J Trommler and L Nguyen and S Van Rest and P C Nickels and T Liedl and M J Urban},

url = {https://doi.org/10.1038/s41467-025-57385-6},

doi = {10.1038/s41467-025-57385-6},

issn = {2041-1723},

year  = {2025},

date = {2025-04-04},

journal = {Nature Communications},

volume = {16},

number = {1},

pages = {3216},

abstract = {Lateral flow immunoassays (LFIAs) enable a rapid detection of analytes in a simple, paper-based test format. Despite their multiple advantages, such as low cost and ease of use, their low sensitivity compared to laboratory-based testing limits their use in e.g. many critical point-of-care applications. Here, we present a DNA origami-based signal amplification technology for LFIAs. DNA origami is used as a molecularly precise adapter to connect detection antibodies to tailored numbers of signal-generating labels. As a proof of concept, we apply the DNA origami signal amplification in a sandwich-based LFIA for the detection of cardiac troponin I (cTnI) in human serum. We show a 55-fold improvement of the assay sensitivity with 40-nm gold nanoparticle labels and an adjustable signal amplification of up to 125-fold with fluorescent dyes. The technology is compatible with a wide range of existing analytes, labels, and sample matrices, and presents a modular approach for improving the sensitivity and reliability of lateral flow testing.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {The Interaction of Sub-Monolayer Ta Adatoms and Clusters with Oxygen at the Pt(111) Interface},

author = {K Bertrang and T Hinke and S Kaiser and M Knechtges and F Loi and P Lacovig and M Jahangirzadeh Varjovi and F Esch and A Baraldi and S Tosoni and A Kartouzian and U Heiz},

url = {https://doi.org/10.1021/acs.jpcc.5c00699},

doi = {10.1021/acs.jpcc.5c00699},

issn = {1932-7447},

year  = {2025},

date = {2025-04-03},

journal = {The Journal of Physical Chemistry C},

volume = {129},

number = {13},

pages = {6511-6523},

abstract = {The interaction of submonolayer quantities of size-selected and soft-landed Tan (n = 4, 5, 6, 8, 13) clusters with Pt(111) is investigated employing high-resolution X-ray photoelectron spectroscopy (HR-XPS), scanning tunneling microscopy (STM), and density functional theory (DFT) simulations. The deposited clusters are monodispersed and stable under ultrahigh vacuum (UHV) conditions at 40 K. They display a size-specific trend in photoemission spectra, which is reasoned in terms of the distinct in plane coordination of Ta atoms in the clusters. Both the Ta coordination number and distance from the Pt surface influence its Bader charge and, accordingly, the oxidation state of the atoms in the Ta cluster. They already fragment in the presence of low amounts of oxygen and form a common oxidation product observed for all cluster sizes. Based on our observations, we propose an oxidation mechanism in the example of Ta8 clusters, which is closely comparable to the one discussed in gas-phase studies on the oxidation of cationic Ta clusters of similar size. Concomitant to oxidation-induced fragmentation, the agglomeration into Ta-oxide islands with Ta in an oxidation state of +5 is observed. However, the strong interaction with the Pt surface leads to Ta 4f orbital photoemission features that differ from those commonly observed for Ta2O5. Computational insights concerning the structure of the Ta-oxide islands indicate flat agglomerates that agree with STM observations. They suggest distinct Ta 4f photoemission contributions from interfacial and surface-related Ta configurations. The respective HR-XPS spectra display specific core-level shifts as a function of bonding configuration and vicinity to the Pt surface. By annealing at 900 K in UHV, we observe oxygen loss and concomitant intermixing of Ta atoms with the Pt subsurface lattice to which results in the formation of a Ta\textendashPt alloy. These species, Ta-oxide islands, and Ta\textendashPt alloy, can reversibly interconvert by oxidative surface segregation and reductive intermixing.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction},

author = {Q Wang and T Luo and X Cao and Y Gong and Y Liu and Y Xiao and H Li and F Gr\"{o}bmeyer and Y-R Lu and T-S Chan and C Ma and K Liu and J Fu and S Zhang and C Liu and Z Lin and L Chai and E Cortes and M Liu},

url = {https://doi.org/10.1038/s41467-025-57464-8},

doi = {10.1038/s41467-025-57464-8},

issn = {2041-1723},

year  = {2025},

date = {2025-03-27},

journal = {Nature Communications},

volume = {16},

number = {1},

pages = {2985},

abstract = {Single-atom catalysts (SACs) have received increasing attention due to their 100% atomic utilization efficiency. The electrochemical CO2 reduction reaction (CO2RR) to CO using SAC offers a promising approach for CO2 utilization, but achieving facile CO2 adsorption and CO desorption remains challenging for traditional SACs. Instead of singling out specific atoms, we propose a strategy utilizing atoms from the entire lanthanide (Ln) group to facilitate the CO2RR. Density functional theory calculations, operando spectroscopy, and X-ray absorption spectroscopy elucidate the bridging adsorption mechanism for a representative erbium (Er) single-atom catalyst. As a result, we realize a series of Ln SACs spanning 14 elements that exhibit CO Faradaic efficiencies exceeding 90%. The Er catalyst achieves a high turnover frequency of ~130,000 h−1 at 500 mA cm−2. Moreover, 34.7% full-cell energy efficiency and 70.4% single-pass CO2 conversion efficiency are obtained at 200 mA cm−2 with acidic electrolyte. This catalytic platform leverages the collective potential of the lanthanide group, introducing new possibilities for efficient CO2-to-CO conversion and beyond through the exploration of unique bonding motifs in single-atom catalysts.},

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 = {Redox-Active Microporous Covalent Organic Frameworks for Additive-Free Supercapacitors},

author = {R Guntermann and J M Rotter and A Singh and D D Medina and T Bein},

url = {https://doi.org/10.1002/smsc.202400585},

doi = {https://doi.org/10.1002/smsc.202400585},

year  = {2025},

date = {2025-03-21},

journal = {Small Science},

volume = {n/a},

number = {n/a},

pages = {2400585},

abstract = {2D covalent organic frameworks (COFs) have garnered significant attention by virtue of their porous nature, structural tunability, and ability to incorporate highly reversible redox-active groups. These characteristics qualify them for a range of energy storage devices, including supercapacitors, which can assume a pivotal role towards attaining a more sustainable future amid escalating energy needs. Herein, two 2D COFs are reported containing wurster (W) and pyrene (PY) units, WW COF and WPy-I COF, which demonstrate reversible redox behavior and characteristic pseudocapacitance. Both COFs exhibit high crystallinity demonstrated with X-ray diffraction analysis, exhibiting a thermal dependence of the intralayer bonding and interlayer stacking arrangement from WPy-I toward WPy-II COFs. Additionally, the WW and WPy-I COFs were grown on glass and stainless-steel meshes (SSMs) featuring different surface coatings. These coated SSMs proved suitable as current collectors for testing the COFs regarding their specific capacitance, without the need to add any conducting additives, revealing a promising capacitance of 48.9?F?g?1 for the WW COF. Moreover, these electrodes can be applied in symmetrical supercapacitor devices with an ionic liquid serving as electrolyte. The remarkable performance of the redox-active Wurster unit identifies it as a promising building motif for COFs with high specific capacitance, even in devices devoid of carbon additives.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {High-pressure pump\textendashprobe experiments reveal the mechanism of excited-state proton-coupled electron transfer and a shift from stepwise to concerted pathways},

