Publications

@article{nokey,

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

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

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

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

issn = {2211-2855},

year  = {2025},

date = {2025-10-01},

journal = {Nano Energy},

volume = {143},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {0927-796X},

year  = {2025},

date = {2025-09-01},

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

volume = {166},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Selective growth and characterization of GaN nanowires on SiC substrates},

author = {T H\"{o}ldrich and A Wieland and F Pantle and J Winnerl and M Stutzmann},

url = {https://www.sciencedirect.com/science/article/pii/S0022024825001423},

doi = {https://doi.org/10.1016/j.jcrysgro.2025.128194},

issn = {0022-0248},

year  = {2025},

date = {2025-09-01},

journal = {Journal of Crystal Growth},

volume = {665},

pages = {128194},

abstract = {GaN on SiC is a promising material combination for high power devices, where especially nanostructures, such as nanowires or nanofins, are a space and resource saving solution. In this work we demonstrate the selective area growth of GaN nanowires on SiC substrates, using the polytype 6H-SiC. We investigate the influence of the Si- and C-polarity of the substrate on the structural properties of the GaN nanowires by scanning electron microscopy and photoluminescence spectroscopy. On both substrates uniform and hexagonal nanowires are achieved for the respective optimal growth temperature, which is determined to be 20$circ $C higher for Si-polarity. As the polarity combination of the SiC substrate and GaN nanowires strongly influences the electrical properties at the heterointerface due to different charge accumulations, it is necessary to investigate the epitaxial relationship. X-ray diffraction revealed that the GaN nanowires exclusively adopt the orientation of the underlying SiC lattice, leading to an in-plane epitaxial relationship of (11¯00)GaN/(11¯00)6H-SiC. Polarity-selective wet chemical etching and Kelvin probe force microscopy showed that the GaN nanowires preserve the polarity of the substrate, thus, either a predominantly metal-polar (Si-polar/Ga-polar) or non-metal-polar (C-polar/N-polar) orientation is present. The complete epitaxial relationship on both substrate polarities can be identified as (11¯00)[0001]GaN||(11¯00)[0001]6H-SiC for the large majority of NWs at their respective optimum growth temperatures.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Simulating Electrochemical Aging in NCM111 Materials Through Controlled Chemical Delithiation},

author = {S M Qian and A T S Freiberg and F Friedrich and C Gr\"{o}n and H A Gasteiger},

url = {\<Go to ISI\>://WOS:001559898400001},

doi = {10.1149/1945-7111/adfca2},

issn = {0013-4651},

year  = {2025},

date = {2025-08-28},

journal = {Journal of the Electrochemical Society},

volume = {172},

number = {8},

abstract = {To meet the cycle life requirements and to guarantee the safe operation of lithium-ion batteries, the upper cutoff potential of cathode active materials based on mixed transition metal layered oxides like NCM (LiMO2, with M = Ni, Co, Mn) must be restricted, thereby limiting the available specific capacity. A significant degradation mechanism in NCM materials involves the harmful release of lattice oxygen at high degrees of delithiation (reached at high cathode potentials), forming an oxygen-depleted surface phase on the active material particles accompanied by electrolyte oxidation. To mimic the electrochemically-induced lattice oxygen release, NCM materials can be subjected to chemical delithiation and subsequent heat-treatment. We thus investigated the chemical delithiation of NCM111 (Li1.0(Ni1/3Co1/3Mn1/3)O2) with NO2BF4, followed by a heat-treatment. The resulting materials are characterized with regards to their electrochemical characteristics as well as by thermogravimetric analysis-mass spectrometry, X-ray diffraction, scanning electron microscopy, and gas adsorption analysis. We discovered that chemical delithiation initially produces a disordered layered phase that is electrochemically less active. Upon heat-treatment, this phase restructures into a fully-lithiated and well-ordered layered phase and an electrochemically inactive spinel phase. This study enhances our understanding of the phases that form when NCM materials undergo extensive delithiation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {A Comparative Analysis of Plasmonic and Dielectric Metasurface Sensing Platforms Powered by Bound States in the Continuum},

author = {T Jiang and A Bhattacharya and M Barkey and A Aigner and L Rohrer and T Weber and J Wang and S A Maier and A Tittl},

url = {\<Go to ISI\>://WOS:001558957300001},

doi = {10.1002/adfm.202516021},

issn = {1616-301X},

year  = {2025},

date = {2025-08-28},

journal = {Advanced Functional Materials},

abstract = {Nanophotonic platforms based on surface-enhanced infrared absorbance spectroscopy (SEIRAS) have emerged as an effective tool for molecular detection. Sensitive nanophotonic sensors with robust resonant modes and amplified electromagnetic near fields are essential for spectroscopy, especially in lossy environments. Metasurfaces driven by bound state in the continuum (BICs) have unlocked a powerful platform for molecular detection due to their exceptional spectral selectivity. While plasmonic BIC metasurfaces are preferred for molecular spectroscopy due to their high surface fields, enhancing the interaction with analytes, dielectric BICs have become popular due to their high-quality factors and, thus, high sensitivity. However, their sensing performance has largely been demonstrated in air, neglecting the intrinsic infrared (IR) losses found in common solvents. This study evaluates the suitability of plasmonic versus dielectric platforms for in situ molecular spectroscopy. Here, the sensing performance of plasmonic (gold) and dielectric (silicon) metasurfaces is assessed across liquid environments with varying losses resembling typical solvents. The results show that dielectric metasurfaces excel in dry conditions, while plasmonic BIC metasurfaces outperform them in lossy solvents, with a distinct crossover point where both show similar performance. The results provide a framework for selecting the optimal metasurface material platform for SEIRAS studies based on environmental conditions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Optimizing Carrier Balance in CsPbBr3 Nanocrystal LEDs: The Role of Alkyl Ligands and Polar Electron Transport Layers},

author = {R Jayabalan and G K Hanumantharaju and T Hettiger and A Sarkar and F S Zu and A Ullrich and A Abfalterer and A S Urban and N Koch and D Andrienko and M Scheele and W Br\"{u}tting},

url = {\<Go to ISI\>://WOS:001556372500001},

doi = {10.1002/adom.202501361},

issn = {2195-1071},

year  = {2025},

date = {2025-08-26},

journal = {Advanced Optical Materials},

abstract = {The study of lead halide perovskite nanocrystal based light-emitting diodes (LEDs) has advanced significantly, with notable improvements in stability and optical properties. However, optimizing charge carrier injection and transport remains a challenge. Efficient electroluminescence requires a balanced transport of both holes and electrons within the emitting material. Here, cubic CsPbBr3 nanocrystals passivated with oleylamine and oleic acid are investigated, comparing them to ligand-exchanged nanocrystals with didodecyldimethylammonium bromide (DDABr). Nuclear magnetic resonance spectroscopy and transmission electron microscopy confirm successful ligand exchange, revealing reduced ligand coverage in DDABr-treated nanocrystals. Photoelectron spectroscopy, spectroelectrochemistry, and single-carrier devices indicate improved hole injection in DDABr-capped nanocrystals. Density functional theory calculations further reveal the influence of ligand type and coverage on energy levels, with oleic acid introducing localized states in native nanocrystals. Additionally, incorporation of a polar electron transport layer enhances LED performance by over an order of magnitude in DDABr-capped nanocrystals, driven by improved charge balance arising from the spontaneous orientation polarization of the electron transport layer. These findings highlight the critical role of ligand selection, passivation degree, and charge transport control by the adjacent organic transport layers in optimizing LED efficiency.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

doi = {10.29026/oea.2025.240316},

issn = {2096-4579},

year  = {2025},

date = {2025-08-24},

journal = {Opto-Electronic Advances},

volume = {8},

number = {8},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Phase-Stable Palladium Hydride Derived from PdCoO2 for Sustainable Hydrogen Evolution Reaction},

author = {L Camuti and S Kim and F Podjaski and M Vega-Paredes and A M Mingers and T Acart\"{u}rk and U Starke and B V Lotsch and C Scheu and B Gault and S Y Zhang},

url = {\<Go to ISI\>://WOS:001555162600001},

doi = {10.1002/adfm.202514366},

issn = {1616-301X},

year  = {2025},

date = {2025-08-22},

journal = {Advanced Functional Materials},

abstract = {Active and reliable electrocatalysts are fundamental to renewable energy technologies. PdCoO2 is recently recognized as a promising catalyst template for the hydrogen evolution reaction (HER) in acidic media, thanks to the formation of exceptionally active PdHx. In this article, the transformation process of single PdCoO2 particles during HER is monitored and elucidated, confirming their almost complete transformation to PdHx. Using operando mass spectrometry, Co dissolution from the PdCoO2 template is observed under reductive potentials, with a partial current of 0.1% of the HER current, while PdHx is formed simultaneously. High HER activity of this phase is retained with long-term operation, dry storage, or vacuum exposure. Isotope labeling of hydrogen using D2O confirms the formation of a stable PdHx phase by secondary ion mass spectrometry and down to the near-atomic scale by atom probe tomography. A separation between D-poor alpha- and D-rich beta-Pd hydrides is observed with an overall composition of beta-PdD0.64. These findings highlight the critical role of a templated growth method for obtaining stabilized PdHx, enabling Pt-like efficient HER without the commonly slow activation processes observed in Pd due to rate-limiting material hydrogenation. This offer insights into the design of more efficient electrocatalysts for renewable energy technologies.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Cobalt-Based Catalyst Integration Into a Hierarchically Ordered Macro-Meso-microporous Carbon Cathode for High-performance Aqueous Zn-Sulfur Batteries},

