Publikationen

@article{nokey,

title = {A Platform for the Development of Highly Red-Shifted Azobenzene-Based Optical Tools},

author = {K L\"{u}tzel and H Laqua and M B Sathian and B Nissl and J K Sz\'{a}nt\'{o} and C A Senser and G Savasci and L Allmendinger and B Kicin and V Ruf and D Kammerer and T Lohm\"{u}ller and K Karaghiosoff and A M Ali and U Storch and M M Y Schnitzler and C Ochsenfeld and D B Konrad},

url = {\<Go to ISI\>://WOS:001512840500001},

doi = {10.1002/anie.202501779},

year  = {2025},

date = {2025-06-04},

journal = {Angewandte Chemie-International Edition},

abstract = {Azobenzenes are versatile photoswitches that can be used to generate elaborate optical tools, including photopharmaceuticals. However, the targeted application-guided design of new photoswitches with specific properties remains challenging. We have developed synthetic protocols for derivatives of the dfdc (di-ortho-fluoro-di-ortho-chloro) azobenzene scaffold with chemical alterations in the para-/ortho-positions and performed an in-depth study into the effects of their structures on their photophysical properties with an emphasis on the n -\> pi* absorption band using NMR, UV-vis, and X-ray analysis. The data was used to establish and validate a computational approach that allows to compute realistic UV-vis spectra by combining TD-DFT excited-state calculations from 6000 thermally accessible structures generated through MD simulations while considering the high structural flexibility of ortho-substituted azobenzenes. We added 15 new visible light-operated photoswitches to the toolbox for the development of optical devices with relaxation rates across multiple orders of magnitude and identified several examples with stronger bathochromic shifts than the dfdc azobenzene lead structure. Our combined experimental and computational study forms the foundation for the advanced in silico design and synthesis of new highly red-shifted photoswitches. To showcase the potential of dfdc azobenzenes for the development of chemical tools, we synthesized dfdc-OptoBI-1 and demonstrated its biological activity as a red light-operated activator of TRPC6 channels in HEK293 cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Insight Generation from Information-Dense Formation Protocols},

author = {L Merker and B J Zhang and J Yuan and S L Ji and H S Stein},

url = {\<Go to ISI\>://WOS:001594137000001},

doi = {10.1002/batt.202500153},

year  = {2025},

date = {2025-06-03},

journal = {Batteries \& Supercaps},

abstract = {Accelerated formation protocols that utilize pulsed charging offer an unprecedented wealth of electrochemical data. Herein, methods are presented to extract diagnostic data relating to pseudodiffusion coefficients, internal resistance, and others that give live insight into solid electrolyte interphase (SEI) growth. Specifically, a purely mathematical method is used to track formation progression in near-real time and chart a path toward incorporation of adjustable pulse parameters for targeted SEI synthesis. The method and analysis are performed on 3 mAh cells but can also be applied to higher-capacity cells.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Identifying Bottlenecks in the Photocatalytic Oxygen Evolution Reaction with Covalent Organic Frameworks},

author = {S Trenker and H A Vignolo-Gonzalez and A Rodr\'{i}guez-Camargo and L Yao and M A Zwijnenburg and B V Lotsch},

url = {\<Go to ISI\>://WOS:001501845400001},

doi = {10.1021/acs.chemmater.5c00804},

issn = {0897-4756},

year  = {2025},

date = {2025-06-03},

journal = {Chemistry of Materials},

abstract = {Covalent organic frameworks (COFs) have emerged as promising semiconducting materials for photocatalytic applications due to their large surface area, high crystallinity, and vast synthetic tunability. This is especially noticeable in the context of photocatalytic water splitting, where many COFs have been employed for the hydrogen evolution half-reaction. There, sacrificial reagents typically replace the kinetically demanding oxygen evolution half-reaction. On the contrary, only few reports focus on (sacrificial) water oxidation with COF photocatalysts. In most of these cases, cobalt species are employed as oxygen evolution cocatalyst, often with limited insight into their structure and detailed role in the catalysis. Herein, we use heterogenization of a molecularly defined iridium half-sandwich complex onto a bipyridine-based COF (Ir@TAPB-BPY COF) and provide detailed structural insights ensuring the integrity of the targeted cocatalyst. First, we demonstrate the retained catalytic activity of the anchored Cp*Ir(III) motifs in chemical water oxidation experiments. In contrast, subsequent photocatalytic and electrocatalytic tests indicate that Ir@TAPB-BPY COF does not evolve oxygen and that careful control experiments have to be conducted in order to avoid false positive results, caused for example by the sacrificial electron acceptor. Using computational methods, we trace back the missing performance to thermodynamic and kinetic limitations of the employed systems. This work demonstrates the pitfalls associated with low-performing oxygen evolution photocatalysts as well as the indispensability of control experiments and their careful evaluation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Shifting Gears: Photochromic Metal-Organic Frameworks with Stimulus-Adaptable Performance},