author = {D Langford and R Rohr and S Bauroth and A Zahl and A Franke and I Ivanovi\'{c}-Burmazovi\'{c} and D M Guldi},

url = {https://doi.org/10.1038/s41557-025-01772-5},

doi = {10.1038/s41557-025-01772-5},

issn = {1755-4349},

year  = {2025},

date = {2025-03-20},

journal = {Nature Chemistry},

abstract = {Chemical energy conversion and storage in natural and artificial systems rely on proton-coupled electron transfer (PCET) processes. Concerted proton-electron transfer (CPET) can provide kinetic advantages over stepwise processes (electron transfer (ET)/proton transfer (PT) or PT/ET), so understanding how to distinguish and modulate these processes is important for their associated applications. Here, we examined PCET from the excited state of a ruthenium complex under high pressures. At lower buffer or quencher concentrations, a stepwise PT/ET mechanism was observed. With increasing pressure, PT slowed and ET sped up, indicating a merging of the two steps. In contrast, CPET at higher concentrations of buffer or quencher showed no pressure dependence of the reaction rate. This is because the simultaneous transfer of electrons and protons circumvents changes in charges and, consequently, in solvent electrostriction during the transition state. Our findings demonstrate that pressure can serve as a tool to monitor charge changes along PCET pathways, aiding in the identification of its mechanisms.},

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 = {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 = {Competition Between One- and Two-Electron Unimolecular Reactions of Late 3d-Metal Complexes [(Me3SiCH2)nM]\textendash (M = Fe, Co, Ni, Cu; n = 2 \textendash 4)},

author = {T K\"{u}hl and L Hetzel and C J Stein and K Koszinowski},

url = {https://doi.org/10.1002/anie.202500524},

doi = {https://doi.org/10.1002/anie.202500524},

issn = {1433-7851},

year  = {2025},

date = {2025-03-15},

journal = {Angewandte Chemie International Edition},

volume = {n/a},

number = {n/a},

pages = {e202500524},

abstract = {Although organometallic complexes of the late 3d elements are known to undergo both one- and two-electron reactions, their relative propensities to do so remain poorly understood. To gain direct insight into the competition between these different pathways, we have analyzed the unimolecular gas-phase reactivity of a series of well-defined model complexes [(Me3SiCH2)nM]? (M = Fe, Co, Ni, Cu; n = 2 ? 4). Applying a combination of tandem-mass spectrometry, quantum-chemical computations, and statistical rate theory calculations, we find several different fragmentation reactions, among which the homolytic cleavage of metal-carbon bonds and radical dissociations are particularly prominent. In all cases, these one-electron reactions are entropically favored. For the ferrate and cobaltate complexes, they are also energetically preferred, which explains their predominance in the corresponding fragmentation experiments. For [(Me3SiCH2)4Ni]? and, even more so, for [(Me3SiCH2)4Cu]?, a concerted reductive elimination as a prototypical two-electron reaction is energetically more favorable and gains in importance. [(Me3SiCH2)3Ni]? is special in that it has two nearly degenerate spin states, both of which react in different ways. A simple thermochemical analysis shows that the relative order of the first and second bond-dissociation energies is of key importance in controlling the competition between radical dissociations and concerted reductive eliminations.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Process cost analysis of performance challenges and their mitigations in sodium-ion battery cathode materials},

author = {M Munjal and T Prein and M M Ramadan and H B Smith and V Venugopal and J L M Rupp and I I Abate and E A Olivetti and K J Huang},

url = {https://www.sciencedirect.com/science/article/pii/S2542435125000522},

doi = {https://doi.org/10.1016/j.joule.2025.101871},

issn = {2542-4351},

year  = {2025},

date = {2025-03-14},

journal = {Joule},

pages = {101871},

abstract = {Summary The success of sodium-ion batteries (SIBs) hinges on mitigating underperformance in ways that are cost effective, manufacturable, and scalable. This work investigates interfacial, morphological, and bulk interventions to enhance the performance of layered metal oxide cathode active materials (CAMs) for SIBs. We mapped the full space of literature-reported SIB CAM challenges and their mitigations. We then estimated the manufacturing costs for a diverse and representative set of mitigation approaches. Adding sacrificial salts can be cost effective, given low materials costs and minimal process changes. By contrast, many methods are reported to tune CAM morphology. Several are likely challenging at scale due to process throughput and yield limitations. Finally, bulk modifications can mitigate the moisture sensitivity of some CAMs, a likely less costly route than expanding stringent atmosphere controls during manufacturing. We end by discussing the limits and promise of process cost analysis, given the current state of battery reporting in the literature.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Chiral Plasmonic Crystals Self-Assembled by DNA Origami},

author = {C Sikeler and S Kempter and I Sekulic and S Burger and T Liedl},

url = {https://doi.org/10.1021/acs.jpcc.4c08768},

doi = {10.1021/acs.jpcc.4c08768},

issn = {1932-7447},

year  = {2025},

date = {2025-03-13},

journal = {The Journal of Physical Chemistry C},

volume = {129},

number = {10},

pages = {5116-5121},

abstract = {Periodic lattices of high refractive index materials manipulate light in exceptional manners. Resulting remarkable properties range from photonic band gaps to chiral active matter, which critically depend on parameters of crystal lattices such as the unit cell, lattice type, and periodicity. In self-assembled materials, the lattice properties are inherited by the geometry and size of the macromolecules or colloidal particles assembling the unit cell. DNA origami allows for excellent control over the size and shape of assembled macromolecules while simultaneously allowing control over the interaction between them and ultimately the crystal’s structure. Here, we present the assembly of chiral, rhombohedral crystals in one, two, and three dimensions built by a DNA origami tensegrity triangle. Subsequent modification of the lattice with gold nanorods converts the lattices into chiral plasmonic metamaterials active in the visible and near-infrared spectral range. We demonstrate their chiral activity and corroborate the experimental results with simulated data.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Effective Electron-Vibration Coupling by Ab Initio Methods},