author = {L Z Liu and M Z Hussain and D Lei and O Henrotte and E Cortes and A S Bandarenka and R A Fischer},

url = {\<Go to ISI\>://WOS:001554583800001},

doi = {10.1002/advs.202509945},

year  = {2025},

date = {2025-08-21},

journal = {Advanced Science},

abstract = {The pyrolytic synthesis of an ordered macro-meso-micro porous carbon cathode material (OM-PC) with integration of a Co3ZnC/Co catalyst is reported. It is derived from a Co-doped ZIF-8 framework via a templated in situ growth within the interstitial spaces of a preformed self-assembled polystyrene monolith, followed by the template removal. The hierarchical 3D architecture facilitates Zn2(+) diffusion and enhances reaction kinetics during charge-discharge processes. The integrated Co3ZnC/Co catalyst significantly improves the surface affinity of the porous carbon host for polysulfide trapping and accelerates polysulfide redox conversion, leading to enhanced sulfur utilization, mitigated shuttle effects, and longer cycling stability. The fabricated aqueous Zn-S battery with the sulfur-loaded cathode denoted as S@Co3ZnC/Co/OM-PC delivers a synergistic high discharge capacity of approximate to 1685 mA h g-1, which includes approximate to 115 mA h g-1 contributed from the I3 -/I- redox couple. The device shows low polarization and exhibits a minimal capacity decay of approximate to 0.027% per cycle over 400 cycles. It maintained a good rate performance of approximate to 1035 mA h g-1 at 3 A g-1, with long cycling stability. In-depth investigation reveals a multistep intermediate polysulfides conversion pathway in the aqueous electrolyte, which effectively avoids the sluggish solid-solid conversion.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {CsPbBr3 Nanocrystals as Bottom Interface Nucleation Seeds for Printing Oriented FAPbI3 Thin Films: An In Situ Study},

author = {A Buyan-Arivjikh and J Fricker and T Baier and X J Ci and L X Li and D Gaur and L Polavarapu and M Schwartzkopf and S K Vayalil and P Mueller-Buschbaum},

url = {\<Go to ISI\>://WOS:001552870900001},

doi = {10.1002/smll.202505895},

issn = {1613-6810},

year  = {2025},

date = {2025-08-20},

journal = {Small},

abstract = {The exceptional optoelectronic properties of lead halide perovskites are highly sensitive to processing conditions, as uncontrolled crystallization driven by random nucleation often results in defect-rich active layers that impair device performance. Achieving controlled and oriented crystallization in printed films remains a major challenge. To address this, we introduce a pre-deposited CsPbBr3 nanocrystal seed layer at the bottom interface to guide crystallization and suppress defect formation. This strategy is evaluated via an in situ study on FAPbI3, offering mechanistic insights into the influence of seeding on film growth and optoelectronic quality. Using in situ grazing-incidence wide-angle X-ray scattering, transmission-mode UV-vis absorption, and photoluminescence spectroscopy, phase evolution and seed-mediated growth kinetics are tracked. Seeding accelerates the transition from the photoinactive delta-phase to the photoactive alpha-phase, yielding a crystallization rate constant over six times higher than in unseeded films. Moreover, the seed layer governs the crystallographic orientation of the resulting perovskite film, leading to improved optical absorption and reduced defect density.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

doi = {10.1002/adfm.202515801},

issn = {1616-301X},

year  = {2025},

date = {2025-08-19},

journal = {Advanced Functional Materials},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Photosystem II-Carbon Nitride Photoanodes for Scalable Biophotoelectrochemistry},

author = {H Y Zhang and W J Tian and J K Lin and P Zhang and G S Shao and S K Ravi and H Q Sun and E Cort\'{e}s and V Andrei and S B Wang},

url = {\<Go to ISI\>://WOS:001550386200001},

doi = {10.1002/adma.202508813},

issn = {0935-9648},

year  = {2025},

date = {2025-08-15},

journal = {Advanced Materials},

abstract = {Photosystem II (PSII) is a vital photosynthetic enzyme with the potential for sustainable bioelectricity and fuel generation. However, interfacing PSII with intricate, small-scale electrodes for practical applications has been challenging. This study addresses this by creating protonated macroporous carbon nitride (MCN) as support and developing a scalable spray-freeze method to wire PSII with MCN. This facilitates the production of large-area MCN-PSII photoanodes up to 33 cm2 for biophotoelectrochemical water oxidation to O2, achieving efficient interfacial charge transfer and initial photocurrents in the mA range with Faradaic yield of 93.5 +/- 8.5% over 5 h. A bias-free biophotoelectrochemical (BPEC) device is designed by connecting the MCN-PSII photoanode to a carbon nanotube cathode loaded with bilirubin oxidase. An array of eight tandem BPEC cells with a photoactive area of 72 cm2 successfully powers low-power electronics, such as LEDs. This work paves an efficient way for bioelectrode fabrication, showcasing the potential of PSII-based semi-artificial systems for BPEC and biophotovoltaic applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Structure and Transport Properties in the Pseudobinary Phase System Li4SiS4-Li4SnS4},

author = {L G Balzat and Y Li and S Dums and I Moudrakovski and K Gjorgjevikj and A Schulz and Y H Li and S Krause and P Canepa and B V Lotsch},

url = {\<Go to ISI\>://WOS:001551105400001},

doi = {10.1021/acs.chemmater.5c00358},

issn = {0897-4756},

year  = {2025},

date = {2025-08-15},

journal = {Chemistry of Materials},

abstract = {Thio-lithium superionic conductors (thio-LISICONs) are a family of promising solid electrolyte materials for potential applications in solid-state batteries. The orthorhombic polymorph of the thio-LISICON Li4SiS4 (o-Li4SiS4) has been known for decades, but its complete crystal structure has been reported only recently. Here, using single-crystal X-ray diffraction, we reevaluated the crystal structure of o-Li4SiS4 and showed that o-Li4SiS4 crystallizes in space group Pmn21 (no. 31},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

doi = {10.1002/anie.202511336},

year  = {2025},

date = {2025-08-14},

journal = {Angewandte Chemie-International Edition},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Sub-Bandgap Photon-to-Current Conversion in Bismuth Vanadate Photoanodes and Its Impact on the Maximum Photocurrent Density Achievable for Water Splitting},

author = {C G Ferreira and C Ros and M Y Zhang and G D Zhou and V Gacha and D Raptis and I D Sharp and J Martorell},

url = {\<Go to ISI\>://WOS:001549528700001},

doi = {10.1021/acsenergylett.5c01894},

issn = {2380-8195},

year  = {2025},

date = {2025-08-13},

journal = {Acs Energy Letters},

abstract = {The physical properties of bismuth vanadate (BiVO4) make it an appealing semiconductor photoanode for water oxidation in photoelectrochemical cells that aim to produce hydrogen or other solar fuels. However, it has been estimated that its relatively wide bandgap limits achievable photocurrent densities to approximately 7.5 mA/cm2 under 1 sun AM1.5G illumination. Here, we perform high-sensitivity external quantum efficiency measurements and demonstrate that sub-bandgap states within BiVO4 also contribute to photocurrent generation, regardless of the fabrication method or mesoscopic structure. Based on these results and considering Lambertian scattering at the electrolyte/BiVO4 interface, we show that the maximum theoretical current density from BiVO4 can be as high as 12.2 mA/cm2, when assuming complete absorption and conversion of sunlight photons extending to the lowest photon energy for which we experimentally measured photocurrent generation promoted by sub-bandgap states. This finding opens new avenues for design of BiVO4 photoanodes with efficiencies that are much greater than were previously assumed to be possible.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Long Used but Hardly Known: Synthesis and Crystal Structure of Tritium Breeding Li2Be2O3},

author = {G Krach and J Steinadler and R Calaminus and B V Lotsch and W Schnick},

