Perovskite solar modules, particularly those using ultrathin self-assembled monolayer (SAM)-based hole transport layers, suffer from reverse-bias instability. Here we identified that discontinuous SAM distribution causes shunting and a lower breakdown voltage, while indium tin oxide-triggered electrochemical deprotonation of formamidinium ions leads to reduced long-term stability under reverse-bias conditions. To address these issues, we developed a molecular-templated pre-assembly strategy driven by hydrogen-bonding interactions between the SAM and a polycarbazole template. This approach ensures homogeneous clusters in solution and strong substrate interactions, yielding dense and uniform layers. Subsequently, we prepared minimodules with 24.0% efficiency (certified steady-state efficiency of 23.2%) and improved reverse-bias stability. Small-area devices retained 95% efficiency after 300 h at -4.8 V, while minimodules exhibited a T-98 lifetime of 312 h under negative open-circuit voltage stress. We showed that a single bypass diode can protect at least 16 subcells, setting a new reliability benchmark for scalable perovskite photovoltaics.

Metal-metal-to-ligand charge-transfer (MMLCT) complexes are emerging as next-generation emitters that combine molecular precision with metallic coherence, achieving fast exciton decay and high photoluminescence quantum yields. Despite their promise, the lack of mechanistic insight linking molecular structure to exciton dynamics has hindered rational design. Here, we establish the microscopic origin of MMLCT emission in Pt(II) systems by integrating quantum-chemical modelling, ultrafast spectroscopy, and synchrotron-based x-ray probes to deliver an end-to-end mechanistic picture of MMLCT-state formation and decay. Direct measurements on Pt(fppz)2 and its alkylated analogue Pt(8ppz)2 quantify Pt-Pt spacings, revealing that few-ångström variations govern the emergence and coherence of the MMLCT state. Coherently stacked Pt(fppz)2 aggregates (Pt-Pt ≈3.3 Å) exhibit sub-microsecond exciton decay with nearly complete exciton utilization, whereas Pt(8ppz)2 (Pt-Pt >5 Å) yields long-lived ligand-centred emission. These contrasting exciton dynamics translate directly into different device performance, with Pt(fppz)2-based organic light-emitting diodes (OLEDs) achieving ∼29% external quantum efficiency and negligible roll-off, enabling applications in visible-light communication, bioimaging, and transparent displays. Our findings establish a generalizable structure-property relationship for MMLCT emitters, extending beyond Pt(II) to aggregated d8-d8 and coinage-metal systems, unlocking new opportunities across optoelectronic and photonic technologies.

The integration of high-quality SrTiO 3 thin films on silicon substrates is crucial for various applications.

Hybrid two-step deposition offers a scalable route for fabricating metal halide perovskites in tandem architectures, particularly for achieving excellent conformality on textured substrates. However, using this approach for ultrawide-bandgap perovskites (>1.85 eV) remains a fundamental challenge, due to issues of incomplete conversion and inhomogeneous crystallization. Here we reveal that the bromine/iodine (Br/I) ratio critically governs the crystallinity of the evaporated inorganic framework (IOF), which plays a key role in the halide distribution and phase quality of the perovskite film during the following hybrid conversion process. In situ grazing incidence wide-angle X-ray scattering indicates that high Br content induces a low-crystallinity IOF and enables uniform and complete incorporation of organic cations. As a result, the high Br IOF enhances photoluminescence quantum yield in the final perovskite film from 0.28% to 1.14% and enables more homogeneous halide distribution. The resulting 1.88-eV perovskite achieves a power conversion efficiency of 17.13% in single-junction devices. When further integrated as the top subcell in monolithic perovskite/perovskite/silicon triple-junction solar cells, the triple-junction device delivers a maximum efficiency of 28.71% over an active area of 1 cm2 (certified 27.53%). We expect our findings to pave the way for the fabrication of ultrawide-bandgap perovskites and to contribute to continued improvements in triple-junction solar cells.