author = {J Haimerl and G C Thaggard and B Kankanamalage and R B\"{u}hler and J Lim and K C Park and J Warnan and R A Fischer and N B Shustova},

url = {\<Go to ISI\>://WOS:001499947800001},

doi = {10.1021/jacs.5c04466},

issn = {0002-7863},

year  = {2025},

date = {2025-05-29},

journal = {Journal of the American Chemical Society},

abstract = {The tunability of the reaction parameter space is probed in the presented work through photoswitch-directed energy and charge transfer pathways induced by organic chromophores, hierarchically organized within a well-defined, light-harvesting metal-organic framework. Unique matrix-imposed changes in photoswitch photophysical properties, including the first report of visible light-induced photoisomerization of a spiropyran derivative, illustrate the critical synergy between the selected matrix and the photoresponsive compound. Moreover, the confined space of the utilized porous matrix allowed for mimicking isomerization kinetics of integrated sterically demanding photochromic moieties in solution. More importantly, such photoisomerization suppresses the charge transfer processes in favor of resonance energy transfer pathways instead. The demonstrated ability to shift between multiple relaxation pathways (e.g., charge transfer, energy transfer, or photoluminescence) as a function of the excitation wavelength resulted in photoswitch-directed tailoring of model phosphinylation reaction outcomes. Thus, incorporating spiropyran moieties within the framework allows for visible light to be harvested and funneled toward either a ligand-based reactive center or an acceptor molecule such as a photochromic unit. Moreover, the framework's chemical activity was promoted exclusively by organic linkers without the participation of metal nodes, the addition of (co)catalysts, or the use of harsh conditions at room temperature. Overall, this work paves the way for the development of stimulus-responsive platforms, for which chemical activity could be controlled through a photochromic moiety.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Impact of Halide Substitution in the Inorganic Framework on the Optical Activity of Chiral Metal-Halide Perovskites},

author = {N Solhtalab and S P Liu and M Kepenekian and L Hoffmann and J A Gessner and T Fischer and D Sandner and A Shcherbakov and J Zerhoch and S Bodnar and F Rominger and J Ballmann and C Katan and H Iglev and F Deschler},

url = {\<Go to ISI\>://WOS:001498687700001},

doi = {10.1021/acs.jpcc.5c02987},

issn = {1932-7447},

year  = {2025},

date = {2025-05-29},

journal = {Journal of Physical Chemistry C},

abstract = {The combination of chiroptical and semiconducting properties makes chiral hybrid metal-halide perovskites a promising class of materials for optoelectronic and optospintronic devices. Still, the detailed connection between the material composition and optical activity remains to be fully understood. Here, we study the effect of halogen substitution on optical activity in the chiral hybrid perovskite (R,S,rac)-3BrMBA2PbI4(1-x)Br4x . We find that an unusual sign-flip occurs in the circular dichroism (CD) spectrum as the optical gap blue-shifts with increasing bromide content. We explain this observation by shifts in the energy level alignment caused by the halide substitution. We also observed an inverse relationship between the CD intensity and the microstrain induced in the lattice for mixed-halide compositions, which we attribute to inhomogeneity in chirality transfer across the inorganic framework. Last but not least, transient Faraday rotation measurements reveal that the (R/S)-3BrMBA2PbBr4 system exhibits a significant spin lifetime even at room temperature, underscoring its potential for spintronic applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {An embedding scheme for constraint-based orbital-optimized excitations in molecular and bulk environments},

author = {Y Lemke and J Kussmann and C Ochsenfeld},

url = {http://dx.doi.org/10.1039/D5CP00839E},

doi = {10.1039/D5CP00839E},

issn = {1463-9076},

year  = {2025},

date = {2025-05-29},

journal = {Physical Chemistry Chemical Physics},

abstract = {We recently presented a novel approach to variationally determine electronically excited states based on constrained density functional theory calculations. The constraint-based orbital-optimized excited state method (COOX) [Kussmann et al., J. Chem. Theory Comput., 2024, 20, 8461\textendash8473] allows the evaluation of arbitrary electronic excitations and has several advantages compared to other methods like ΔSCF. In this work, we present an embedding scheme for COOX where the constraint potential is drawn from a sub-system calculation. This approach enables the accurate evaluation of specific excited states within complex environments that are difficult to obtain with conventional methods. The validity and range of applicability of the presented method are investigated for first exemplary calculations.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Rediscovery of the Forgotten Middle Child: A Comprehensive Study on the Coordination Chemistry of Melam},

author = {T J Koller and L G Balzat and J Blahusch and A Pichler and B V Lotsch and W Schnick},