author = {M F X Dorfner and F Ortmann},

url = {https://doi.org/10.1021/acs.jctc.4c01608},

doi = {10.1021/acs.jctc.4c01608},

issn = {1549-9618},

year  = {2025},

date = {2025-03-11},

journal = {Journal of Chemical Theory and Computation},

volume = {21},

number = {5},

pages = {2371-2385},

abstract = {The description of electron\textendashphonon coupling in materials is complex, with varying definitions of coupling constants in the literature and different theoretical approaches available. This article analyzes different levels of theory to introduce and compute these coupling constants. Within the quasi-particle picture, we derive an effective linear-coupling Hamiltonian, describing the interaction of electronic quasi-particles with vibrations. This description allows a comparison between coupling constants computed using density functional theory and higher-level quasi-particle approaches by identifying the Kohn\textendashSham potential as an approximation to the frequency-independent part of the self-energy. We also investigate their dependence on the exchange-correlation (XC) functional. Despite significant deviations of the Kohn\textendashSham eigenvalues, which arise from different XC functionals, the resulting coupling constants are remarkably similar. A comparison to quasi-particle methods, such as the well-established G0W0 approach, reveals significant quasi-particle weight renormalization. Surprisingly, however, in nearly all the considered cases, the coupling constants computed in the DFT framework are excellent approximates of the ones in the quasi-particle framework, which is traced back to a significant cancellation of competing terms. Other quasi-particle methods, such as the Outer Valence Green’s Function approach and the ΔSCF method, are also included in the comparison. Moreover, we investigate the coupling of vibrations to excitonic excitations and find, by comparison to time-dependent density functional theory and extended multiconfiguration quasi-degenerate second-order perturbation theory, that knowing the underlying electron- and hole-vibration couplings is sufficient to accurately determine the exciton-vibration coupling constants in the studied cases.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Upconversion Nanoparticle-Covalent Organic Framework Core\textendashshell Particles as Therapeutic Microrobots Trackable With Optoacoustic Imaging},

author = {D W Kim and P Wrede and A Rodr\'{i}guez-Camargo and Y Chen and N O Dogan and C Gl\"{u}ck and B V Lotsch and D Razansky and M Sitti},

url = {https://doi.org/10.1002/adma.202418425},

doi = {https://doi.org/10.1002/adma.202418425},

issn = {0935-9648},

year  = {2025},

date = {2025-03-07},

journal = {Advanced Materials},

volume = {n/a},

number = {n/a},

pages = {2418425},

abstract = {Abstract Despite the development of various medical imaging contrast agents, integrating contrast signal generation with therapeutic and microrobotic functions remains challenging without complicated fabrication processes. In this study, upconversion nanoparticle-covalent organic framework (UCNP-COF) core?shell sub-micron particles are developed that function as therapeutic microrobots trackable with multi-spectral optoacoustic tomography (MSOT) imaging and can be loaded with desired therapeutic molecular agents in a customizable manner. The mechanism of optoacoustic signal generation in UCNP-COF particles is attributed to the quenching of upconversion luminescence emitted by the UCNPs, which is absorbed by the encapsulating COF and subsequently converted into acoustic waves. Unlike other microparticulate agents previously imaged with MSOT, UCNP-COF particles do not pose concerns about their stability and biocompatibility. Simultaneously, the mesoporous texture of the COF provides a large surface area, allowing for the efficient loading of various drug molecules, which can be released at target sites. Furthermore, the magnetic UCNP-COF Janus particles can be magnetically navigated through in vivo vasculature while being visualized in real-time with volumetric MSOT. This study proposes an approach to design photonic materials with multifunctionality, enabling high-performance medical imaging, drug delivery, and microrobotic manipulation toward their future potential clinical use.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Designing Atomically Precise and Robust COF Hybrids for Efficient Photocatalytic CO₂ Reduction},

author = {L Spies and M E G Carmo and M D\"{o}blinger and Z Xu and T Xue and A Hartschuh and T Bein and J Schneider and A O T Patrocinio},

url = {https://doi.org/10.1002/smll.202500550},

doi = {https://doi.org/10.1002/smll.202500550},

issn = {1613-6810},

year  = {2025},

date = {2025-03-03},

journal = {Small},

volume = {n/a},

number = {n/a},

pages = {2500550},

abstract = {Abstract Hybrid photocatalysts based on molecular species and solid substrates are elegant solutions for improving the performance and stability of molecular catalytic systems aiming at solar-driven CO2 conversion. In this work, a new dibenzochrysene-based covalent organic framework (COF) is developed to accept ReI centers, keeping its high crystallinity and allowing for atomistic control of the position of the catalytic centers. The rigid structure of the COF leads to long-term stability under illumination, whereas the efficient light-harvesting capability and the strong electronic interactions between the COF and the ReI centers lead to CO evolution rates of up to 1.16 mmol g?1 h?1. The favorable photocatalytic performance of this novel ReI-COF offers new insights regarding the development of efficient photocatalytic hybrid systems.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Integrating Automated Electrochemistry and High-Throughput Characterization with Machine Learning to Explore Si─Ge─Sn Thin-Film Lithium Battery Anodes},

author = {A Sanin and J K Flowers and T H Piotrowiak and F Felsen and L Merker and A Ludwig and D Bresser and H S Stein},

url = {https://doi.org/10.1002/aenm.202404961},

doi = {https://doi.org/10.1002/aenm.202404961},

issn = {1614-6832},

year  = {2025},

date = {2025-03-01},

journal = {Advanced Energy Materials},

volume = {15},

number = {11},

pages = {2404961},

abstract = {Abstract High-performance batteries need accelerated discovery and optimization of new anode materials. Herein, we explore the Si─Ge─Sn ternary alloy system as a candidate fast-charging anode materials system by utilizing a scanning droplet cell (SDC) as an autonomous electrochemical characterization tool with the goal of subsequent upscaling. As the SDC is performing experiments sequentially, an exploration of the entire ternary space is unfeasible due to time constraints. Thus, closed-loop optimization, guided by real-time data analysis and sequential learning algorithms, is utilized to direct experiments. The lead material identified is scaled up to a coin cell to validate the findings from the autonomous millimeter-scale thin-film electrochemical experimentation. Explainable machine learning (ML) models incorporating data from high-throughput Raman spectroscopy and X-ray diffraction (XRD) are used to elucidate the effect of short and long-range ordering on material performance.},