High-throughput screening has revolutionized material design, enabling the accelerated development and optimization of materials through data-driven approaches. This study employs drop-on-demand inkjet printing to fabricate combinatorial superconducting (REBCO, ) thin films with a controlled compositional gradient, allowing a systematic investigation of Rare Earth composition effects on the Transient Liquid Assisted Growth (TLAG) process. A methodological framework is established for fabricating and characterizing combinatorial REBCO thin films. Automated and synchrotron-based techniques-including Interferometry, EDX, XRD, and Scanning Hall Probe Microscopy (SHPM)-are used to build comprehensive property maps, revealing composition-driven variations in crystal growth and superconducting properties. Furthermore, SEM and STEM confirm REBCO crystal quality and provide deeper material insights at specific combinatorial sample locations. This framework also lays the groundwork for integrating machine learning approaches into the understanding of the TLAG process and predicting the final quality of REBCO superconductive thin films. By bridging combinatorial synthesis, advanced characterization, and data-driven analysis, this study establishes a workflow that can be leveraged in the future to facilitate the scaling-up of TLAG technology for industrial applications.

Understanding and mitigating nanoparticle (NP) sintering is critical for enhancing the durability of metal nanocatalysts in industrial chemical processes, such as propane dehydrogenation (PDH). Herein, we explore in situ grazing-incidence small-angle X-ray scattering (GISAXS) as an innovative, high-throughput tool to monitor the morphological evolution of model Pt-based catalysts in real-time during PDH reaction and O-2 regeneration cycling at 600 degrees C - significantly expanding the capabilities of existing characterization methods. In situ GISAXS reveals that Pt NP sintering predominantly occurs within the first two PDH-O-2 cycles, where the NP shape remains near-spherical while its size increases. To suppress sintering, atomic layer deposition (ALD) is explored as nanofabrication method to atomically tailor Pt NPs via two strategies: (i) sub-monolayer MgO overcoating and (ii) Sn alloying. MgO decoration (similar to 30 % surface coverage) significantly delays sintering by physically hindering Pt migration, while maintaining the active site accessibility. Sn-alloyed Pt3Sn NPs dynamically restructure into SnO2/Pt shell-core configurations under oxidative conditions, the SnO2-shell functioning as reversible encapsulation that inhibits sintering. Both strategies provide NP stabilization, albeit through a different mechanism and with a final morphology of either isolated MgO-coated Pt NPs or worm-type Pt-Sn NPs after extended cycling. This work highlights the synergy between in situ GISAXS and ALD nanofabrication as an effective platform for rational catalyst design, propelling the development of sintering-resistant nanocatalysts for future sustainable catalytic processes.

X-ray diffraction pole-figure measurements are essential to analyze crystallographic texture in thin films and nanoparticles. Conventionally, large and equal incident and exit angles beyond the critical angle of the studied material are used, limiting surface sensitivity. This study demonstrates the use of grazing-incidence wide-angle X-ray scattering (GIWAXS) while rotating the sample azimuthally in its own plane to acquire pole figures that are more sensitive to the near-surface region compared with pole figures measured in standard Schulz geometry. Comparative measurements on supported Pt nanoparticles in GIWAXS and Schulz geometry at two different synchrotron beamlines confirm the improved sensitivity of the GIWAXS pole figures. By tuning the incident angle, the substrate diffraction background can be reduced and the information depth inside a Pt thin film can be selected. In addition, the near-horizontal sample orientation during GIWAXS - only tilted by the small incident angle - reduces constraints on sample environments compared with conventional Schulz geometry. The increased sensitivity to the near-surface region of a grazing-incidence X-ray beam, combined with the simpler measurement geometry, prove grazing-incidence pole figures to be powerful for future in situ and ex situ texture analysis on thin films and supported nanoparticles.

Perovskite-silicon triple-junction photovoltaics offer efficiency gains beyond dual-junction devices but at the expense of added complexity1. Here we address two key bottlenecks in perovskite-silicon-based triple-junction solar cells: reduced open-circuit voltage (VOC) in the wide-bandgap (WBG) top cell and limited photocurrent generation in the middle cell1,2. A non-volatile additive, 4-hydroxybenzylamine (HBA), regulates WBG perovskite crystallization and passivates defects, promoting oriented growth and suppressing non-radiative recombination. Together with improved energy-level alignment, this yields VOCs of up to 1.405 V and enhanced stability. To overcome the current limitations in the middle cell, a three-step deposition strategy enables the formation of thick, low-bandgap perovskite absorbers while preserving microstructural integrity and enhancing electron extraction. Also, low-refractive-index SiOx-nanoparticles (SiOx-np) that accumulate in the front valleys of the textured silicon bottom cell act as an optical middle reflector, enhancing light absorption in the middle cell. These advances are then combined in 1-cm2 perovskite-perovskite-silicon devices, achieving a certified efficiency of 30.02%.