url = {\<Go to ISI\>://WOS:001546654300001},

doi = {10.1002/chem.202502209},

issn = {0947-6539},

year  = {2025},

date = {2025-08-11},

journal = {Chemistry-a European Journal},

abstract = {A main challenge for the operation of a nuclear fusion reactor is the consumption of tritium during the fusion process and the limited availability of tritium in natural resources or its production in nuclear power plants. The most promising approach is breeding of new tritium within the operating fusion reactor. For this purpose, suitable breeding materials are needed. Lithium beryllium oxides are a promising class of compounds, as they unite both target and neutron multiplier in one material. While there have already been studies on sintered ceramics in the Li2OBeO system, the crystal structure of compounds of a defined composition has so far remained unsolved. Herein, we report on the synthesis of phase-pure Li2Be2O3 in a high-temperature (HT) approach and its structure determination by single-crystal X-ray diffraction (sc-XRD). In addition, the compound was characterized by powder X-ray diffraction (PXRD), solid-state nuclear magnetic resonance (NMR) spectroscopy, and elemental analysis. The thermal stability, which is important for use as blanket material in a fusion reactor, was examined with differential scanning calorimetry (DSC).},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Efficient Electronic-Structure Methods Toward Catalyst Screening: Projection-Based Embedding Theory for CO2 Reduction Reaction Intermediates},

author = {E Kolodzeiski and C J Stein},

url = {\<Go to ISI\>://WOS:001547141000001},

doi = {10.1002/anie.202503418},

year  = {2025},

date = {2025-08-07},

journal = {Angewandte Chemie-International Edition},

abstract = {Catalyst screening is a demanding task for computational chemistry since the profound diversity of surface structures under operando conditions is accompanied by high demands on the accuracy to predict the relevant kinetics. Embedding approaches that allow researchers to focus the computational effort on the chemically active regions of interest are promising tools in the pursuit of balancing accuracy and efficiency. However, for metallic catalysts, the required separation of the system into an active part treated with highly accurate methods and an environment is technically hard to achieve due to the delocalization of electrons in the conducting surface. Therefore, studies analyzing the potential of embedding methods for heterogeneous (electro-)catalyst screening are scarce. In this contribution, we demonstrate that simple embedding approaches are indeed achievable for studying metallic catalysts if i) the active orbital space is held consistent over a reaction coordinate and ii) the nonadditive exchange-correlation functional used to calculate the embedding potential includes a fraction of exact exchange to mitigate delocalization errors. We verify the approach for a set of open- and closed-shell CO2 reduction reaction intermediates on different adsorption sites of a Cu(111) surface represented by cluster models to demonstrate that catalyst screening with embedding approaches is achievable.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Applying an Anti-Kasha Model Resolves Differences Between Photosynthetic and Artificial Pigments},

author = {J P G\"{o}tze and S Petry and S Reiter and H Lokstein and R De Vivie-Riedle},

url = {\<Go to ISI\>://WOS:001535152400001},

doi = {10.1021/acs.jpcb.5c02465},

issn = {1520-6106},

year  = {2025},

date = {2025-08-07},

journal = {Journal of Physical Chemistry B},

volume = {129},

number = {31},

pages = {7884-7895},

abstract = {The current interpretation of excitation energy transfer (EET) processes in natural photosynthesis generally relies on Kasha's rule, suggesting that internal conversion (IC) processes usually outpace any EET between higher excited states. It is, however, known from research on artificial systems that Kasha's rule does not apply to many dyes, especially when found in assembled clusters analogous to photosynthetic chlorophyll (Chl)-protein complexes. In this contribution, a semiempirical Forster-type model is applied to otherwise well-investigated pigments of natural photosynthesis (Chls a, b, c1 and various carotenoids). Strong potential for anti-Kasha processes is identified in all investigated pigments, based on their high Coulomb coupling elements, similar to compounds with already known anti-Kasha properties. The pigments are further found to form strongly delocalized excitons, especially between the higher excited states usually responsible for anti-Kasha pathways. Test calculations with different pigment compositions for various natural light harvesting complexes (LHCII, CP24, CP26, CP29, FCP) demonstrate how the higher band EET network and absorbance could be affected by the presence of accessory pigments: Chl a-only networks should perform anti-Kasha EET, but this is suppressed by the presence of accessory pigments via several mechanisms (exciton disruption, spectral competition, energy sinks and fast, non-Chl a IC). The apparent "special" behavior of photosynthetic systems is thus resolved as the result of pigment mixtures.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Covalent Organic Framework Bipolar Pseudocapacitive Electrodes in an All-Organic Symmetric Lithium-Ion Battery},

author = {A Singh and P Bhauriyal and L Quincke and D Bl\"{a}tte and R Guntermann and J L Rupp and T Heine and T Bein},

url = {\<Go to ISI\>://WOS:001544766400001},

doi = {10.1002/aenm.202501494},

issn = {1614-6832},

year  = {2025},

date = {2025-08-06},

journal = {Advanced Energy Materials},

abstract = {Covalent organic frameworks (COFs) have emerged as promising active materials for secondary-ion battery electrodes, owing to their robust porous structure and the flexibility in selecting redox-active building blocks. Here, a novel highly crystalline, electro-active, bipolar-type WTTF-COF, obtained by integrating p-type N,N,N ',N '-tetrakis(4-aminophenyl)-1,4-phenylenediamine (W) and 4,4 ',4 '',4 '''-([2,2'-bi(1,3-dithiolylidene)]-4,4 ',5,5 '-tetrayl)tetrabenzaldehyde (TTF) molecular building blocks via n-type imine linkages, is reported, serving as a Li-ion battery electrode. In Li-ion half cells, WTTF-COF as a cathode features 12-electron dual-ion redox chemistry per unit cell within a stable, unusually wide potential window of 0.1-3.6 V versus Li/Li+, corresponding to a high theoretical capacity of 315 mAh g-1, with an experimental reversible specific capacity of 271 mAh g-1 at 0.1 A g-1. The hybrid redox features coupled with the long-range ordered nanostructure of WTTF-COF enable an efficient pseudo-capacitive charge-storage mechanism. Different diffusion pathways and diffusion coefficients for Li+ and PF6- transport are established through detailed diffusion measurements and theoretical modeling. Among hybrid storage electrodes, WTTF-COF is reported to offer the option to serve as both anode and cathode up to a high rate of 200 mV s-1, as demonstrated in fully organic symmetric cell tests. Summarizing, judiciously designed COFs are suitably established for efficient bipolar electrode applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Unveiling Coexisting Battery-Type and Pseudocapacitive Intercalation Mechanisms in Lithium Titanate},

author = {L P Kong and P J Williams and F Brushett and J L M Rupp},

url = {\<Go to ISI\>://WOS:001544773300001},

doi = {10.1002/aenm.202503080},

issn = {1614-6832},

year  = {2025},

date = {2025-08-06},

journal = {Advanced Energy Materials},

abstract = {Conventional lithium-ion (Li-ion) batteries and supercapacitors face inherent trade-offs between power and energy densities, restricting their adaptability in applications requiring dynamic performance across both regimes. Here, a "zero-strain" lithium titanate (Li4Ti5O12) as a new class of battery-capacitive material exhibiting dual lithiation mechanisms, combining diffusion-controlled battery-type redox reactions and surface-controlled pseudocapacitive intercalation, depending on the operating potential, is revealed. At approximate to 1.55 V (vs Li/Li+), lithium titanate undergoes a two-phase transition reaction between Li4Ti5O12 and Li7Ti5O12, involving Li migration between 8a and 16c Wyckoff sites. Upon deeper lithiation to potentials near 0 V, Li ions reoccupy the 8a sites, triggering a reversible pseudocapacitive response with fast kinetics. Leveraging these dual lithiation mechanisms, lithium titanate delivers a high reversible capacity of approximate to 215 mAh g-1 at 20 mA g-1, retaining 148 mAh g-1 at 2000 mA g-1. The high-rate capability and cycling stability are attributed to a unique structure with minimal lattice strain during Li-site occupation. This work presents the first clear demonstration of a unique dual-mode charge storage mechanism in lithium titanate, which can reversibly operate in either battery-type or pseudocapacitive regimes.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Optical control of resonances in temporally symmetry-broken metasurfaces},

author = {A Aigner and T Possmayer and T Weber and A A Antonov and L D Menezes and S A Maier and A Tittl},

url = {\<Go to ISI\>://WOS:001545391600001},

doi = {10.1038/s41586-025-09363-7},

issn = {0028-0836},

year  = {2025},

date = {2025-08-06},

journal = {Nature},

abstract = {Tunability in active metasurfaces has mainly relied on shifting the resonance wavelength1,2 or increasing material losses3,4 to spectrally detune or quench resonant modes, respectively. However, both methods face fundamental limitations, such as a limited Q factor and near-field enhancement control and the inability to achieve resonance on-off switching by completely coupling and decoupling the mode from the far field. Here we demonstrate temporal symmetry breaking in metasurfaces through ultrafast optical pumping, providing an experimental realization of radiative-loss-driven resonance tuning, allowing resonance creation, annihilation, broadening and sharpening. To enable this temporal control, we introduce restored symmetry-protected bound states in the continuum. Even though their unit cells are geometrically asymmetric, coupling to the radiation continuum remains fully suppressed, which, in this work, is achieved by two equally strong antisymmetric dipoles. By using selective Mie-resonant pumping in parts of these unit cells, we can modify their dipole balance to create or annihilate resonances as well as tune the linewidth, amplitude and near-field enhancement, leading to potential applications in optical and quantum communications, time crystals and photonic circuits.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Comparative convolutional neural networks for perovskite solar cell PCE predictions},