url = {https://doi.org/10.1002/ejic.202500240},

doi = {https://doi.org/10.1002/ejic.202500240},

issn = {1434-1948},

year  = {2025},

date = {2025-05-28},

journal = {European Journal of Inorganic Chemistry},

volume = {28},

number = {15},

pages = {e202500240},

abstract = {Melam or bis(4,6-diamino-1,3,5-triazin-2-yl)amine is a chemical compound that has already been studied by Liebig almost 200?years ago. Despite this, melam's ability to act as a bidentate ligand has hardly been explored so far. The main focus of this work was therefore to advance the knowledge about melam's coordination chemistry by the synthesis of its complexes with CuCl, CuBr, CuI, CuCN, and AgCl as well as their structural characterization by single crystal and powder X-ray diffraction. Their crystal structures were found to feature channels along the molecules? stacking direction. It was further shown that these melam complexes have excellent hydrolytic and thermal stability, making them potentially interesting for heterogeneous catalysis in aqueous media either as promising precursors for polymeric carbon nitrides or possibly already on their own, especially since it should be possible to fine-tune properties by preparing solid solutions of these melam complexes, which was exemplarily demonstrated between the CuBr and CuI derivatives. Additionally, the crystal structure of melam's HCl salt was elucidated, which proved to be closely related to that of the coordination complex between melam and CuCl, underlining the similar chemical behavior of Cu+ and H+ toward melam.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Atomic-layer assembly of ultrathin optical cavities in van der Waals heterostructure metasurfaces},

author = {L Sortino and J Biechteler and L Lafeta and L K\"{u}hner and A Hartschuh and L D Menezes and S A Maier and A Tittl},

url = {\<Go to ISI\>://WOS:001495232400001},

doi = {10.1038/s41566-025-01675-4},

issn = {1749-4885},

year  = {2025},

date = {2025-05-26},

journal = {Nature Photonics},

abstract = {Photonics has been revolutionized by advances in optical metasurfaces, unlocking design and engineering opportunities for flat optical components. Similarly, layered two-dimensional materials have enabled breakthroughs in physics via the deterministic assembly of vertical heterostructures, allowing precise control over the atomic composition of each layer. However, integrating these fields into a single system has remained challenging, limiting progress in atomic-scale optical cavities and metamaterials. Here we demonstrate the concept of van der Waals heterostructure metasurfaces, where ultrathin multilayer van der Waals material stacks are shaped into precisely engineered resonant nanostructures for enhancing light-matter interactions. By leveraging quasi-bound states in the continuum physics, we create intrinsic high-quality-factor resonances originating from WS2 monolayers encapsulated in hexagonal boron nitride at thicknesses below 130 nm, achieving room-temperature strong coupling and polaritonic photoluminescence emission. Furthermore, the metasurface-coupled exciton-polaritons exhibit strong nonlinearities, leading to a saturation of the strong-coupling regime at ultralow fluences of \<1 nJ cm(-2), three orders of magnitude lower than in previous two-dimensional-material-based cavity systems. Our approach monolithically integrates metasurfaces and van der Waals materials and can be extended to the vast library of existing two-dimensional materials, unlocking new avenues for ambient operation of ultrathin polaritonic devices with atomic-scale precision and control.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

doi = {10.1021/acsnano.5c04141},

issn = {1936-0851},

year  = {2025},

date = {2025-05-22},

journal = {Acs Nano},

volume = {19},

number = {21},

pages = {20084-20095},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Molecular spectroscopies with semiconductor metasurfaces: towards dual optical/chemical SERS},

author = {A Berestennikov and H Y Hu and A Tittl},

url = {\<Go to ISI\>://WOS:001492589700001},

doi = {10.1039/d4tc05420b},

issn = {2050-7526},

year  = {2025},

date = {2025-05-22},

journal = {Journal of Materials Chemistry C},

abstract = {Surface-enhanced Raman spectroscopy (SERS) has emerged as a powerful technique for the ultra-sensitive detection of molecules and has been widely applied in many fields, ranging from biomedical diagnostics and environmental monitoring to trace-level detection of chemical and biological analytes. While traditional metallic SERS substrates rely predominantly on electromagnetic field enhancement, emerging semiconductor SERS materials have attracted growing interest because they offer the additional advantage of simultaneous chemical and electromagnetic enhancements. Here, we review some of the recent advancements in the design and optimization of semiconductor SERS substrates, with a focus on their dual enhancement mechanisms. We also discuss the transition from nanoparticle-based platforms to more advanced nanoresonator-based SERS metasurfaces, highlighting their superior sensing performance.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Oriented Naphthalene-O-propylammonium-Based (NOP)4AuBIIII8 (B = Au, Bi, Sb) Ruddlesden\textendashPopper Two-Dimensional Gold Double Perovskite Thin Films Featuring High Charge-Carrier Mobility},

author = {F Wolf and T Chau and D Han and K B Spooner and M Righetto and P D\"{o}rflinger and S Wang and R Guntermann and R Hooijer and D O Scanlon and H Ebert and V Dyakonov and L M Herz and T Bein},