Lithium iron phosphate (LiFePO4, LFP) is one of the main cathode materials for lithium-ion batteries on the market; however, its implementation in all-solid-state thin-film batteries remains challenged by transport and interfacial limitations, as well as by compatibility and reactivity issues arising from thin film fabrication processes. In this work, carbon-free LiFePO4 thin films with thicknesses between 120 and 300 nm were deposited by pulsed laser deposition and investigated as cathodes in LFP/ lithium-phosphorus oxynitride (LiPON)/Li all-solid-state thin-film batteries. Structural and morphological analyses confirm the growth of phase-pure, crystalline LiFePO4 films without post deposition annealing. Electrochemical measurements reveal reversible lithium insertion and extraction, yet the theoretical capacity of LiFePO4 is not fully accessed under most operating conditions. When cycled at elevated temperature (50 degrees C), the full cells show a clear enhancement in capacity utilization, with the 200 nm-thick cathode delivering an areal capacity of 7.2 & micro;A & centerdot;h & centerdot;cm(-2) (100 mA & centerdot;h & centerdot;g(-1)) at 5 & micro;A & centerdot;h & centerdot;cm(-2). The limited utilization of the active material may originate, in part, from interfacial phenomena at the LFP/Pt current-collector interface. From an application perspective, the achieved areal capacities and current densities fall within the operational range required for low-power autonomous microsystems, highlighting the potential relevance of LFP/LiPON thin-film batteries for internet-of-things applications.

Perovskite/silicon (Pero/Si) tandem solar cells are rapidly advancing toward high-efficiency photovoltaic deployment; yet, their long-term stability remains a critical bottleneck. Here, we systematically investigated interface degradation in monolithic Pero/Si tandem architectures based on two leading configurations: perovskite/tunnelling oxide passivated contact solar cells (Pero/TOPCon) and perovskite/heterojunction solar cells (Pero/HJT). Illumination and damp heat tests (following the ISOS-L-3 and ISOS-D-3 protocols) indicated that both tandem devices suffered from a pronounced interfacial instability. By revealing the buried interface properties with a multimodal interface characterization toolkit, we identified two degradation pathways: (i) perovskite decomposition at the buried interface driven by ion migration and deprotonation, and (ii) interfacial degradation of the silicon substrate exacerbated by ion invasion and hydrogen effusion. It is highlighted that the amorphous nature of the interconnection layers facilitated ion/hydrogen permeation and defect formation. Our work elucidated the additional interface degradation path of Pero/Si tandem, thus highlighting the importance of interconnection contact quality for developing durable Pero/Si tandem photovoltaics.

Perovskite quantum dots (PQDs) combine solution processability with excellent optoelectronic properties for next-generation photovoltaics. However, ligand depletion across synthesis, purification, film formation, and storage accumulates surface defects that drive aggregation and Ostwald ripening of the PQDs. Meanwhile, long-chain oleic acid (OA)/oleylamine (OAm) ligands act as insulating barriers within PQD solids, inhibiting charge carrier transport and solar cell performance. Here, we introduce a ligand-assisted ripening control (LARC) strategy that fortifies aromatic-molecule binding on formamidinium lead triiodide (FAPbI3) QDs to strengthen surface coordination and suppress ripening. Post-synthesis dosing with thiopheneacetic acid (TEAA) tunes the native OA/OAm acid-base equilibrium, facilitating proton exchange that drives controlled ligand desorption. The enhanced surface coordination suppresses ion detachment and breaks the dissolution-reprecipitation loop, thereby improving inter-QD electronic coupling. These synergistic effects yield FAPbI3 QD-based solar cells with power conversion efficiencies up to 18.88% and enhanced stability under both humidity storage and standard one-sun operational conditions.