author = {M Harth and D K Kumar and S Kassou and K El Idrissi and R K Gupta and Y Daniel and O Makdasi and I Visoly-Fisher and A Gagliardi},

url = {\<Go to ISI\>://WOS:001544453700001},

doi = {10.1038/s41524-025-01744-w},

year  = {2025},

date = {2025-08-04},

journal = {Npj Computational Materials},

volume = {11},

number = {1},

abstract = {Imaging offers a fast and accessible means for spatial characterization of halide perovskite photovoltaic materials, yet extracting optoelectrical properties-such as power conversion efficiency (PCE)-remains challenging. This study presents a deep learning methodology that correlates optical reflective images of perovskite solar cells with their PCE by focusing on image differences rather than absolute visual features. The approach predicts relative changes in PCE by comparing images of the same device in different states (e.g., before and after encapsulation) or against a reference image. This comparative technique significantly outperforms traditional methods that attempt to directly infer PCE from a single image. Furthermore, it demonstrates high effectiveness in low-data regimes, using only 115 samples. By leveraging convolutional neural networks (CNNs) trained on small datasets, the method offers an adaptable and scalable solution for device characterization. Overall, the comparative approach enhances the accuracy and applicability of machine vision in perovskite solar cell analysis.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Reflection-Enhanced Raman Identification of Single Bacterial Cells Patterned Using Capillary Assembly},

author = {J Lee and E Rho and M Kim and S Huh and S Kim and S A Maier and E Cort\'{e}s and S Jo and Y S Jung and Y Nam},

url = {\<Go to ISI\>://WOS:001543629000001},

doi = {10.1021/acssensors.5c01225},

issn = {2379-3694},

year  = {2025},

date = {2025-08-03},

journal = {Acs Sensors},

abstract = {Raman spectroscopy is an enticing tool for the rapid identification of pathogenic bacteria and has the potential to meet the demand for early diagnosis and timely treatment of patients. However, it remains a challenge to devise a reliable Raman detection platform to obtain reproducible signals from single bacterial cells. Herein, we utilize a reflective Ag/SiO2 film that enhances the intrinsically weak Raman signals by re-excitation of the bacteria and reflection of downward-scattered photons, with maximum Raman intensities recorded by exciting the central edge of each single cell. The reflection-based configuration is simple, and its reliability as a sensing platform is validated by deep learning analysis. Importantly, given the positional dependence of the laser light on the Raman intensity, we employ capillarity-assisted particle assembly (CAPA) to selectively position single bacterial cells into a reflective topographical template to align the most Raman active region of the cell per the trap site geometry. Moreover, CAPA is utilized to directly isolate single cells from a suspension of artificial urine, eradicating any additional steps previously required to separate bacteria from biological samples. The proposed system has positive implications for future clinical settings that require simple, accurate, and reproducible detection of bacteria at the single-cell level.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Water Oxidation and Degradation Mechanisms of BiVO4 Photoanodes in Bicarbonate Electrolytes},

author = {G D Zhou and C C Aletsee and A Lemperle and T Rieth and L Mengel and J Y Gao and M Tschurl and U Heiz and I D Sharp},

url = {\<Go to ISI\>://WOS:001530023100001},

doi = {10.1021/acscatal.5c03025},

issn = {2155-5435},

year  = {2025},

date = {2025-08-01},

journal = {Acs Catalysis},

volume = {15},

number = {15},

pages = {13048-13058},

abstract = {The photoelectrochemical hydrogen peroxide evolution reaction (HPER) has attracted increasing attention as an environmentally friendly approach to generate a commercially and industrially valuable water oxidation product. BiVO4 photoanodes operated in bicarbonate-containing electrolytes have been shown to offer remarkable performance characteristics for HPER, with HCO3 - serving as a reaction mediator. However, the factors affecting the stability of both the semiconductor photoanode and the aqueous electrolyte remain poorly understood. Here, we investigated BiVO4 photoanodes to quantitatively assess the roles of electrolyte composition, bias potential, and illumination on competitive reaction pathways associated with HPER, oxygen evolution reaction, and photocorrosion. Our results confirm that HCO3 - serves as a highly efficient mediator, leading to rapid hole extraction and near complete suppression of interfacial recombination on BiVO4. In addition, these favorable hole transfer kinetics significantly decrease the rate of photocorrosion, leading to dramatically enhanced stability compared to bicarbonate-free electrolytes. While the elevated pH of unbuffered bicarbonate electrolyte leads to gradual chemical attack of BiVO4, the stability is greatly enhanced in near-neutral buffered bicarbonate electrolytes. Finally, we confirm that HCO3 - is regenerated during the photoanodic reaction, though pH swings during operation in an unbuffered electrolyte can lead to electrolyte instabilities. Overall, we find that BiVO4 photoanodes operating in buffered bicarbonate-containing solutions exhibit significantly enhanced stability and can efficiently drive water oxidation reactions, including HPER, thus providing a route to robust production of high value oxidation products.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {The Role of Defects in the Photocatalytic Conversion of Alcohols on Rutile TiO2(110)},

author = {P Petzoldt and L Mengel and S Mackewicz and C A Walenta and M Tschurl and U Heiz},

url = {\<Go to ISI\>://WOS:001529526500001},

doi = {10.1021/acscatal.5c03149},

issn = {2155-5435},

year  = {2025},

date = {2025-08-01},

journal = {Acs Catalysis},

volume = {15},

number = {15},

pages = {12859-12869},

abstract = {The role of defects is controversially discussed in photocatalysis. Commonly, they are seen as trap states for photon-generated charge carriers, which either promote charge separation and enhance the activity of the photocatalyst or act as recombination centers and lower the photocatalytic performance of the material. The present work illustrates the crucial role of defects as potential reaction centers in photocatalysis. We show that the photocatalytic activity of a rutile TiO2(110) single crystal toward alcohols in the gas phase can be varied by its degree of reduction. Specific heat treatments of the semiconductor lead to the formation of different concentrations of defect states, in particular bridge-bonded oxygen vacancies (BBOV), to which we assign the role of photoactive sites. Here, the dissociative adsorption of the alcohol and its subsequent photoconversion occurs. Our evaluation of the catalytic methanol photooxidation under different reaction conditions further reveals the importance of alcohol surface diffusion, whose influence on the catalytic activity is rationalized based on a capture zone around each BBOV. If a methanol molecule hits the TiO2 surface in this zone, it can be photoconverted even when it does not land directly on the photoactive site. Finally, an analysis of the return to the dark state of reactant and products upon interrupting the illumination enables us to determine methoxy coverages on the photocatalyst prior to illumination, which also scale with the concentration of BBOVs. We find that methoxies abound on Pt-loaded titania in the dark, which explains the increased product formation in the first seconds of photocatalysis.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Identification of Hexagonal Boron Nitride Thickness on SiO2/Si Substrates by Colorimetry and Contrast},

author = {E Blundo and N H T Schmidt and A V Stier and J J Finley},

url = {\<Go to ISI\>://WOS:001549028800001},

doi = {10.3390/app15158400},

year  = {2025},

date = {2025-07-29},

journal = {Applied Sciences-Basel},

volume = {15},

number = {15},

abstract = {Hexagonal boron nitride (hBN) is a layered material with a wide variety of excellent properties for emergent applications in quantum photonics using atomically thin materials. For example, it hosts single-photon emitters that operate up to room-temperature, it can be exploited for atomically flat tunnel barriers, and it can be used to form high finesse photonic nanocavities. Moreover, it is an ideal encapsulating dielectric for two-dimensional (2D) materials and heterostructures, with highly beneficial effects on their electronic and optical properties. Depending on the use case, the thickness of hBN is a critical parameter and needs to be carefully controlled from the monolayer to hundreds of layers. This calls for quick and non-invasive methods to unambiguously identify the thickness of exfoliated flakes. Here, we show that the apparent color of hBN flakes on different SiO2/Si substrates can be made to be highly indicative of the flake thickness, providing a simple method to infer the hBN thickness. Using experimental determination of the colour of hBN flakes and calculating the optical contrast, we derived the optimal substrates for the most reliable hBN thickness identification for flakes with thickness ranging from a few layers towards bulk-like hBN. Our results offer a practical guide for the determination of hBN flake thickness for widespread applications using 2D materials and heterostructures.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Collective motion of methylammonium cations affects phase transitions and self-trapped exciton emission in A-site engineered MAPbI3 films},

author = {C H Yeh and W Y Cheng and T C Chou and Y C Liu and C W Chang and Y S Chen and C H Wang and S C Weng and I D Sharp and P T Chou and C M Jiang},