url = {https://doi.org/10.1021/jacs.5c01102},

doi = {10.1021/jacs.5c01102},

issn = {0002-7863},

year  = {2025},

date = {2025-05-21},

journal = {Journal of the American Chemical Society},

volume = {147},

number = {20},

pages = {16992-17001},

abstract = {Two-dimensional perovskites show intriguing optoelectronic properties due to their anisotropic structure and multiple quantum well structure. Here, we report the first three gold-based Ruddlesden\textendashPopper type two-dimensional double perovskites with a general formula (NOP)4AuIBIIII8 (B = Au, Bi, Sb) employing naphthalene-O-propylammonium (NOP) as an organic cation. They were found to form highly crystalline thin films on various substrates, predominantly oriented in the [001] direction featuring continuous, crack-free film areas on the μm2 scale. The thin films show strong optical absorption in the visible region, with band gap energies between 1.48 and 2.32 eV. Density functional theory calculations support the experimentally obtained band gap energies and predict high charge-carrier mobilities and effective charge separation. A comprehensive study with time-resolved microwave conductivity (TRMC) and optical-pump-THz-probe (OPTP) spectroscopy revealed high charge-carrier mobilities for lead-free two-dimensional perovskites of 4.0 ± 0.2 cm2(V s)−1 and charge-carrier lifetimes in the range of μs. Photoconductivity measurements under 1 sun illumination demonstrated the material’s application as a photodetector, showing a 2-fold increase in conductivity when exposed to light.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Surface Charge Modulation in Covalent Organic Frameworks for Controlled Pt-Photodeposition and Enhanced Photocatalytic Hydrogen Evolution},

author = {K Paliusyte and L L Nascimento and H Illner and M Wiedmaier and R Guntermann and M D\"{o}blinger and T Bein and A O T Patrocinio and J Schneider},

doi = {10.1002/smll.202500870},

issn = {1613-6810 

1613-6829},

year  = {2025},

date = {2025-05-19},

journal = {SMALL},

abstract = {Covalent organic frameworks (COFs) represent a new class of organic photocatalysts for the hydrogen evolution reaction (HER). While the influence of COF structural and optoelectronic properties on HER is well-studied, the role of surface charge in optimizing interfacial interactions with reactants remains underexplored. In this study, it is demonstrated that converting imine to amide linkages in a thiophene-based COF allows for altering surface charge through different protonation behaviors of the linkages. Zeta potential measurements reveal that the amide-linked COF, due to its lower basicity, is deprotonated and negatively charged in the presence of ascorbic acid, while the imine-linked COF is protonated and positively charged. This electrostatic contrast drives the photoreduction of [PtCl6]2(-) to Pt, with the imine-linked COF yielding uniformly distributed small Pt particles (1-2 nm), whereas the amide-linked COF forms larger Pt particles (up to 100 nm). The amide-linked COF, acting as an antenna that facilitates interdomain electron transport along COF agglomerates, promotes both Pt growth and subsequent proton reduction demonstrating a 300% increase in photocatalytic HER rate compared to its imine form. This work introduces surface charge modulation as a novel tool for controlling photocatalytic processes in COF-based systems expanding the COF functionality in photocatalysis.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {AUGUR, A flexible and efficient optimization algorithm for identification of optimal adsorption sites},

author = {I Kouroudis and N Misciaci and F Mayr and L M\"{u}ller and Z Gu and A Gagliardi},

doi = {10.1038/s41524-025-01630-5},

year  = {2025},

date = {2025-05-17},

urldate = {2024-09-24},

journal = {NPJ COMPUTATIONAL MATERIALS},

volume = {11},

issue = {1},

abstract = {In this paper, we propose a novel flexible optimization pipeline for determining the optimal adsorption sites, named AUGUR (Aware of Uncertainty Graph Unit Regression). Our model combines graph neural networks and Gaussian processes to create a flexible, efficient, symmetry-aware, translation, and rotation-invariant predictor with inbuilt uncertainty quantification. This predictor is then used as a surrogate for a data-efficient Bayesian Optimization scheme to determine the optimal adsorption positions. This pipeline determines the optimal position of large and complicated clusters with far fewer iterations than current state-of-the-art approaches. Further, it does not rely on hand-crafted features and can be seamlessly employed on any molecule without any alterations. Additionally, the pooling properties of graphs allow for the processing of molecules of different sizes by the same model. This allows the energy prediction of computationally demanding systems by a model trained on comparatively smaller and less expensive ones.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Angular dispersion suppression in deeply subwavelength phonon polariton bound states in the continuum metasurfaces},

author = {L Nan and A Mancini and T Weber and G L Seah and E Cort\'{e}s and A Tittl and S A Maier},