Abstract Halide and organic linker-free, all-inorganic cubic (ABO3) and Ruddlesden–Popper perovskites (RPPs) with the general formula An+1BnO3n+1 are less explored in the field of alcohol fuel cells. Subsequently, the impact of variation in the synthesis approach leading to phase transformation with the change of nanoarchitecture is also not known, especially for compositional high-entropy-based Ruddlesden–Popper perovskites (HERPPs). At the same time, the literature is very silent with regard to the application of 2D and 3D phases of such perovskites for the methanol oxidation reaction (MOR) in an alkaline medium and the oxygen evolution reaction (OER). The present manuscript thus brings into light the influence of the transformation of RP perovskites from 2D layered to 3D cubic perovskite (ABO3) phases, along with the change of compositional entropy and how structural dimensionality governs the balance between active site density and intrinsic activity of the perovskites in electrocatalytic oxidation of methanol. The structural information on these synthesized materials was analyzed through synchrotron XRD, and other parameters were evaluated through various other analytical tools. During the MOR study, at a scan rate of 100 mV s–1, the 2D RPPs exhibited an onset potential of 1.59 V vs RHE with a maximum current density of 79.06 mA cm–2 and an overpotential of 310 mV. In contrast, at the same scan rate, the 3D cubic perovskite phase displayed a maximum current density of 168.79 mA cm–2 at a lower onset potential of 1.32 V vs RHE and an overpotential of 110 mV. OER showed a similar trend with improved kinetics. The Tafel slope also showed a decrease in value from 197 to 22 mV dec–1 in MOR and from 361 to 217 mV dec–1 in OER. The compositional high-entropy-based 3D cubic perovskite (ABO3) phase having minor impurity of the “n” = 4 RP phase with a diamond-like morphology showed the highest MOR and OER activity compared to medium-entropy-based RPPs with “n” = 1, 2 and “n” = 1, 3. The MOR activity of the materials was found to be the same until 18 h under alkaline conditions. Further, from the theoretical analysis, it was evident that the compositional high-entropy-based perovskites showed metallic and semimetallic nature on phase transformation.

Efficient wide-bandgap perovskite solar cells have pushed tandem efficiencies to 34.9%, reinforcing their promise for next-generation photovoltaics. However, their commercial adoption is hindered by stability issues of wide-bandgap perovskites, especially under high-temperature maximum power point tracking conditions. Here we report the stabilization of ~1.7-eV wide-bandgap perovskites via intermediate phase evolution, enabling a self-guided crystal-growth mode. A CsI2Br intermediate phase forms during early stage deposition, directing the oriented growth of polycrystalline films with unique texturing. Atomic-scale scanning transmission electron microscopy reveals that the CsI2Br ( 1 2 ¯ 3 ) facet, with a 2.9-Å interplanar spacing, matches the perovskite (200) facet, guiding coherent {100} growth. This results in enhanced crystallinity, with a 2-order-magnitude increase in the (100) diffraction intensity and a reduced full-width at half-maximum from 0.249° to 0.148°, compared with solution-processed films. The resulting solar cells exhibit outstanding thermal and operational stability, maintaining performance under maximum power point tracking for over 3,000 h at room temperature and over 500 h at 110 °C, with a projected lifetime of ~70,000 h. With 21.37% power conversion efficiency and >84% fill factor, this work presents a compelling route towards stable, high-efficiency tandem photovoltaics.

The performance of organic electronic devices, such as solar cells, depends on understanding and controlling the solid‐state microstructure of semiconducting polymers. In this study, a detailed understanding of the aggregate states, solid‐state microstructure, and thermotropic behavior of the best‐performing family of polymers for solar cells, i.e., benzodithiophene‐based semiconducting polymers, is provided. Using D18, PBnDT‐FTAZ, and PBDB‐T‐Cl as model systems, this study reveals a unique solid mesophase, distinct from previously observed polymer mesophases, comprising stacked solid‐like and liquid‐like layers. This mesophase resembles sanidic structures while also sharing features with columnar mesophases like condis crystals and paracrystals. At a larger length scale, it organizes into nanoscale fibril‐like domains, with polymer backbones aligned along the fibril axis, coexisting with amorphous‐like glassy regions, reported here for the first time. Notably, high‐performance polymers such as D18, D18‐Cl, and PM6 contain minimal glassy regions. The thermotropic behavior of this biphasic nanomorphology is also examined, providing insights into how thermal annealing influences polymer structure. Understanding these solid‐aggregate states, the microstructure, and the thermal behavior enables a more precise framework for defining structure–function relationships in semiconducting polymers. This will have a significant impact on the entire field of organic electronics, from organic photovoltaics to bioelectronics to wearable electronics.