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 = {Metal vacancies in semiconductor oxides enhance hole mobility for efficient photoelectrochemical water splitting},

author = {J Wang and K Liu and W Liao and Y Kang and H Xiao and Y Chen and Q Wang and T Luo and J Chen and H Li and T-S Chan and S Chen and E Pensa and L Chai and F Liu and L Jiang and C Liu and J Fu and E Cort\'{e}s and M Liu},

url = {https://doi.org/10.1038/s41929-025-01300-1},

doi = {10.1038/s41929-025-01300-1},

issn = {2520-1158},

year  = {2025},

date = {2025-03-01},

journal = {Nature Catalysis},

volume = {8},

number = {3},

pages = {229-238},

abstract = {Achieving efficient carrier separation in transition-metal-oxide semiconductors is crucial for their applications in optoelectronic and catalytic devices. However, the substantial disparity in mobility between holes and electrons heavily limits device performance. Here we develop a general strategy for enhancing hole mobility via reducing their effective mass through metal vacancy (VM) management. The introduction of VM yields remarkable improvements in hole mobility: 430% for WO3, 350% for TiO2 and 270% for Bi2O3. To illustrate the importance of this finding, we applied the VM concept to photoelectrochemical water splitting, where efficient carrier separation is highly coveted. In particular, VM-WO3 achieves a 4.4-fold enhancement in photo-to-current efficiency, yielding a performance of 4.8 mA cm−2 for both small- and large-scale photoelectrodes with exceptional stability for over 120 h.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Catalytic Hydrolysis of Perfluorinated Compounds in a Yolk\textendashShell Micro-Reactor},

author = {J Zheng and X Wang and X Zi and H Zhang and H Chen and E Pensa and K Liu and J Fu and Z Lin and L Chai and E Cort\'{e}s and M Liu},

url = {https://doi.org/10.1002/advs.202413203},

doi = {https://doi.org/10.1002/advs.202413203},

issn = {2198-3844},

year  = {2025},

date = {2025-03-01},

journal = {Advanced Science},

volume = {12},

number = {9},

pages = {2413203},

abstract = {Abstract Perfluorinated compounds (PFCs) are emerging environmental pollutants characterized by their extreme stability and resistance to degradation. Among them, tetrafluoromethane (CF4) is the simplest and most abundant PFC in the atmosphere. However, the highest C─F bond energy and its highly symmetrical structure make it particularly challenging to decompose. In this work, a yolk?shell Al2O3 micro-reactor is developed to enhance the catalytic hydrolysis performance of CF4 by creating a local autothermic environment. Finite element simulations predict that the yolk?shell Al2O3 micro-reactor captures the heat released during the catalytic hydrolysis of CF4, resulting in a local autothermic environment within the yolk?shell structure that is 50 °C higher than the set temperature. The effectiveness of this local autothermic environment is experimentally confirmed by in situ Raman spectroscopy. As a result, the obtained yolk?shell Al2O3 micro-reactor achieves 100% CF4 conversion at a considerably low temperature of 580 °C for over 150 h, while hollow and solid Al2O3 structures required higher temperatures of 610 and 630 °C, respectively, to achieve the same conversion rate, demonstrating the potential of yolk?shell Al2O3 micro-reactor to significantly reduce the energy requirements for PFCs degradation and contribute to more sustainable and effective environmental remediation strategies.},

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 = {Printed CsMg\textendashZnO ETLs achieve over 9 % efficiency in PbS quantum dot solar cells},

author = {R Holfeuer and C Maheu and H Illner and R Hoojier and H Balakrishnan and B M\"{a}rz and S Lotfi and H Sezen and K M\"{u}ller-Caspary and T Bein and J P Hofmann and T Ameri and A Hartschuh and A Yousefiamin},

url = {https://www.sciencedirect.com/science/article/pii/S2468606925000218},

doi = {https://doi.org/10.1016/j.mtener.2025.101813},

issn = {2468-6069},

year  = {2025},

date = {2025-03-01},

journal = {Materials Today Energy},

volume = {48},

pages = {101813},

abstract = {Zinc oxide (ZnO) is a key electron transport layer (ETL) material in next-generation lead sulfide (PbS) colloidal quantum dot solar cells (CQDSCs) due to its high transparency, strong exciton binding energy, and good electron mobility. Here, we demonstrate a scalable doctor-blading printing protocol for ZnO ETLs that integrates dual defect passivation with magnesium (Mg2⁺) and caesium (Cs⁺) and employs solvent engineering to achieve uniform, defect-minimized films. Using a ternary solvent blend (methanol, chloroform, and 2-methoxyethanol) optimizes the ink's viscosity and boiling point, preventing particle migration and ensuring full substrate coverage. Our modified ZnO ink leads to improved crystallinity, smoother surfaces, and reduced trap states, boosting the fill factor (FF) and short-circuit current (Jsc). Consequently, we achieve a power conversion efficiency increase from 5.98 % to 9.53 % using a printed CsMg-ZnO film. Notably, 80 % of dual-doped devices exceeded 7.5 % efficiency, demonstrating high reproducibility and reliability. This performance enhancement underscores the effectiveness of dual metal ion treatment and solvent engineering strategies in overcoming printability challenges. Moreover, the compatibility of our approach with low-temperature processing and established coating techniques paves the way for seamless integration into large-scale manufacturing, bringing PbS CQDSCs closer to commercial viability.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Coupled Nuclear and Electron Dynamics in Chlorophyll Unraveled by XMS-CASPT2 X-ray Absorption Spectra},

author = {L B\"{a}uml and R De Vivie-Riedle},

url = {https://doi.org/10.1021/acs.jpcb.4c07787},

doi = {10.1021/acs.jpcb.4c07787},

issn = {1520-6106},

year  = {2025},

date = {2025-02-27},

journal = {The Journal of Physical Chemistry B},

volume = {129},

number = {8},

pages = {2159-2167},

abstract = {Attosecond spectroscopy, especially time-resolved X-ray absorption spectra (XAS), enables direct observation of ultrafast molecular dynamics. The complementary and even preceding development of theoretical simulations can offer the necessary guidance and stimulate new experiments. In this work, we simulated high-level XAS for the magnesium and nitrogen K-edge of chlorophyll a. In our previous work on the ultrafast relaxation process in the Q-band, our quantum dynamics simulations found the Qx and Qy states to be energetically close and therefore strongly coupled. Here, we analyze the strong coupling between Qx and Qy via XAS, indicating promising possibilities for experimental observation. The excited-state energies, potential energy surfaces, and XAS are computed at the XMS-CASPT2 level of theory to capture the complex multireference character of chlorophyll excitations. In our simulated spectra, we could follow the ultrafast population transfer between Qx and Qy and thus draw conclusions about the strong vibrational coupling between them.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Aberration measurement by electron ptychography and consistency among different algorithms},

author = {T Lorenzen and B Diederichs and C Otieno Ogolla and B Butz and K M\"{u}ller-Caspary},