url = {\<Go to ISI\>://WOS:001541463200001},

doi = {10.1039/d5na00599j},

issn = {2516-0230},

year  = {2025},

date = {2025-07-28},

journal = {Nanoscale Advances},

abstract = {Hybrid organic-inorganic halide perovskites are celebrated for their exceptional optoelectronic properties and facile fabrication processes, making them prime candidates for next-generation photovoltaic and optoelectronic devices. By incorporating larger organic cations at the A-site, a novel class of '3D hollow perovskites' has been developed, exhibiting enhanced stability and tunable optoelectronic properties. This study systematically explores the structural, phase transition, and photophysical characteristics of enMAPbI3 thin films with varying ethylenediammonium (en2+) content. The incorporation of less polar en2+ expands the perovskite unit cell, prolongs carrier lifetimes, and disrupts MA+ dipole-dipole interactions, thereby lowering the tetragonal-to-orthorhombic phase transition temperature. Temperature-dependent photoluminescence studies reveal that en2+ incorporation reduces the intensity and Stokes shift of self-trapped exciton emission at low temperatures, which are attributed to the diminished collective rotational dynamics of MA+ cations. These findings underscore the critical role of A-site cation dynamics in modulating phase stability and excitonic behaviour within hybrid halide perovskites, deepening our understanding of the interplay between organic cations and the inorganic framework and highlighting the potential of 3D hollow perovskites for stable and tunable optoelectronic applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Bringing Attomolar Detection to the Point-of-Care with Nanopatterned DNA Origami Nanoantennas},

author = {R Yaadav and K Trofymchuk and M Dass and V Behrendt and B Hauer and J Sch\"{u}tz and C Close and M Scheckenbach and G Ferrari and L M\"{a}urer and S Sebina and V Glembockyte and T Liedl and P Tinnefeld},

url = {\<Go to ISI\>://WOS:001536107000001},

doi = {10.1002/adma.202507407},

issn = {0935-9648},

year  = {2025},

date = {2025-07-26},

journal = {Advanced Materials},

abstract = {Creating increasingly sensitive and cost-effective nucleic acid detection methods is critical for enhancing point-of-care (POC) applications. This requires highly specific capture of biomarkers and efficient transduction of capture events. However, the signal from biomarkers present at extremely low amounts often falls below the detection limit of typical fluorescence-based methods, necessitating molecular amplification. Here, we present single-molecule detection of a non-amplified, 151-nucleotide sequence specific to antibiotics-resistant Klebsiella pneumoniae down to attomolar concentrations, using Trident NanoAntennas with Cleared HOtSpots (NACHOS). This NACHOS-diagnostics assay leverages a compact microscope with a large field-of-view, including microfluidic flow to enhance capturing efficiency. Fluorescence enhancement is provided by NanoAntennas, arranged using a combination of nanosphere lithography and site-specific DNA origami placement. This method can detect 200 +/- 50 out of 600 molecules in a 100 mu L sample volume within an hour. This represents a typical number of pathogens in clinical samples commonly detected by Polymerase Chain Reaction. We achieve similar sensitivity in untreated human plasma, enhancing the practical applicability of the system. This platform can be adapted to detect shorter nucleic acid fragments that are not compatible with traditional amplification-based technologies. This provides a robust and scalable solution for sensitive nucleic acid detection in diverse clinical settings.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Spatially resolved photocatalytic active sites and quantum efficiency in a 2D semiconductor},

author = {O Henrotte and S Saris and F Gr\"{o}bmeyer and C G Gruber and I Bilgin and A H\"{o}gele and N J Halas and P Nordlander and E Cort\'{e}s and A Naldoni},

url = {\<Go to ISI\>://WOS:001538017700012},

doi = {10.1038/s41467-025-62284-x},

year  = {2025},

date = {2025-07-26},

journal = {Nature Communications},

volume = {16},

number = {1},

abstract = {Identifying reactive sites and measuring their activities is crucial for enhancing the efficiency of every catalyst. Reactivity maps can guide the development of next-generation photocatalysts like 2D transition metal dichalcogenides, which suffer from low conversion rates. While their electrocatalytic sites are well-studied, their photocatalytic sites remain poorly understood. Using scanning photoelectrochemical microscopy, we spatially resolve the photoreactivity of MoS2 monolayers, a prototypical 2D transition metal dichalcogenide, for redox reactions, including H2 production from water. Aligned-unaligned excitation-detection measurements reveal that photogenerated holes and electrons exhibit distinct behaviors. Oxidation products localize at the excitation spot, indicating stationary holes, while photoreduction occurs up to at least 80 microns away, showing exceptional electron mobility. We also elucidate the photochemical reactivity according to the nature of the electronic excitation, showing that the internal quantum efficiency of strongly-bound A-excitons outperforms weakly-bound (free-carrier like) C-excitons across the flake. These findings offer novel guidance to rationally design 2D photocatalysts via engineering their optical and charge extraction abilities for efficient solar energy conversion.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {An improved guess for the variational calculation of charge-transfer excitations in large systems},

author = {N Bogo and Z Y Zhang and M Head-Gordon and C J Stein},

url = {\<Go to ISI\>://WOS:001544470300001},

doi = {10.1039/d5cp01867f},

issn = {1463-9076},

year  = {2025},

date = {2025-07-25},

journal = {Physical Chemistry Chemical Physics},

abstract = {Ab initio quantum-chemical methods that perform well for computing the electronic ground state are not straightforwardly transferable to electronically excited states, particularly in large molecular systems. Wave function theory offers high accuracy, but is often prohibitively expensive. Methods based on time-dependent density functional theory (TD-DFT) are crucially sensitive to the chosen exchange-correlation functional (XCF) parameterization, and system-specific tuning protocols were therefore proposed to address the method's robustness. Methods based on the variational relaxation of the excited-state electron density showcased promising results for the calculation of charge-transfer excitations, but the complex shape of the electronic hypersurface makes convergence to a specific excited state much more difficult than for the ground state when standard variational techniques are applied. We address the latter aspect by providing suitable initial guesses, which we obtain by two separate constrained algorithms. Combined with the squared-gradient minimization algorithm for all-electrons relaxation in a freeze-and-release scheme (FRZ-SGM), we demonstrate that orbital-optimized density functional theory (OO-DFT) calculations can reliably converge to the charge-transfer states of interest even for large molecular systems. We test the FRZ-SGM method on a phenothiazine-anthraquinone CT excitation in a supramolecular Pd(ii) coordination cage complex as a function of the cage conformation. This compound has been studied experimentally prior to our work. We compare this freeze-and-release scheme to two XCF reparameterizations, which were recently proposed as low-cost TD-DFT-based alternatives to variational methods. Two dye-semiconductor complexes, which were previously investigated in the context of photovoltaic applications, serve as a second example to investigate the convergence and stability of the FRZ-SGM approach. Our results demonstrate that FRZ-SGM provides reliable convergence for charge-transfer excited states and avoids variational collapse to lower-lying electronic states, whereas time-dependent DFT calculations with an adequate tuning procedure for the range-separation parameter provide a computationally efficient initial estimate of the corresponding energies, with a computational cost comparable to that of configuration-interaction singles (CIS) calculations.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Near-Infrared Emitting Lanthanide Catecholate Giant Single Crystals - Morphology Control and Photon Down-Conversion},

author = {M I Sch\"{o}nherr and A Biewald and A M\"{a}hringer and T J Koller and P Mayer and M D\"{o}blinger and A Hartschuh and D D Medina},

url = {\<Go to ISI\>://WOS:001535016700001},

doi = {10.1002/adfm.202507464},

issn = {1616-301X},

year  = {2025},

date = {2025-07-25},

journal = {Advanced Functional Materials},

abstract = {Lanthanide coordination polymers (Ln-CPs), an intriguing type of near-infrared (NIR) emitting materials, hold significant potential as fast-response platforms in light-emitting devices. The controlled crystallization of a series of Ln-DHBQ (2,5-dihydroxy-1,4-benzoquinone) CPs yielding photoactive single crystals is reported herein. Single crystal X-ray diffraction analysis revealed the impact of the synthesis conditions employed on the structure of Ln-DHBQ CPs. Hereby, the well-known isostructural series of [Ln2(C6H2O4)3(H2O)6]18H2O (Ln = Yb (1), Nd (3)) is expanded with a novel member [Ln2(C6H2O4)3(H2O)4]6H2O (Ln = Yb (2)), that crystallizes in the monoclinic space group C2/m instead of the trigonal space group R 3$bar 3$, which is typical of the parent series. Scanning electron microscopy and optical microscopy images showed that controlover the size and morphology of Yb-DHBQ and Nd-DHBQ crystals was achieved, where emerging as either disc-like single crystals of up to 100 mu m in size or faceted large single crystals up to 500 mu m, respectively. This series of Ln-DHBQ (1-3) features NIR photoluminescence with nanosecond lifetimes. Photon bunching is observed on the timescale of the excited-state lifetime in the second-order time correlation function, demonstrating a photon down-conversion process for both Yb-DHBQ CPs. This places Ln-DHBQ crystals as excellent candidates for the development of operational platforms requiring intense and short period light emission read out cycles.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Defects Dynamic in Photo-Excited CeO2 and their Influence on CO2 Photoreduction},