Black-phase cesium lead iodide (CsPbI3) is a promising candidate for high-efficiency perovskite optoelectronics, but its instability under ambient conditions remains a major challenge. Among several strategies, dimethylammonium iodide (DMAI) has emerged as a potential stabilizer; however, inconsistencies in phase stability (3-7 days) and lower solar power conversion efficiencies (∼20 vs ∼27% for hybrid perovskites) highlight the need for further improvements. This study not only demonstrates enhanced stabilization of the high-symmetry black phase of CsPbI3 and improved film morphology through optimized composition and annealing conditions but also more importantly provides detailed mechanistic insights obtained from comprehensive experimental and theoretical analyses. Systematic tuning of the DMAI concentration (1.2 M), annealing temperature (200 °C, 1 min), and Cs+ substitution (12-15%) significantly extends phase stability to 7 days under ambient conditions (35-52% relative humidity) and maintains stability even after 16 months in a drybox environment by reducing orthorhombic strain and octahedral tilting. Additionally, a minor (∼5%) zero-dimensional (0D) Cs4PbI6 phase fills pinholes, enhancing the film quality. Optimized photodiodes exhibit a low dark current (∼1 μA/cm2), high external quantum efficiency (∼80% at -2 V), and a ≥100 dB linear dynamic range. These findings provide mechanistic insights into the stabilization of the black phase of CsPbI3, advancing the development of more stable and efficient perovskite-based optoelectronic devices.

Vacuum-assisted hybrid deposition for wide-bandgap (WBG) perovskites has been widely recognized for its advantages, including convenience for scaling up and conformal growth, while avoiding toxic solvents. However, the growth of WBG perovskites (>1.8 eV), which is critical for advancing the performance of thin-film-based tandem solar cells, remains insufficiently controlled under hybrid deposition. In this work, we introduce n-propylamine hydrochloride (PACl), which shows enhanced face-on stacking of (100) plane, effectively regulating the oriented crystal growth of 1.84 eV WBG perovskites during the annealing process. This approach reduces defect density and, consequently, improves carrier diffusion length. As a result, the hybrid-deposited WBG perovskite (>1.8 eV) solar cells realize a maximum efficiency of 17.48% and an open-circuit voltage (Voc) exceeding 1.315 V. When integrated with organic sub-cell in a two-terminal tandem configuration, the tandem device demonstrates a record efficiency of 26.46%, with a certified efficiency of 25.82% over an active area of 0.05 cm2.

The mechanical deformation of regenerated silk fibroin (RSF) films induces notable changes in their fluorescence properties, yet the underlying molecular mechanisms remain poorly understood. In this work, we investigate the interplay between mechanical, structural, and optical response of RSF films processed with glycerol (gly) and with polyethylene glycol (PEG) as a plasticizer. PEG-containing films exhibited enhanced ductility, a significant increase of the absorption coefficient in the UV spectral range and narrower fluorescence spectra, with reduced intensity at longer wavelengths, suggesting fewer cross-links. These differences in the mechanical and optical properties of the investigated polymers may be due to the higher amorphous phase content of the samples with PEG, as it is revealed by wide-angle X-ray scattering (WAXS). Ab initio calculations of model systems confirmed that fluorescence, primarily due to tryptophan residues, is highly sensitive to local conformation and hydrogen-bonding interactions. To elucidate the effect of deformation on silk fibroin fluorescence, WAXS patterns, using synchrotron radiation, and fluorescence spectra were acquired while simultaneous tensile measurements were performed. Notably, strain-induced backbone alignment favors the formation of electronically coupled cross-links, which give rise to the observed changes in fluorescence. These findings provide further insights into the structure-property relationships governing RSF fluorescence, with potential implications for the design of deformation-responsive biomaterials.

We report on an examination of mobile ion concentration ( N 0 ) in perovskite solar cells (PSCs) as a function of temperature and device architecture.

The natural self-assembly tendency of proteins to build complex structural architectures has kindled inspiration in developing supramolecular structures through the rational design of biomacromolecules. While there has been significant progress in achieving precise control over the morphology of self-assembled structures, combining different molecules within assemblies enables the design of materials with increased complexity, sophisticated structures, and a broad spectrum of functionalities. Here, the development of 1D and 2D peptide-protein coassembled systems based on the design of amphiphilic peptides and engineered proteins is described. The peptide was optimized to form stable self-assembled fibers by evaluating, computationally and experimentally, the assembling tendencies and the supramolecular features of peptides with different lengths and negative charges. A superhelical repeat protein was engineered by fusing one or two amphiphilic peptides into one or both termini. This modification drove the coassembly between the self-assembled fibers and the protein with one or two peptides, resulting in 1D or 2D coassembled systems. The protein films and the 2D coassembled system exhibited high ionic conductivity for a biomolecular system, attributed to their high content of charged residues, positioning these materials as promising candidates for developing bioelectronic devices. Thus, this work provides a versatile framework for developing coassembled materials with tunable dimensionality by using biocompatible building blocks without any additional chemical moieties, highlighting the potential for their use in biocompatible electronics.