doi = {10.1038/s41566-025-01670-9},

issn = {1749-4885 

1749-4893},

year  = {2025},

date = {2025-05-16},

journal = {NATURE PHOTONICS},

abstract = {Quasi-bound states in the continuum (qBICs) achieved through symmetry breaking in photonic metasurfaces are a powerful approach for engineering resonances with high quality factors and tunability. However, miniaturization of these devices is limited as the in-plane unit-cell size typically scales linearly with the resonant wavelength. By contrast, polariton resonators can be deeply subwavelength, offering a promising solution for achieving compact devices. Here we demonstrate that low-loss mid-infrared surface phonon polaritons enable metasurfaces supporting qBICs with unit-cell volumes up to 105 times smaller than the free-space volume lambda 03documentclass[12pt]minimal usepackageamsmath usepackagewasysym usepackageamsfonts usepackageamssymb usepackageamsbsy usepackagemathrsfs usepackageupgreek setlength\oddsidemargin-69pt begindocument$$\lambda_0\<^\>3$$enddocument. Using 100-nm-thick free-standing silicon carbide membranes, we achieve highly confined qBIC states with exceptional robustness against incident-angle variations, a feature unique among qBIC systems. This absence of angular dispersion enables mid-infrared vibrational sensing of thin, weakly absorbing molecular layers using a reflective objective, a method that typically degrades resonance quality in standard qBIC metasurfaces. We introduce surface-phonon-polariton-based qBICs as a platform for ultraconfined nanophotonic systems, advancing the miniaturization of mid-infrared sensors and devices for thermal radiation engineering.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

doi = {10.1021/acsami.5c03859},

issn = {1944-8244},

year  = {2025},

date = {2025-05-14},

journal = {ACS Applied Materials \& Interfaces},

volume = {17},

number = {19},

pages = {28459-28471},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Understanding the structure and mechanism of Na+ diffusion in NASICON solid-state electrolytes and the effect of Sc- and Al/Y-substitution},

author = {I Pivarn\'{i}kov\'{a} and S Seidlmayer and M Finsterbusch and G D\"{u}ck and N Jalarvo and P M\"{u}ller-Buschbaum and R Gilles},

url = {\<Go to ISI\>://WOS:001465925900001},

doi = {10.1039/d4sc04544k},

issn = {2050-7488},

year  = {2025},

date = {2025-05-13},

journal = {Journal of Materials Chemistry A},

volume = {13},

number = {19},

pages = {14353-14371},

abstract = {NASICON (sodium superionic conductor) based ceramics are one of the most promising classes of solid-state electrolytes for all-solid-state batteries. However, the mechanism of sodium ion diffusion is not understood in great detail since there is still a discrepancy between reported average structure models, local structures, and the number and position of sodium sites. To close this gap, we investigate the underlying diffusion mechanism and structural changes governing the Na+ transport in Na3.4Zr2Si2.4P0.6O12 using quasielastic neutron scattering (QENS) and powder X-ray diffraction (XRD). In the temperature range from 298 K to 640 K, the correlations between structural changes of a monoclinic C2/c to rhombohedral R3c phase transition and the result of ion diffusion are investigated. The analysis of the quasielastic neutron scattering data reveals two quasielastic components corresponding to the Chudley-Elliott jump-diffusion model. It clearly shows two different Na+ diffusion processes, local and long-range, on two different time and length scales and allows calculations of their corresponding activation energies. Additionally, the effects of Sc3+ and Al3+/Y3+ aliovalent substitution of Zr4+ ions on the crystal structure and Na+ diffusion are also studied. We can distinguish a local, chain, and cross-chain diffusion mechanism based on correlated QENS and XRD comparison of relevant nearest crystallographic Na-Na distances. The results reveal that the Na+ diffusion in these NASICONs is three-dimensional and can provide guidelines on how dopants and changes in the crystal structure can affect the Na+ conductivity.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Control and enhancement of optical nonlinearities in plasmonic semiconductor nanostructures},

author = {A Rossetti and H T Hu and T Venanzi and A Bousseksou and F De Luca and T Deckert and V Giliberti and M Pea and I Sagnes and G Beaudoin and P Biagioni and E Ba\`{u} and S A Maier and A Tittl and D Brida and R Colombelli and M Ortolani and C Cirac\`{i}},

url = {\<Go to ISI\>://WOS:001495020200001},

doi = {10.1038/s41377-025-01783-4},

issn = {2095-5545},

year  = {2025},

date = {2025-05-13},

journal = {Light-Science \& Applications},

volume = {14},

number = {1},

abstract = {The efficiency of nanoscale nonlinear elements in photonic integrated circuits is hindered by the physical limits to the nonlinear optical response of dielectrics, which cannot be engineered as it is a fundamental material property. Here, we experimentally demonstrate that ultrafast optical nonlinearities in doped semiconductors can be engineered and can easily exceed those of conventional undoped dielectrics. The electron response of heavily doped semiconductors acquires in fact a hydrodynamic character that introduces nonlocal effects as well as additional nonlinear sources. Our experimental findings are supported by a comprehensive computational analysis based on the hydrodynamic model. In particular, by studying third-harmonic generation from plasmonic nanoantenna arrays made out of heavily n-doped InGaAs with increasing levels of free-carrier density, we discriminate between hydrodynamic and dielectric nonlinearities. Most importantly, we demonstrate that the maximum nonlinear efficiency as well as its spectral location can be engineered by tuning the doping level. Crucially, the maximum efficiency can be increased by almost two orders of magnitude with respect to the classical dielectric nonlinearity. Having employed the common material platform InGaAs/InP that supports integrated waveguides, our findings pave the way for future exploitation of plasmonic nonlinearities in all-semiconductor photonic integrated circuits.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Fluorescence-Detected Pump\textendashProbe Spectroscopy for Artifact-Free Detection of Stokes Shift Dynamics},