author = {R Yalavarthi and S B Mishra and O Henrotte and E Cortes},

url = {\<Go to ISI\>://WOS:001527447200001},

doi = {10.1002/adfm.202513933},

issn = {1616-301X},

year  = {2025},

date = {2025-07-14},

journal = {Advanced Functional Materials},

abstract = {Defects play a crucial role in shaping the efficiency and performance of semiconductor-based technologies. Under illumination, the interaction between photo-excited charge carriers and defect states in the semiconductor can significantly influence the response of devices and catalysts. Here, an X-ray photoelectron spectroscopy study conducted under light excitation is presented to track exciton generation and its interaction with defects in CeO2, a widely used metal-oxide support in (photo) catalysis. The light intensity-dependent measurements reveal that photo-excited electrons in CeO2 can effectively reduce Ce4+ to Ce3+. Surface-enhanced Raman spectroscopy further highlights the critical role of Ce3+ states in governing charge and energy transport across the CeO2-molecule interface. Finally, how these photo-induced states (Ce3+) can be leveraged is demonstrated to control the selectivity in the photocatalytic CO2 reduction reaction, dramatically influencing the yields of CO, CH4, and H2.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Optimized Oxidation Temperature Enhances OER Performance of IrO2-Loaded SnO2 Nanofibers - Role of Charge Carrier Percolation Pathways},

author = {M Kost and J F Dushimineza and K M\"{u}ller-Caspary and T Bein},

url = {\<Go to ISI\>://WOS:001527460600001},

doi = {10.1002/admi.202400997},

issn = {2196-7350},

year  = {2025},

date = {2025-07-14},

journal = {Advanced Materials Interfaces},

volume = {12},

number = {14},

abstract = {The potential for reducing iridium content in large-scale proton-exchange membrane (PEM) electrolysis is examined using a fibrous support morphology to enhance electron percolation. Focusing on high activity, stability, and conductivity, ultra-small, interconnected IrOx/IrO2 nanoparticles anchored to electrospun SnO2 nanofibers (IrOx/IrO2@SnO2) are investigated, with particular attention to the crystallinity of the iridium phase. Scanning transmission electron microscopy (STEM), conducted both before and after use as an electrocatalyst for the oxygen evolution reaction (OER), reveals how the oxidation temperature impacts the crystallinity and stability of the iridium oxide phase. The results suggest that further reductions in iridium content may be achieved by optimizing synthesis parameters. Here, the highest iridium utilization is achieved at an oxidation temperature of 375 degrees C, with improved conductivity and electrochemical activity. Transmission electron microscopy (TEM) indicates that higher oxidation temperatures result in fragmentation of conduction pathways, negatively affecting catalyst performance. Furthermore, TEM reveals the onset of IrO2 crystallization between 365 and 375 degrees C, with cyclic voltammetry (CVA) emphasizing the critical role of conductivity in ensuring efficient charge carrier transport to active sites. This study not only deepens the understanding of iridium-based catalysts but also identifies practical strategies to enhance cost-effectiveness and efficiency in PEM electrolysis technologies.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Design Rules for Perovskite Nanocrystals: Volume-Governed Absorption Versus Shape-Controlled Auger Recombination},

author = {A Singldinger and P Haussmann and G Debuisschert and N A Henke and J Paul and L Luber and P Ganswindt and A Abfalterer and A S Urban},

url = {\<Go to ISI\>://WOS:001523269600001},

doi = {10.1002/adom.202501137},

issn = {2195-1071},

year  = {2025},

date = {2025-07-07},

journal = {Advanced Optical Materials},

abstract = {Understanding the interplay between morphology and optical properties in lead halide perovskite nanocrystals is critical for advancing optoelectronic applications. In this study, the one-photon absorption (OPA) cross-section and biexciton Auger lifetimes of CsPbBr3 nanocrystals with varying dimensionality, including nanocubes, nanoplatelets, and nanorods, are investigated. Using ultrafast transient absorption spectroscopy, the OPA cross-section is extracted from fluence-dependent measurements and the decay dynamics of excitonic states are examined. The results reveal that the OPA cross-section scales linearly with nanocrystal volume, irrespective of morphology, providing the most comprehensive experimental validation of this relationship to date. Furthermore, the universal volume scaling law for biexciton Auger recombination is confirmed in the strong confinement regime, but deviations from it in the weak confinement regime are demonstrated. The biexciton Auger lifetime saturates for nanocrystals with dimensions exceeding the exciton Bohr radius, while nanorods and nanoplatelets exhibit shape-dependent confinement effects that influence their carrier recombination dynamics. These findings offer valuable insights into the design of perovskite nanocrystals for high-performance optoelectronic devices, including light-emitting diodes, lasers, and photodetectors.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Numerically efficient quasi-adiabatic propagator path integral approach with two independent non-commuting baths},

author = {R Ovcharenko and B P Fingerhut},

url = {\<Go to ISI\>://WOS:001523461500005},

doi = {10.1063/5.0271212},

issn = {0021-9606},

year  = {2025},

date = {2025-07-07},

journal = {Journal of Chemical Physics},

volume = {163},

number = {1},

abstract = {Path integral methods, such as the quasi-adiabatic propagator path integral (QUAPI), are widely used in general-purpose and highly accurate numerical benchmark simulations of open quantum systems, particularly in regimes inaccessible to perturbative methods. Nevertheless, the applicability of the QUAPI method to realistic systems of interest is restricted by the exponentially growing computer memory requirements with respect to the size of the quantum system and the time range of non-Markovian correlation effects. This exponential "wall" becomes even more severe for multiple non-commuting fluctuating environments. In the present work, we address the numerical efficiency and accuracy of approximations that have been introduced for the QUAPI method with a single general environment, for the case of two independent non-commuting environments where one of them is considered as a pure dephasing environment. In particular, we consider a sharply defined cutoff of the memory time, path filtering, and mask assisted coarse graining of influence functional coefficients as approximations. We demonstrate that commonly applied numerical techniques, such as path filtering, cannot be straightforwardly transferred to the two-bath case even in the weak-coupling and quasi-Markovian limits. On the other hand, the sharply defined memory cutoff can be accurately handled with the mask assisted coarse graining approach. Our findings demonstrate that if system coupling operators to different baths do not commute, the additive nature of the statistically independent environments may be misleading. In particular, the quasi-Markovian nature of a pure dephasing bath is lost once there simultaneously exists another non-commuting source of fluctuations. (c) 2025 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license(https://creativecommons.org/licenses/by/4.0/)},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

doi = {10.1002/admi.202500298},

issn = {2196-7350},

year  = {2025},

date = {2025-07-04},

journal = {Advanced Materials Interfaces},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Predict before You Precipitate: Learning Templating Effects in Hybrid Antimony and Bismuth Halides},

author = {J Blahusch and K S Jakob and J T Margraf and K Reuter and B V Lotsch},

url = {\<Go to ISI\>://WOS:001522359000001},

doi = {10.1021/acs.chemmater.5c00350},

issn = {0897-4756},

year  = {2025},

date = {2025-07-02},

journal = {Chemistry of Materials},

abstract = {Hybrid organic-inorganic (HOI) antimony and bismuth halides exhibit diverse structural features and have been studied intensely for their promising electronic and optical properties. There are well-explored structure-property relations for these materials. However, a thorough understanding of the synthesis routes and templating effects is lacking, turning their targeted synthesis into an open challenge. In this study, we assemble a literature data set of established HOI material candidates and train an explainable machine learning classification model to explore the templating effects in more detail. With a classification accuracy upward of 70%, our model is effective in predicting HOI structure types based on the reactants and points out several structural and electrostatic design features for the organic cation that influence the inorganic substructure most strongly. We further demonstrate the validity of our classifier on 9 newly synthesized members of this materials class and propose incremental learning routes to expand the model in future research.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Sulfur Mediated Interfacial Proton-Directed Transfer Boosts Electrocatalytic Nitric Oxide Reduction to Ammonia over Dual-Site Catalysts},

author = {Z L Wang and H Y Duan and W Q Qu and D L Han and X C Li and L Zhu and X Jiang and D H Cheng and Y J Shen and M Xie and E Cortes and D S Zhang},