url = {https://doi.org/10.1063/5.0238580},

doi = {10.1063/5.0238580},

issn = {0003-6951},

year  = {2025},

date = {2025-02-24},

journal = {Applied Physics Letters},

volume = {126},

number = {8},

pages = {081602},

abstract = {Control over and knowledge of the electron probe is important in all scanning transmission electron microscopy (STEM) techniques. This is emphasized especially in electron ptychography, where the accurate probe wave function is required to deconvolve illumination from the specimen. The majority of ptychographic algorithms, such as the extended ptychographic iterative engine, reconstruct the electron probe on a pixelated grid numerically self-consistently. Solutions are thus not necessarily bound to wave functions physically realizable by the optical system. A method is presented to characterize reconstructed probes by conventional lens aberrations. The fitted aberrations are then used to investigate the quality of the retrieved probes, and their consistency is examined in a systematic study using a 4D-STEM focal series recorded for a thin SnS2 2D flake. Additionally, the influences of partial coherence and limited electron dose on the retrieved probes are analyzed, and the usefulness of the retrieved probes for different ptychographic methods, such as single sideband, Wigner distribution deconvolution ptychography, and gradient descent-based schemes, is elucidated. Finally, applications for ptychography-driven alignments of aberration-correcting electron optics are outlined.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Hot carrier dynamics in III\textendashV semiconductor nanowires under dominant radiative and Auger recombination},

author = {H Esmaielpour and P Schmiedeke and N Isaev and C Doganlar and M D\"{o}blinger and J J Finley and G Koblm\"{u}ller},

url = {https://doi.org/10.1063/5.0248247},

doi = {10.1063/5.0248247},

issn = {0003-6951},

year  = {2025},

date = {2025-02-24},

journal = {Applied Physics Letters},

volume = {126},

number = {8},

pages = {083505},

abstract = {One-dimensional structures such as nanowires (NWs) show great promise in tailoring the rates of hot carrier thermalization in semiconductors with important implications for the design of efficient hot carrier absorbers. However, the fabrication of defect-free crystal structures and control of their intrinsic electronic properties can be challenging, raising concerns about the role of competing radiative and non-radiative recombination mechanisms that govern hot carrier effects. Here, we elucidate the impact of crystal purity and altered electronic properties on the hot carrier properties by comparing two classes of III\textendashV semiconductor NW arrays with similar bandgap energies and geometries, yet different crystal quality: one composed of GaAsSb NWs, which host antisite point defects but are free of planar stacking defects, and the other InGaAs NWs with a very high density of stacking defects. Photoluminescence spectroscopy demonstrates distinct hot carrier effects in both NW arrays; however, the InGaAs NWs exhibit stronger hot carrier effects, as evidenced by increased carrier temperature under identical photo-absorptivity. This difference arises from higher rates of Auger recombination in the InGaAs NWs due to their increased n-type conductivity, as confirmed by excitation power-dependent measurements. Our findings suggest that while enhancing material properties is crucial for improving the performance of hot carrier absorbers, optimizing conditions to increase the rates of Auger recombination will further boost the efficiency of these devices.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Synthesis of micrometre-thick oriented 2D covalent organic framework films by a kinetic polymerization pathway},

author = {L Cusin and P Cieci\'{o}rski and S Van Gele and F Heck and S Krause and P W Majewski and B V Lotsch and W Danowski and P Samor\`{i}},

url = {https://doi.org/10.1038/s44160-025-00741-7},

doi = {10.1038/s44160-025-00741-7},

issn = {2731-0582},

year  = {2025},

date = {2025-02-20},

journal = {Nature Synthesis},

abstract = {Despite advances in the field of 2D polymerization, the synthesis of high-quality, micrometre-thick films of oriented 2D covalent organic frameworks (COFs) remains challenging. Conventional approaches focusing on thermodynamic control of the polymerization pathway face a detrimental trade-off between orientation and thickness. Here we describe a straightforward method for preparing imine-linked 2D COF films with a near-perfect face-on orientation by leveraging kinetically trapped amorphous 3D covalent adaptable network (CAN) intermediates. These off-pathway intermediates are generated as coatings through solution casting, during which the CANs spontaneously align to relax tensile stresses induced by solvent evaporation. A subsequent lift-off process, followed by an amorphous-to-crystalline transformation under solvothermal conditions, converts the 3D-oriented polymer networks into thermodynamically stable, porous and free-standing 2D COF films. This versatile kinetic trapping strategy is suitable for a range of building blocks and network topologies, constituting a convenient synthetic tool for accessing high-quality, robust, large-area 2D COF films with a strongly aligned polycrystalline structure.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Influence of the Electrolyte pH on the Double Layer Capacitance of Polycrystalline Pt and Au Electrodes in Acidic Solutions},

author = {K-T Song and P M Schneider and I Grabovac and B Garlyyev and S A Watzele and A S Bandarenka},

url = {https://doi.org/10.1002/celc.202400587},

doi = {https://doi.org/10.1002/celc.202400587},

issn = {2196-0216},

year  = {2025},

date = {2025-02-16},

journal = {ChemElectroChem},

volume = {12},

number = {4},

pages = {e202400587},

abstract = {Abstract A deeper understanding of electrified solid/liquid interfaces of polycrystalline materials is crucial for optimizing energy conversion and storage devices, such as fuel cells, electrolyzers, and supercapacitors. After more than a century of research, the double-layer capacitance (CDL) has proven to be one of the few relatively easily experimentally accessible quantitative measures for characterizing such interfaces. However, despite their great importance, systematic CDL measurements are still not frequently associated with other interfacial properties. This work investigates the effect of the electrolyte pH on the CDL for polycrystalline platinum (Pt(pc)) and gold (Au(pc)) electrodes using cyclic voltammetry and impedance spectroscopy in acidic solutions with a pH ranging from 0 to 2 without adding any supporting electrolyte. Interestingly, under these conditions, the CDL for the Pt(pc) electrode increases with increasing electrolyte pH, while the CDL for the Au(pc) electrode shows the opposite trend. The increasing trend for Pt(pc) cannot be quantitatively described by the classical Stern model due to the stronger adsorption phenomenon on Pt surfaces. Moreover, positive linear trends with pH were found for the potentials of minimum CDL values and the potentials of maximum entropy for both electrodes, which closely correlate with reaction activities. However, the transition potentials of the constant phase element exponent (an element commonly used to approximate the behavior of the double layer in experiments) are only observed for the Pt electrode due to the phase transitions within the hydrogen adsorption/desorption and double-layer regions. These findings pose an important step toward revealing the interplay between essential interfacial parameters, which is crucial for a complete understanding of the electrical double layer.},