author = {H Hao and P Mal\'{y} and Y Cui and M Binzer and E Thyrhaug and J Hauer},

url = {https://doi.org/10.1021/acs.jpclett.5c00646},

doi = {10.1021/acs.jpclett.5c00646},

year  = {2025},

date = {2025-05-09},

journal = {The Journal of Physical Chemistry Letters},

pages = {4861-4868},

abstract = {Fluorescence-detected pump\textendashprobe (F-PP) spectroscopy is a recently developed method to study excited-state dynamics. F-PP combines the temporal resolution of conventional transient absorption (TA) spectroscopy with the sensitivity of fluorescence detection. In this work, we demonstrate inherently phase-stable F-PP spectroscopy using 20 fs pulses to monitor the ultrafast Stokes shift dynamics of a solvated fluorophore (Y12). We observed a shift in the stimulated emission maximum with a time constant of 84 fs. In contrast to TA, F-PP provides a coherent artifact-free view of this process. Using quantitative signal background subtraction, as discussed in this work, F-PP uncovers the pure stimulated emission spectrum and its ultrafast dynamics. This signal isolation is a clear advantage over TA, where different contributions often overlap heavily. We compare results from F-PP and TA on an equal footing using the same excitation pulses, emphasizing the features and advantages of the F-PP technique.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {All-optical permittivity-asymmetric quasi-bound states in the continuum},

author = {R Bert\'{e} and T Possmayer and A Tittl and L D S Menezes and S A Maier},

url = {https://doi.org/10.1038/s41377-025-01843-9},

doi = {10.1038/s41377-025-01843-9},

issn = {2047-7538},

year  = {2025},

date = {2025-05-07},

journal = {Light: Science \& Applications},

volume = {14},

number = {1},

pages = {185},

abstract = {Resonances are usually associated with finite systems\textemdashthe vibrations of clamped strings in a guitar or the optical modes in a cavity defined by mirrors. In optics, resonances may be induced in infinite continuous media via periodic modulations of their optical properties. Here we demonstrate that periodic modulations of the permittivity of a featureless thin film can also act as a symmetry-breaking mechanism, allowing the excitation of photonic quasi-bound states in the continuum (qBICs). By interfering two ultrashort laser pulses in the unbounded film, transient resonances can be tailored through different parameters of the pump beams. We show that the system offers resonances tunable in wavelength and quality-factor, and spectrally selective enhancement of third-harmonic generation. Due to a fast decay of the permittivity asymmetry, we observe ultrafast dynamics, enabling time-selective near-field enhancement with picosecond precision. Optically induced permittivity asymmetries may be exploited in on-demand weak to ultrastrong light-matter interaction regimes and light manipulation at dynamically chosen wavelengths in lithography-free metasurfaces.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Sustainable High-Performance Aqueous Batteries Enabled by Optimizing Electrolyte Composition},

author = {R L Streng and S Reiser and A Senyshyn and S Wager and J Sterzinger and P Schneider and D Gryc and M Z Hussain and A S Bandarenka},

url = {https://doi.org/10.1002/advs.202417587},

doi = {https://doi.org/10.1002/advs.202417587},

issn = {2198-3844},

year  = {2025},

date = {2025-05-05},

journal = {Advanced Science},

volume = {n/a},

number = {n/a},

pages = {2417587},

abstract = {Lithium-free aqueous batteries (LFABs) offer a sustainable alternative to lithium-ion batteries for large-scale energy storage, addressing issues like material scarcity and flammability. However, their economic viability is limited by low energy density and cycle life due to the narrow electrochemical stability window of water and active material dissolution. High-concentration water-in-salt electrolytes typically used to tackle these issues are expensive and potentially hazardous. This work presents a novel, cost-efficient electrolyte design using safe salts at lower concentrations. The influence of different cation species on the copper hexacyanoferrate cathode and polyimide anode is systematically explored, optimizing the electrolyte for improved cell voltage and cycling stability. The resulting battery, with a 1.8 mol kg?1 MgCl2 + 1.8 mol kg?1 KCl aqueous electrolyte, achieves a competitive energy density of 48 Wh kg?? and 95% efficiency. It also shows 70% capacity retention even at extremely high (dis-)charge rates of 50 C and a maximum specific power of over 10000 W kg??, indicating its strong potential for supercapacitor applications. Utilizing exclusively inexpensive and safe salts, this work significantly advances the practical application of low-cost LFABs for large-scale energy storage.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Effects of Tail States in Cs2AgBiBr6 Double Perovskites on Solar Cell Performance: A Temperature-Dependent Study of Photovoltaic External Quantum Efficiency, Open-Circuit Voltage, and Luminescence},