url = {\<Go to ISI\>://WOS:001524469700001},

doi = {10.1002/anie.202511398},

year  = {2025},

date = {2025-07-01},

journal = {Angewandte Chemie-International Edition},

abstract = {Electrocatalytic nitric oxide reduction reaction (NORR) for ammonia (NH3) synthesis represents a sustainable strategy that simultaneously realizes the nitrogen cycle and resource integration. The key issue hindering the NORR efficiency is accelerating proton (*H) transfer to facilitate NO hydrogenation while inhibiting the hydrogen evolution reaction (HER). Herein, we demonstrate an interface-engineered sulfur-mediated Cu@Co electrocatalyst (S-Cu@Co/C) that boosts NORR performance through dual modulation of electronic structure and proton transfer on active sites. A comprehensive program of experimental and theoretical calculations was employed to discover that sulfur incorporation induces electron redistribution in the Cu-Co interface, creating electron-rich sulfur and electron-deficient metals. This electronic configuration synergistically enhances NO adsorption on Cu sites and promotes water dissociation on Co sites. More critically, sulfur could direct the rapid transfer of *H from Co to Cu sites, thereby accelerating the NO hydrogenation and suppressing HER. Consequently, S-Cu@Co/C achieves an NH3 yield rate of 655.3 mu mol h-1 cm-2 in a flow cell and a Faradaic efficiency of 92.4% in an H-cell. Remarkably, the catalyst could maintain continuous electrolysis tests and steady NH3 yield up to 100 h. This work provides innovative insights into the fabrication of efficient electrocatalysts via heteroatom-mediated interfacial engineering strategies.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Near-Unity Nitrate to Ammonia conversion via reactant enrichment at the solid-liquid interface},

author = {W R Liao and J Wang and Y Tan and X Zi and C X Liu and Q Y Wang and L Zhu and C W Kao and T S Chan and H M Li and Y L Zhang and K Liu and C Cai and J W Fu and B D Xi and E Cortes and L Y Chai and M Liu},

url = {\<Go to ISI\>://WOS:001523450400034},

doi = {10.1038/s41467-025-60671-y},

year  = {2025},

date = {2025-07-01},

journal = {Nature Communications},

volume = {16},

number = {1},

abstract = {Electroreduction of nitrate (NO3-) to ammonia (NH3) is a promising approach for addressing energy challenges. However, the activity is limited by NO3- mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO3- from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO3- concentration decreases, impeding practical applications in the conversion of NO3\textendashto-NH3. Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO3- reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS2 (Ag-MoS2) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO3-. Thus, Ag-MoS2 exhibits a similar to 28.6-fold NO3- concentration in the IHP than the counterpart without junction, and achieves near-100% NH3 Faradaic efficiency with an NH3 yield rate of similar to 20 mg h(-1) cm(-2) under ultralow NO3- concentrations.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2211-2855},

year  = {2025},

date = {2025-07-01},

journal = {Nano Energy},

volume = {140},

pages = {111043},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {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 = {Exploring On-Surface Synthesis under Mild Conditions},

author = {Y Q Zhang and J Bj\"{o}rk and J V Barth},

url = {\<Go to ISI\>://WOS:001518560000001},

doi = {10.1021/acs.accounts.5c00157},

issn = {0001-4842},

year  = {2025},

date = {2025-06-26},

journal = {Accounts of Chemical Research},

abstract = {Bottom-up approaches combining tailor-made molecular precursors and surface-mediated reactions under ultrahigh-vacuum (UHV) conditions attracted significant attention over the past decade as a promising strategy for synthesizing novel, functional, molecule-based materials. These methods have been remarkably successful in creating unconventional covalent products with atomic precision, though largely focusing on one-dimensional (1D) polymeric products. Extending the established protocols to synthesize two-dimensional (2D) covalent architectures presents a major challenge, primarily due to high annealing temperatures required that often entail competing reactions, high defect densities, and structural degradation.In this Account, we highlight the exciting potential of low-temperature (LT) on-surface reactions as an alternative pathway and discuss their largely unexploited capabilities. We summarize major recent advances, focusing on coinage metal surface-assisted chemical transformations at mild conditions in UHV, proceeding frequently near or below room temperature (RT). Special emphasis is placed on alkyne derivatives, either alone or combined with other functional groups, identified as versatile building blocks for next-generation carbon-rich nanomaterials such as graphyne or graphdiyne and their metalated derivatives, which offer immense potential for future technological applications.We discuss four major pathways for initiating LT on-surface reactions of alkyne species, following largely the chronological order of their discovery, and merging insights from high-resolution scanning probe microscopy, X-ray spectroscopies and density functional theory calculations: (i) Conversions catalyzed by in situ generated species and extrinsic elements; (ii) quantum tunneling-mediated reactions; (iii) reaction pathways involving surface-assisted radical or hydrogen transfer processes; and (iv) gas-mediated on-surface reactions. These and other selected examples of LT synthesis protocols offer significant advantages in terms of high selectivity and efficiency, notably enabling the controlled synthesis of extended, regular 2D organometallic and covalent compounds or architectures, and bearing promise for a multitude of all-carbon scaffolds, which currently remain challenging. We aim to inspire the development of functional robust nanoarchitectures with long-range order and atomic-scale precision, contributing to the advancement of molecule-based materials for diverse technological applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Efficient near-infrared harvesting in perovskite-organic tandem solar cells},

author = {Z R Jia and X Guo and X X Yin and M Sun and J W Qiao and X Y Jiang and X Wang and Y D Wang and Z J Dong and Z J Shi and C H Kuan and J C Hu and Q L Zhou and X K Jia and J X Chen and Z Y Wei and S C Liu and H M Liang and N X Li and L K Lee and R J Guo and S V Roth and P Mueller-Buschbaum and X T Hao and X Y Du and Y Hou},

url = {\<Go to ISI\>://WOS:001516586700001},

doi = {10.1038/s41586-025-09181-x},

issn = {0028-0836},

year  = {2025},

date = {2025-06-25},

journal = {Nature},

abstract = {The broad bandgap tunability of both perovskites and organic semiconductors enables the development of perovskite-organic tandem solar cells with promising theoretical efficiency. However, the certified efficiencies of reported perovskite-organic tandem solar cells remain lower than those of single-junction perovskite solar cells, primarily because of insufficient near-infrared photocurrent in narrow-bandgap organic subcells1, 2-3. Here we design and synthesize an asymmetric non-fullerene acceptor (NFA), P2EH-1V, featuring a unilateral conjugated pi-bridge to reduce the optical bandgap to 1.27 eV while maintaining ideal exciton dissociation and nanomorphology. Transient absorption spectroscopy confirms efficient hole transfer from P2EH-1V to the donor PM6. Devices based on P2EH-1V exhibit reduced non-radiative voltage losses of 0.20 eV without compromising charge-generation efficiency. We achieve a 17.9% efficiency for the organic bottom cell, with a high short-circuit current density (Jsc) of 28.60 mA cm-2. Furthermore, we minimize interface recombination losses, enabling the perovskite top cell to achieve an impressive open-circuit voltage (Voc) of 1.37 V and a fill factor (FF) of 85.5%. These advancements result in perovskite-organic tandem solar cells achieving a record efficiency of 26.7% (certified at 26.4%) over an aperture area greater than 1 cm2.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Role of Manganese Oxide Nanosheets in Pyrolyzed Carbonaceous Supports for Water Oxidation},

author = {A Wark and T O Schmidt and R W Haid and R M Kluge and S Suzuki and Z Siroma and E Sk\'{u}lason and A S Bandarenka and J Maruyama},

url = {\<Go to ISI\>://WOS:001516876000001},

doi = {10.1021/acs.chemmater.5c00212},

issn = {0897-4756},

year  = {2025},

date = {2025-06-23},

journal = {Chemistry of Materials},

abstract = {The oxygen-evolving complex in photosystem II, a manganese-oxide-based cluster, is nature's solution for water oxidation, while most efficient artificial catalysts consist of costly noble-metal-based oxides. However, tackling the upcoming challenges of the climate crisis requires sustainable electrocatalysts based on affordable and efficient materials. Herein, we extensively probe carbonized iron phthalocyanine without and with deposited manganese-oxide nanosheets as model electrocatalysts mimicking the biological solution. We employed electrochemical and spectroscopic techniques, noise electrochemical scanning tunneling microscopy, and density functional theory calculations to understand their water-splitting performance holistically. Both compound materials show remarkable electrocatalytic activity, outperforming previously investigated systems based on earth-abundant elements. The origin of this enhanced performance is assigned to the metal centers and the edges at the substrate-nanosheet interface, providing the design guidelines to optimize further sustainable and affordable electrocatalysts for water oxidation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Machine-Learning Force Fields Reveal Shallow Electronic States on Dynamic Halide Perovskite Surfaces},