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 = {Lone Pair and Unique N-Bridging of Novel Titanium Nitridophosphate},

author = {P Ufondu and Sakshi and T D Boyko and M M Pointner and W Schnick and A Moewes},

url = {https://doi.org/10.1002/advs.202412830},

doi = {https://doi.org/10.1002/advs.202412830},

issn = {2198-3844},

year  = {2025},

date = {2025-02-11},

urldate = {2025-02-11},

journal = {Advanced Science},

volume = {12},

pages = {2412830},

abstract = {Abstract In exploring advanced materials for solar power, the novel titanium nitridophosphate (TiP4N8) stands out due to its unique linear nitrogen bridging. To investigate the elemental interactions responsible for the photovoltaic performance under visible light, the titanium L2, 3-edges and nitrogen K-edge are specifically explored using X-ray absorption spectroscopy (XAS), X-ray emission spectroscopy (XES), and resonant inelastic X-ray scattering (RIXS) techniques to map the unoccupied and occupied electronic states. It is shown that the indirect interaction between the linear nitrogen bearing the lone pair and titanium is responsible for the bandgap of 1.55 ± 0.30 eV and 1.77 ± 0.30 eV in the ?- and α-TiP4N8 phases as well as the stability of the α-phase. The formal oxidation state of the Ti ion in the ?- and α-phases are also validated to be trivalent (Ti+3) and both trivalent (Ti+3) and tetravalent (Ti+4), respectively.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Scanning impedance microscopy under oxygen reduction reaction conditions. Proof of the concept},

author = {C Schott and L Hofbauer and E Gubanova and P Schneider and A S Bandarenka},

url = {https://www.sciencedirect.com/science/article/pii/S0013468624017699},

doi = {https://doi.org/10.1016/j.electacta.2024.145533},

issn = {0013-4686},

year  = {2025},

date = {2025-02-10},

journal = {Electrochimica Acta},

volume = {513},

pages = {145533},

abstract = {In this study, we demonstrate that localized electrochemical impedance spectroscopy (LEIS) can successfully probe the solid-liquid interface of a model gold surface in low-concentrated aqueous electrolytes. The approach utilizes scanning electrochemical microscopy (SECM) under potential control of the sample, marking a notable improvement over previous SECM-based LEIS studies, which were conducted under open circuit potential conditions. The accuracy of the results was validated by comparing the interfacial parameters, such as the double-layer capacitance minimum and the potential of zero charge, with the results obtained from conventional global measurements. Additionally, local kinetic parameters for the oxygen reduction reaction (ORR) were examined via LEIS by fitting the acquired impedance spectra to a simplified, physical equivalent circuit model. Gold was chosen as a model surface for the ORR with its well-defined ORR potential region due to the absence of hydrogen adsorption and overlapping OH⁻ adsorption. The local kinetic parameter determined from the LEIS experiments corresponds to the apparent rate coefficient (kapp) of the ORR, reflecting the average kapp of individual active sites within the probed area. The dependence of kapp on the ORR overpotential aligns well with the kinetics of the 2-electron reduction of O2 taking place at the gold sample. This proof-of-concept study demonstrates that SECM-based LEIS serves as a powerful tool for the advanced characterization of complex electrochemical interfaces for future experiments, especially those with heterogeneities or different structures/materials.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Stability of the Au/electrolyte interface during hydrogen evolution: A Cyclic Plasmo-Voltammetry study},

author = {M J Feil and S Leisibach and M Becherer and K Krischer},

url = {https://www.sciencedirect.com/science/article/pii/S0013468624017456},

doi = {https://doi.org/10.1016/j.electacta.2024.145509},

issn = {0013-4686},

year  = {2025},

date = {2025-02-10},

journal = {Electrochimica Acta},

volume = {513},

pages = {145509},

abstract = {Metal-electrolyte interfaces are dynamic entities, the potential and electrolyte dependent mobility of the metal atoms leading to surface restructuring with possible dissolution and degradation. In this work, we investigate the stability of the Au/aqueous electrolyte interface with in situ differential Cyclic Plasmo-Voltammetry (dCPV), augmented by ex situ atomic force microscopy and finite differential time domain simulations. We demonstrate that even the onset of hydrogen evolution is accompanied by pronounced morphological changes of the interface which are by far more prominent than those occurring during Au oxidation and reduction. Furthermore, the stability of the interface heavily depends on pH, the degradation of the electrode being considerably stronger in acidic than in neutral electrolyte. In addition, a clear hydrogen adsorption peak was observed in neutral electrolytes during the cathodic scan, which was more pronounced on a freshly prepared Au electrode than on an aged one. The measured dCPVs in acidic and neutral electrolytes can be explained consistently assuming that (1) adsorbed hydrogen is absorbed into the subsurface region of the Au electrode once HER starts; its subsequent removal as molecular hydrogen causes morphological changes; (2) in the presence of metal cations, adsorbed hydrogen is stabilized through the formation of ternary metal hydrides on the gold surface that stabilize the surface Au-H bonds and hinder further absorption of H into the subsurface region as well as the release of hydrogen into the electrolyte.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Tertiary Alcohols as Mechanistic Probes for Photocatalysis: the Gas-Phase Reaction of 2-Methyl-2-Pentanol on Titania P25 in a Microphotoreactor},

author = {C C Aletsee and P Neumann and I Chorkendorff and M Tschurl and U Heiz},

url = {https://doi.org/10.1021/acscatal.4c07001},

doi = {10.1021/acscatal.4c07001},

year  = {2025},

date = {2025-02-07},

journal = {ACS Catalysis},

volume = {15},

number = {3},

pages = {2584-2594},

abstract = {Despite intense research in heterogeneous photocatalysis, a lack of mechanistic understanding still hinders the rational design of efficient photocatalysts to make them competitive with thermal processes that currently dominate the industry. This study elucidates the underlying mechanism of photoreactions by employing tertiary alcohols as probe molecules on a titania P25 catalyst for the understanding of photocatalytic reactions on a molecular scale. We show that the reactions do not follow the commonly assumed reaction mechanism of separate but coupled redox reactions. Instead, the gas-phase reaction occurs selectively via a homolytic bond cleavage of the long alkyl chain, leading to the formation of the corresponding ketone and an alkane, as exemplified for 2-methyl-2-pentanol at ambient pressure. The alkane stems predominantly from the recombination of the alkyl-moiety with surface hydrogen. Additionally, we demonstrate that the alkyl moiety can also undergo a dimerization reaction forming a long chain alkane, which is facilitated on bare TiO2. The high time-resolution enabled by the used microreactor allowed us to confirm that this side reaction is a higher-order process, which is governed by the alcohol surface coverage on TiO2. The parallels of the observed reaction properties with studies performed on a TiO2(110) single crystal in vacuum reveal that no significant pressure and material gap exists. On the one hand, this strongly suggests that also the reaction mechanism for the conversion of other alcohols must be reconsidered on titania-based photocatalysts and, on the other hand, demonstrates the potential of tertiary alcohols as mechanistic probes in photocatalysis. Moreover, the highly selective reactions of tertiary alcohols may open up alternative routes for chemical synthesis.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Oxygen Incorporation as a Route to Nondegenerate Zinc Nitride Semiconductor Thin Films},