author = {F Ebadi and K Meraji and M A Torre Cachafeiro and F Wolf and M T Sirtl and T Bein and W Tress},

url = {https://doi.org/10.1002/aenm.202500758},

doi = {https://doi.org/10.1002/aenm.202500758},

issn = {1614-6832},

year  = {2025},

date = {2025-05-03},

journal = {Advanced Energy Materials},

volume = {n/a},

number = {n/a},

pages = {2500758},

abstract = {Cs2AgBiBr6 double perovskites have been investigated as a lead-free alternatives to lead-based perovskites. However, despite promising features such as high luminescence lifetimes, solar-cell efficiencies and the open-circuit voltage still remain too low. Various spectroscopic studies suggested multiple reasons such as a fast relaxation into localized self-trapped excitonic and polaronic states. However, it remains unclear to what extent the suggested processes are the culprit for the low device performance. In this study, full devices are characterized as a function of temperature, focusing on highly sensitive measurements of tail states. In the spectral response, a strongly-temperature-dependent Urbach energy is identified, indicative of high dynamic disorder. The current generated from the excitonic absorption becomes only limiting at lower temperatures with an activation energy of 0.15 eV. Analysis of light-, temperature- and voltage-dependent photoluminescence (PL) indicates that charge extraction correlates with PL quenching and PL does not originate from geminate pairs. The bandgap deduced from temperature-dependent open-circuit voltage is found at 2.0 eV, coinciding with the PL peak. In contrast, tail-state excitation leads to lower open-circuit voltage and luminescence that cannot be quenched with voltage. Having identified the importance of tail-state features, the methodology might assist in optimizing materials and devices for enhanced efficiency.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Insights into Decoupled Solar Energy Conversion and Charge Storage in a 2D Covalent Organic Framework for Solar Battery Function},

author = {B B Rath and L Fuchs and F Stemmler and A Rodr\'{i}guez-Camargo and Y Wang and M F X Dorfner and J Olbrich and J Van Slageren and F Ortmann and B V Lotsch},

url = {https://doi.org/10.1021/jacs.4c17642},

doi = {10.1021/jacs.4c17642},

issn = {0002-7863},

year  = {2025},

date = {2025-04-28},

journal = {Journal of the American Chemical Society},

abstract = {Decoupling solar energy conversion and storage in a single material offers a great advantage for off-grid applications. Herein, we disclose a two-dimensional naphthalenediimide (NDI)-based covalent organic framework (COF) exhibiting remarkable solar battery performance when used as a photoanode. Light-induced radicals are stabilized within the framework for several hours, offering on-demand charge extraction for electrical energy production. Our study reveals mechanistic insights into the long-term charge stabilization using optical spectroscopy and (photo)electrochemical measurements, in conjunction with density functional theory (DFT) simulations. Among several solvents, water provides the best dielectric screening and energetically favorable proton exchange to stabilize photoinduced radicals for more than 48 h without the need for additional metal cations. This study provides fundamental insights into the optoionic charge storage mechanism in NDI-COF, while introducing a highly tunable, nanoporous material platform that surpasses related materials, such as carbon nitrides, metal\textendashorganic frameworks (MOFs), or metal oxides, in terms of charge storage capacity. This study opens new perspectives for the design of optoionic charge-storing materials and the direct storage of solar energy to overcome the intermittency of solar irradiation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {1433-7851},

year  = {2025},

date = {2025-04-17},

journal = {Angewandte Chemie International Edition},

volume = {64},

number = {17},

pages = {e202500768},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2196-0216},

year  = {2025},

date = {2025-04-14},

journal = {ChemElectroChem},

volume = {n/a},

number = {n/a},

pages = {2500073},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {1433-7851},

year  = {2025},

date = {2025-04-09},

journal = {Angewandte Chemie International Edition},

volume = {n/a},

number = {n/a},

pages = {e202506018},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

title = {Polarization-independent metasurfaces based on bound states in the continuum with high Q-factor and resonance modulation},

author = {X Y Yang and A Antonov and A Aigner and T Weber and Y H Lee and T Jiang and H Y Hu and A Tittl},