author = {F P Delgado and F Simoes and L Kronik and W Kaiser and D A Egger},

url = {\<Go to ISI\>://WOS:001514111900001},

doi = {10.1021/acsenergylett.5c01519},

issn = {2380-8195},

year  = {2025},

date = {2025-06-23},

journal = {Acs Energy Letters},

abstract = {Previous studies indicated that defects in halide perovskites can generate shallow electronic states, which are crucial for their performance in devices. However, how shallow states persist amid pronounced atomic dynamics on halide perovskite surfaces remains unknown. We reveal that electronic states at surfaces of prototypical CsPbBr3 are energetically distributed at room temperature, akin to well-passivated inorganic semiconductors, despite the presence of undercoordinated atoms and cleaved bonds. Notably, approximately 70% of surface-state energies appear within 0.2 eV of the valence-band edge. Although deep states can still form, they are rarely energetically isolated and are less likely to act as traps. Accelerating first-principles calculations via machine learning, we show that the unique atomic dynamics in halide perovskites render the formation of deep electronic states at their surfaces unlikely. These findings reveal the microscopic mechanism behind the low density of deep states at dynamic halide perovskite surfaces, which is key to their device performance.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {The Haber Bosch Catalyst from Solid state Chemistry to Mesotechnology},

author = {K Demb\'{e}l\'{e} and J H Wang and M Boniface and J Folke and L S Diaz and F Girgsdies and A Hammud and D Kordus and G Koch and Z Gheisari and R Blume and W L Y Jiang and A Knop-Gericke and R Eckert and S Reitmeier and A Reitzmann and R Schl\"{o}gl and B R Cuenya and J Timoshenko and H Ruland and T Lunkenbein},

url = {\<Go to ISI\>://WOS:001510987900001},

doi = {10.1002/aenm.202500159},

issn = {1614-6832},

year  = {2025},

date = {2025-06-19},

journal = {Advanced Energy Materials},

abstract = {Ammonia is industrially synthesized over multi-promoted Fe-based catalysts for more than a century. Although ammonia synthesis reflects a prototypical catalytic reaction, rational catalyst design is still impossible as the full structural complexity of this catalyst system often referred to as ammonia iron and its structural entanglement is barely understood. Here, the mesoscopic structure of a technical, multi-promoted ammonia synthesis catalyst is uncovered using a scale-bridging electron microscopy approach complemented by X-ray diffraction and spectroscopy to explore the structural integrity of ammonia iron. Amorphous contributions and structures of the melilite type and tricalcium aluminate as additional phases are identified. Furthermore, the understanding of the ammonia iron family by unveiling the role of the platelet-Fe perimeter, framework Fe, thin film Fe, and refractory Fe is extended. Their interconnectedness is highlighted, suggesting that each component has to be present to fulfill a specific task. The study demonstrates that catalysis science can only proceed if it openly explores the full complexity of catalytic systems.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Electron Spillover into Water Layers: A Quantum Leap in Understanding Capacitance Behavior},

author = {L Li and T Eggert and K Reuter and N G H\"{o}rmann},

url = {\<Go to ISI\>://WOS:001518032200001},

doi = {10.1021/jacs.5c04728},

issn = {0002-7863},

year  = {2025},

date = {2025-06-18},

journal = {Journal of the American Chemical Society},

volume = {147},

number = {26},

pages = {22778-22784},

abstract = {We investigate the electronic and molecular properties of the electrified Pt(111)-water interface using molecular dynamics simulations, leveraging electronic-structure-aware density-functional theory (DFT) and classical force field approaches. Electrification is induced by introducing excess electrons with homogeneously distributed, nonionic counter-charges, allowing for a targeted analysis of electronic and water density responses without interference from electrolyte ions. Our results reveal that, within the DFT framework, the Pt(111)-water interface deviates from the classical picture, where excess electronic charge remains localized at the metallic surface. Instead, approximately 30-40% of the electronic excess charge density penetrates into the interfacial water region-a behavior that is absent in vacuum conditions or when using classical force fields. This redistribution of charge provides a compelling explanation for long-standing discrepancies in the modeling of this interface, including the stabilization of partially charged interfacial species such as H+ and most importantly the severe underestimation-by an order of magnitude-of the interfacial capacitance in force-field-based methods. Our findings highlight the crucial role of electronic charge spillover in defining interfacial behavior which provides critical insights about the approximations in classical descriptions and for the development of more accurate computational models of electrochemical systems.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Exploring the Electrochemical Stability Window of an All-Solid-State Composite Cathode via a Novel Operando Tender XPS Setup},

author = {R Wilhelm and R Schuster and T Kutsch and S M Qian and J Mahl and T Kratky and J Wandt and E J Crumlin and H A Gasteiger},

url = {\<Go to ISI\>://WOS:001514153300001},

doi = {10.1021/acsami.5c01672},

issn = {1944-8244},

year  = {2025},

date = {2025-06-18},

journal = {Acs Applied Materials \& Interfaces},

abstract = {All-solid-state batteries (ASSBs) have the potential to provide greater energy density than conventional batteries based on liquid electrolytes. Here, an operando ASSB cell setup for tender X-ray photoelectron spectroscopy (XPS) was developed, and the interface of a Ni-rich layered transition metal oxide cathode active material (CAM) and an Li6PS5Cl (LPSCl) solid electrolyte (SE) was evaluated during initial charge/discharge cycles. After validating the cell performance against a conventional pouch cell operated at high compression, intermittent galvanostatic cycling was performed, and XPS data were recorded as a function of state of charge (SOC). Upon the initial charge of the cell to approximate to 3.3 V-Li, the LPSCl appears to decompose into LiCl, Li3PS4, and polysulfides, whose amount gradually increases with potential. Upon further charge, at a potential higher than approximate to 3.8 V-Li, initially, present sulfate and sulfite impurities decompose, and at approximate to 74% SOC (corresponding to a cathode potential of approximate to 4.10 V-Li), surface reconstruction of the CAM particles due to lattice oxygen release is detected. In addition, at potentials beyond approximate to 4.6 V-Li, a decrease of the S 1s counts of the sum of the LPSCl, the thiophosphate, and polysulfide species suggests the formation of elemental sulfur that is lost via sublimation into the vacuum chamber.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Broadband shot-to-shot transient absorption anisotropy},

author = {M Binzer and F \v{S}anda and L Mewes and E Thyrhaug and J Hauer},

url = {https://doi.org/10.1063/5.0268081},

doi = {10.1063/5.0268081},

issn = {0021-9606},

year  = {2025},

date = {2025-06-16},

journal = {The Journal of Chemical Physics},

volume = {162},

number = {23},

pages = {234201},

abstract = {Transient absorption (TA) is the most widespread method to follow ultrafast dynamics in molecules and materials. The related method of TA anisotropy (TAA) reports on the ultrafast reorientation dynamics of transition dipole moments, reporting on phenomena ranging from electronic dephasing to orientational diffusion. While these are fundamental aspects complementary to TA, TAA is generally less widely used. The main reason is that TAA signals are usually not measured directly but are retrieved from two consecutive TA measurements with parallel (R‖) and perpendicular (R⊥) polarization of pump and probe pulses. This means that even minor systematic errors in these measurements lead to drastic changes in the TAA signal. In this work, the authors demonstrate alternating shot-to-shot detection of R‖ and R⊥, minimizing systematic errors due to laser fluctuations. The employed broadband detection lets us discuss effects dependent on detection wavelength in the ultrafast anisotropy decay of 2,3-naphthalocyanine, a system previously scrutinized by David Jonas and co-workers. In particular, we compare timescales of population relaxation and decoherence and support the proposals for isotropic type of relaxation in square symmetric molecules.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Highly Crystalline and Oriented Thin Films of Fully Conjugated 3D-Covalent Organic Frameworks},

author = {I Munoz-Alonso and D Bessinger and S Reuter and M Righetto and L Fuchs and M D\"{o}blinger and D D Medina and F Ortmann and L M Herz and T Bein},

url = {\<Go to ISI\>://WOS:001525541100001},

doi = {10.1002/anie.202505799},

year  = {2025},

date = {2025-06-15},

journal = {Angewandte Chemie-International Edition},

abstract = {Fully conjugated 3D covalent organic frameworks (COFs) are a newly emerged class of materials that expands reticular chemistry to extended electron delocalization for optoelectronic applications. To overcome the limitations of sp3-connected 3D frameworks, the pseudo-tetrahedral motif cyclooctatetrathiophene (COTh) has gained attention for forming fully conjugated 3D COFs. We report on a novel COTh building block, featuring functional formyl groups directly attached to the core's conjugated thiophenes. The modulation synthesis approach with mono-functionalized inhibitors enables the formation of COTh-1P COF, which exhibited remarkable crystallinity and permanent porosity. By following this approach and by optimizing the synthesis conditions for the solvothermal growth of thin films, we fabricated the first preferentially oriented conjugated 3D COF films on various substrates without pre-functionalization. With these thin films, optical pump terahertz probe studies allowed us, for the first time with 3D-fully conjugated COFs, to provide insights into the excited state and charge-carrier dynamics of these unique organic frameworks. Low effective masses are discovered for valence and conduction bands by density functional theory simulations. The ability to create crystalline and oriented films of fully pi-conjugated 3D COTh-based COFs on non-modified substrates is expected to open the way for integration of such frameworks into diverse optoelectronic applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}