author = {E Sirotti and B Scaparra and S B\"{o}hm and F Pantle and L I Wagner and F Rauh and F Munnik and C-M Jiang and M Kuhl and K M\"{u}ller and J Eichhorn and V Streibel and I D Sharp},

url = {https://doi.org/10.1021/acsami.4c16921},

doi = {10.1021/acsami.4c16921},

issn = {1944-8244},

year  = {2025},

date = {2025-02-05},

journal = {ACS Applied Materials \& Interfaces},

volume = {17},

number = {5},

pages = {7958-7968},

abstract = {Zinc nitride (Zn3N2) comprises earth-abundant elements, possesses a small direct bandgap, and is characterized by high electron mobility. While these characteristics make the material a promising compound semiconductor for various optoelectronic applications, including photovoltaics and thin-film transistors, it commonly exhibits unintentional degenerate n-type conductivity. This degenerate character has significantly impeded the development of Zn3N2 for technological applications and is commonly assumed to arise from incorporation of oxygen impurities. However, consistent understanding and control of the role of native and impurity defects on the optoelectronic properties of this otherwise promising semiconductor have not yet emerged. Here, we systematically synthesize epitaxial Zn3N2 thin films with controlled oxygen impurity concentrations of up to 20 at % by plasma-assisted molecular beam epitaxy (PA-MBE). Contrary to expectations, we find that oxygen does not lead to degenerate conductivity but instead serves as a compensating defect, the control of which can be used to achieve nondegenerate semiconducting thin films with free electron concentrations in the range of 1017 cm\textendash3, while retaining high mobilities in excess of 200 cm2 V\textendash1 s\textendash1. This understanding of the beneficial role of oxygen thus provides a route to controllably synthesize nondegenerate O-doped Zn3N2 for optoelectronic applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Exploring the atomic-scale dynamics of Fe3O4(001) at catalytically relevant temperatures using FastSTM},

author = {J Reich and S Kaiser and A Bourgund and M Krinninger and U Heiz and F Esch and B A J Lechner},

url = {https://www.sciencedirect.com/science/article/pii/S0039602824001857},

doi = {https://doi.org/10.1016/j.susc.2024.122634},

issn = {0039-6028},

year  = {2025},

date = {2025-02-01},

urldate = {2025-02-01},

journal = {Surface Science},

volume = {752},

pages = {122634},

abstract = {Surfaces and interfaces of functional nanoscale materials are typically highly dynamic when employed at elevated temperatures. Both, lateral surface and vertical bulk exchange diffusion processes set in, which can be relevant for applications such as heterogeneous catalysis. Time-resolved scanning tunneling microscopy (STM) is being pushed to ever faster measurement modes to follow such dynamic phenomena in situ. Here, we present FastSTM movies monitoring a range of atomic-scale dynamics of a prototypical reducible oxide catalyst support, Fe3O4(001), at elevated temperatures. Antiphase domain boundaries between two domains of the reconstructed surface exhibit local mobility from around 350 K, while Fe-rich point defects, in a stable equilibrium with the bulk, appear to diffuse in a peculiar zigzag pattern above 500 K. Finally, exploiting the diffusivity of Fe interstitials, we follow the propagation of step edges in the topmost atomic layer of the Fe3O4(001) surface in an oxygen atmosphere.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {From molecules to materials: SHG-CD microscopy of structured chiral films},

author = {J Pittrich and K Liang and L D\"{o}rringer and R Kienberger and U Heiz and A Kartouzian and H Iglev},

url = {https://www.sciencedirect.com/science/article/pii/S0169433224020464},

doi = {https://doi.org/10.1016/j.apsusc.2024.161331},

issn = {0169-4332},

year  = {2025},

date = {2025-01-30},

journal = {Applied Surface Science},

volume = {680},

pages = {161331},

abstract = {The interplay between molecular and structural chirality as a function of local sample morphology determines the nonlinear optical properties of many organic and hybrid organic\textendashinorganic thin films. Here, we used second harmonic generation circular dichroism (SHG-CD) microscopy of thin molecular films of 1,1′-bi-2-naphthol (R-BINOL) as a research model. Our results show that the SHG signal measured at frequencies close to the electronic transition of BINOL molecules is resonantly enhanced by more than an order of magnitude compared to the non-resonant case. The extracted resonant SHG-CD signal is dominated by the chiral response of the molecule. In contrast, structural chirality determines the non-resonant SHG-CD images. We see clear evidence that the interference of the SHG signals caused by the molecular and structural chirality can lead to a decrease in the overall SHG intensity when both SHG signals are out of phase. These findings highlight the intricate relationship between molecular and structural chirality on the one hand and structural morphology on the other hand and pave the way for novel applications by exploiting the chiroptic properties of thin films.},

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 = {Scalable Bulk Synthesis of Phase-Pure γ-Sn3N4 as a Model for an Argon-Flow-Mediated Metathesis Reaction},

author = {M Zipkat and A Koldemir and T Block and C Ceniza and T D Boyko and S Kl\"{a}ger and R M Pritzl and A Moewes and R P\"{o}ttgen and S S Rudel and W Schnick},

url = {https://doi.org/10.1002/chem.202403745},

doi = {https://doi.org/10.1002/chem.202403745},

issn = {0947-6539},

year  = {2025},

date = {2025-01-23},

urldate = {2024-11-18},

journal = {Chemistry \textendash A European Journal},

volume = {31},

pages = {e202403745},

abstract = {Abstract Nitrides represent a promising class of materials for a variety of applications. However, bulk synthesis remains a challenging task due to the stability of the N2 molecule. In this study, we introduce a simple and scalable approach for synthesizing nitride bulk materials. Moderate reaction temperatures are achieved by using reactive starting materials, slow and continuous mixing of the starting materials, and by dissipating heat generated during the reaction. The impact on the synthesis of using different starting materials as nitrogen source and the influence of a flux were examined. ?-Sn3N4 was selected as the model compound. The synthesis of pure ?-Sn3N4 bulk material on a large scale has still been a challenge, although a few synthesis methods were already described in the literature. Here we synthesized ?-Sn3N4 by metathesis reaction of argon-diluted SnCl4 with Li3N, Mg3N2 or Ca3N2 as nitrogen sources. Products were characterized by powder X-ray diffraction, scanning and transmission electron microscopy, energy-dispersive X-ray spectroscopy, dynamic flash combustion analysis, hot gas extraction analysis, X-ray photoelectron spectroscopy, M\"{o}ssbauer spectroscopy and X-ray absorption and emission spectroscopy. Additionally, single-crystal diffraction data of ?-Sn?N?, previously unavailable, were successfully collected.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A Combined Experimental and Computational Study on the Broadening Mechanism of the Luminescence in Narrow-Band Eu2+-Doped Phosphors},