url = {\<Go to ISI\>://WOS:001503744200007},

doi = {10.1364/oe.547467},

issn = {1094-4087},

year  = {2025},

date = {2025-04-07},

journal = {Optics Express},

volume = {33},

number = {7},

pages = {15682-15689},

abstract = {Metasurfaces offer a powerful platform for effective light manipulation, which is crucial for advanced optical technologies. While designs of polarization-independent structures have reduced the need for polarized illumination, they are often limited by either low Q factors or low resonance modulation. Here, we design and experimentally demonstrate a metasurface with polarization-independent quasi-bound state in the continuum (quasi-BIC), where the unit cell consists of four silicon squares arranged in a two-dimensional array and the resonance properties can be controlled by adjusting the edge length difference between different squares. Our metasurface experimentally achieves a Q factor of approximately 100 and a resonance modulation of around 50%. This work addresses a common limitation in previous designs, which either achieved high Q factors exceeding 200 with a resonance modulation of less than 10%, leading to challenging signal-to-noise ratio requirements, or achieved strong resonance modulation with Q factors of only around 10, limiting light confinement and fine-tuning capabilities. In contrast, our metasurface ensures that the polarization-independent signal is sharp and distinct within the system, reducing the demands on signal-to-noise ratio and improving robustness. Experiments show the consistent performance across different polarization angles. This work contributes to the development of versatile optical devices, enhancing the potential for the practical application of BIC-based designs in areas such as optical filtering and sensing. (c) 2025 Optica Publishing Group under the terms of the Optica Open Access Publishing Agreement},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2058-7546},

year  = {2025},

date = {2025-04-07},

journal = {Nature Energy},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2195-1071},

year  = {2025},

date = {2025-04-07},

journal = {Advanced Optical Materials},

volume = {n/a},

number = {n/a},

pages = {2500166},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {0021-8995},

year  = {2025},

date = {2025-04-06},

journal = {Journal of Applied Polymer Science},

volume = {n/a},

number = {n/a},

pages = {e57089},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2041-1723},

year  = {2025},

date = {2025-04-04},

journal = {Nature Communications},

volume = {16},

number = {1},

pages = {3216},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {1932-7447},

year  = {2025},

date = {2025-04-03},

journal = {The Journal of Physical Chemistry C},

volume = {129},

number = {13},

pages = {6511-6523},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2041-1723},

year  = {2025},

date = {2025-03-27},

journal = {Nature Communications},

volume = {16},

number = {1},

pages = {2985},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

doi = {10.1021/acsami.4c22330},

issn = {1944-8244},

year  = {2025},

date = {2025-03-26},

journal = {ACS Applied Materials \& Interfaces},

volume = {17},

number = {12},

pages = {18339-18350},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {0743-7463},

year  = {2025},

date = {2025-03-24},

journal = {Langmuir},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

year  = {2025},

date = {2025-03-21},

journal = {Small Science},

volume = {n/a},

number = {n/a},

pages = {2400585},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {1755-4349},

year  = {2025},

date = {2025-03-20},

journal = {Nature Chemistry},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

doi = {10.34133/energymatadv.0181},

year  = {2025},

date = {2025-03-19},

journal = {Energy Material Advances},

volume = {0},

number = {ja},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

doi = {10.1021/jacsau.5c00097},

year  = {2025},

date = {2025-03-19},

journal = {JACS Au},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {1433-7851},

year  = {2025},

date = {2025-03-15},

journal = {Angewandte Chemie International Edition},

volume = {n/a},

number = {n/a},

pages = {e202500524},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2542-4351},

year  = {2025},

date = {2025-03-14},

journal = {Joule},

pages = {101871},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {1932-7447},

year  = {2025},

date = {2025-03-13},

journal = {The Journal of Physical Chemistry C},

volume = {129},

number = {10},

pages = {5116-5121},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {1549-9618},

year  = {2025},

date = {2025-03-11},

journal = {Journal of Chemical Theory and Computation},

volume = {21},

number = {5},

pages = {2371-2385},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {0935-9648},

year  = {2025},

date = {2025-03-07},

journal = {Advanced Materials},

volume = {n/a},

number = {n/a},

pages = {2418425},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {1613-6810},

year  = {2025},

date = {2025-03-03},

journal = {Small},

volume = {n/a},

number = {n/a},

pages = {2500550},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {1614-6832},

year  = {2025},

date = {2025-03-01},

journal = {Advanced Energy Materials},

volume = {15},

number = {11},

pages = {2404961},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2520-1131},

year  = {2025},

date = {2025-03-01},

journal = {Nature Electronics},

volume = {8},

number = {3},

pages = {254-266},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2520-1158},

year  = {2025},

date = {2025-03-01},

journal = {Nature Catalysis},

volume = {8},

number = {3},

pages = {229-238},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2198-3844},

year  = {2025},

date = {2025-03-01},

journal = {Advanced Science},

volume = {12},

number = {9},

pages = {2413203},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

doi = {10.1002/advs.202414714},

issn = {2198-3844},

year  = {2025},

date = {2025-03-01},

journal = {Adv Sci (Weinh)},

volume = {12},

number = {12},

pages = {e2414714},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{nokey,

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

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

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

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

issn = {2468-6069},

year  = {2025},

date = {2025-03-01},

journal = {Materials Today Energy},

volume = {48},

pages = {101813},

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

keywords = {},

pubstate = {published},

tppubtype = {article}

}