author = {R Shafei and P J Strobel and P J Schmidt and D Maganas and W Schnick and F Neese},

url = {https://doi.org/10.1021/acs.jpcc.4c06912},

doi = {10.1021/acs.jpcc.4c06912},

issn = {1932-7447},

year  = {2025},

date = {2025-01-16},

journal = {The Journal of Physical Chemistry C},

volume = {129},

number = {2},

pages = {1495-1505},

abstract = {In this work, we present a comprehensive study of the luminescence relaxation mechanism and the associated spectral broadening in a series of Eu2+-doped narrow-band phosphors. It is highlighted that the commonly used full-width at half-maximum (fwhm) is no longer a sensitive measure for quantifying the emission bandwidth of these materials. A thorough understanding of the factors contributing to the narrow bandwidth requires an explicit treatment of the magnetic structure of the ground and emissive excited state manifolds. This requires incorporating spin\textendashorbit coupling effects using wave function-based methods such as the complete active space self-consistent field combined with second-order N-electron valence state perturbation theory (CASSCF/NEVPT2). In addition, for the associated excited state dynamics calculations, one needs to consider vibronic coupling interactions on the basis of Franck\textendashCondon (FC), Herzberg\textendashTeller (HT), and, when necessary, pseudo Jahn\textendashTeller (PJT) coupling effects. Our analysis underscores that understanding and controlling the synergistic roles of these “static” and “dynamic” effects are essential for accurately assessing the narrow band emission relaxation in these systems. We show that these results can, in principle, be generalized to an arbitrary set of narrow-band phosphor candidates and can potentially aid the experimental efforts toward developing novel phosphors with enhanced luminescent properties.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Crystalline porous frameworks based on double extension of metal\textendashorganic and covalent organic linkages},

author = {K Endo and S Canossa and F Heck and D M Proserpio and M S Istek and F Stemmler and J Van Slageren and S Hartmann and A Hartschuh and B V Lotsch},

url = {https://doi.org/10.1038/s44160-024-00719-x},

doi = {10.1038/s44160-024-00719-x},

issn = {2731-0582},

year  = {2025},

date = {2025-01-14},

journal = {Nature Synthesis},

abstract = {Reticular chemistry is a powerful strategy to design materials with fine-tuned chemical functionality and porosity, such as metal\textendashorganic frameworks (MOFs) and covalent organic frameworks (COFs). MOFs typically show high crystallinity due to their reversible coordinative bonds, and the organic backbone of COFs provides chemical stability. Here we synthesize metal\textendashorganic\textendashcovalent\textendashorganic frameworks (MOCOFs) that combine both crystallinity and stability in a single framework by the double extension of metal\textendashorganic and covalent organic linkages. Several MOCOFs are obtained by reaction between a cobalt aminoporphyrin and dialdehydes, which are interconnected by cobalt\textendashamine coordination and imine condensation to form three-dimensional networks. The MOCOFs exhibit chiral topological nets, large surface areas, high crystallinities and high chemical stabilities due to the two types of extended linkages. Thus, MOCOFs present a reticular design strategy that further diversifies the chemical and structural space of porous solids.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Octaethyl vs Tetrabenzo Functionalized Ru Porphyrins on Ag(111): Molecular Conformation, Self-Assembly and Electronic Structure},

author = {D Meier and P Knecht and P Vezzoni Vicente and F Eratam and H Xu and T-L Lee and A Generalov and A Riss and B Yang and F Allegretti and P Feulner and J Reichert and J V Barth and A P Seitsonen and D A Duncan and A C Papageorgiou},

url = {https://doi.org/10.1021/acs.jpcc.4c06978},

doi = {10.1021/acs.jpcc.4c06978},

issn = {1932-7447},

year  = {2025},

date = {2025-01-09},

journal = {The Journal of Physical Chemistry C},

volume = {129},

number = {1},

pages = {858-869},

abstract = {Metalloporphyrins on interfaces offer a rich playground for functional materials and hence have been subjected to intense scrutiny over the past decades. As the same porphyrin macrocycle on the same surface may exhibit vastly different physicochemical properties depending on the metal center and its substituents, it is vital to have a thorough structural and chemical characterization of such systems. Here, we explore the distinctions arising from coverage and macrocycle substituents on the closely related ruthenium octaethyl porphyrin and ruthenium tetrabenzo porphyrin on Ag(111). Our investigation employs a multitechnique approach in ultrahigh vacuum, combining scanning tunneling microscopy, low-energy electron diffraction, photoelectron spectroscopy, normal incidence X-ray standing wave, and near-edge X-ray absorption fine structure, supported by density functional theory. This methodology allows for a thorough examination of the nuanced differences in the self-assembly, substrate modification, molecular conformation and adsorption height.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {DNA Origami Colloidal Crystals: Opportunities and Challenges},

author = {J Lee and J Kim and G Posnjak and A Ershova and D Hayakawa and W M Shih and W B Rogers and Y Ke and T Liedl and S Lee},

url = {https://doi.org/10.1021/acs.nanolett.4c05041},

doi = {10.1021/acs.nanolett.4c05041},

issn = {1530-6984},

year  = {2025},

date = {2025-01-08},

journal = {Nano Letters},

volume = {25},

number = {1},

pages = {16-27},

abstract = {Over the last three decades, colloidal crystallization has provided an easy-to-craft platform for mesoscale engineering of photonic and phononic crystals. Nevertheless, the crystal lattices achieved thus far with commodity colloids are largely limited to symmetric and densely packed structures, restricting their functionalities. To obtain non-close-packed crystals and the resulting complexity of the available structures, directional binding between “patchy” colloids has been pursued. However, the conventional “patchy” colloids have been restricted to micrometer-scale spherical particles or clusters. In this Mini-Review, we argue that the time has come to widen the scope of the colloidal palette and include particles made using DNA origami. By benefiting from its unprecedented ability to control nanoscale shapes and patch placement and incorporate various nanomaterials, DNA origami enables novel engineering of colloidal crystallization, particularly for photonic and phononic applications. This mini-review summarizes the recent progress on using DNA origami for colloidal crystallization, together with its challenges and opportunities.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Spectrally resolved far-field emission pattern of single photon emitters in $mathrmMomathrmS_2$},

author = {K Barthelmi and T Amit and L Sigl and M Troue and T Klokkers and A Herrmann and T Taniguchi and K Watanabe and J J Finley and C Kastl and S Refaely-Abramson and A W Holleitner},

url = {https://link.aps.org/doi/10.1103/PhysRevMaterials.9.016201},

doi = {10.1103/PhysRevMaterials.9.016201},

year  = {2025},

date = {2025-01-08},

urldate = {2025-01-08},

journal = {Physical Review Materials},

volume = {9},

number = {1},

pages = {016201},

keywords = {},

pubstate = {published},

tppubtype = {article}

}