Antimony sulfide (Sb_2S_3) is a semiconductor composed of quasi-one-dimensional ribbon-like structural units, which give rise to pronounced structural anisotropy in the bulk crystal. Despite growing interest in Sb_2S_3, in particular Sb_2S_3 thin films, a detailed understanding of its symmetry-based lattice dynamics remains incomplete. Here, we present a combined experimental and theoretical study of polarization-dependent Raman scattering in Sb_2S_3 thin films. We derive the Raman selection rules from the crystal symmetry and calculate the zone-center phonon modes and corresponding Raman tensors using density functional theory. The calculated polarization dependencies are systematically compared with polarization-dependent Raman measurements performed on oriented crystalline domains of Sb_2S_3 thin films. This combined analysis enables reliable mode assignments, elucidates the anisotropic Raman response associated with the ribbon-like crystal structure, and demonstrates the sensitivity of polarized Raman spectroscopy to crystal orientation and structural order in antimony chalcogenide (Sb_2S_3, Sb_2Se_3) as well as isostructural Bi_2S_3 thin films.

Magnetic nanoparticles (NPs) are widely studied as heat mediators in induction heating in fields like hyperthermia, drug delivery, debonding-on-demand, and industrial processing, where precise thermal control is essential. By adjusting NP size, morphology, and composition, magnetic characteristics including the Curie temperature are engineered to define heating thresholds and prevent overheating. However, achieving customizable induction heating behavior, particularly below 100°C, remains challenging. Herein, a scalable synthesis of nontoxic zinc (Zn) ferrite NPs (ZnxFe3- xO4) with freely tailorable induction heating temperatures between room temperature and 250°C is presented. The heating performance is governed by two key parameters: Zn doping level and postsynthesis annealing temperature, with remarkably high Zn contents up to X = 0.75. Higher annealing temperatures and lower Zn contents yield higher maximum heating temperatures. These trends are observed both in dried NPs and dispersions, with the latter combining exceptional colloidal stability and effective heating performance. Furthermore, the heating temperature can be adjusted externally by varying the amplitude of the applied alternating magnetic field, providing further thermal control. This study establishes a versatile strategy for designing zinc ferrite NPs with precisely adjustable induction heating across a broad temperature range, enabling applications from high-temperature industrial processes to low-temperature biomedical use.

Lines of indium(III) sulfides are deposited by atomic-layer additive manufacturing (ALAM) based on the reaction of indium tris(acetylacetonate) with hydrogen sulfide established in atomic layer deposition (ALD). At 160 °C, solid accretion occurs at a rate of 0.04 Å per pass. The layers are continuous, free of observable pinholes, dense, and very smooth, with a root-mean-squares roughness on the order of 0.5 nm found for deposits up to 25 nm thick. The material is nearly stoichiometric, with a S/. In ratio of 1.6 found experimentally by energy-dispersive X-ray microanalysis in cross-section examination by transmission electron microscopy, and it is polycrystalline. This work delivers In2S3 as a dopant or interfacial layer in opto-electronic devices to be prototyped and optimized by ALAM.

Optimizing the performance of organic solar cells hinges on a comprehensive understanding of their nanostructures, yet traditional characterization methods often fall short, delivering incomplete structural snapshots. We introduce elastically filtered 3D electron diffraction as technique to bridge full reciprocal- and real-space structural analysis within a single transmission electron microscope. Using model bulk heterojunction DRCN5T:PC71BM, 3D electron diffraction reproduces key structural parameters obtained from grazing-incidence wide-angle X-ray scattering, including lattice spacings, coherence lengths, and mosaicity, while also providing true in-plane access and direct registration with high-resolution imaging, diffraction imaging and nano-spectroscopy on the same sample. Application to another archetypal blend, P3HT:PC71BM, demonstrates the generality of the method. Our findings underscore the transformative potential of 3D electron diffraction, particularly in analyzing beam-sensitive organic thin films. The method enables correlative structural characterization of organic solar cells and opens pathways for application to a wide range of other nanostructured materials.

The performance, safety and lifetime of lithium-ion batteries (LIBs) are critically influenced by the evolution of electrode-electrolyte interphases (EEIs), namely the solid electrolyte interphase (SEI) on the anode and the cathode electrolyte interphase (CEI) on the cathode. While numerous studies have investigated SEI and CEI formation in coin cells with defined electrolyte composition, research on aged commercial battery cells remains limited. Commercial LIBs used in heavy goods vehicles (HGVs) contain complex electrolyte compositions with well-chosen additives to affect the formation of the EEIs during the formation cycle and aging. Their analysis therefore requires specialized workflows to preserve interfacial integrity during specimen preparation and nanoscale characterization. The presentation offers a comprehensive experimental approach for the disassembly, preparation and atomic-scale analysis of artificially aged commercial pouch cells using cryogenic focused ion beam (cryo-FIB), transmission electron microscopy (TEM) and atom probe tomography (APT). Furthermore, the results of a parameter study and EEI composition for aged battery cells are presented. Commercial NMC-graphite pouch cells from MAN Bus & Truck SE were fully discharged and disassembled under argon atmosphere in a glovebox (O 2 < 1 ppm, H 2 O < 1 ppm), since the SEI, CEI and lithium plating reacts with N 2 , O 2 and H 2 O thereby changing its composition and structure. Electrode sheets were extracted, cleaned in dimethyl carbonate (DMC), cut into cross sections and ion milled for further FIB preparation. Samples were transferred using a fully closed vacuum-argon chain to prevent exposure to air. A custom cryo-shuttle enabled transfer between the glovebox and FIB. The transfer between the devices was conducted on an open-source setup built by the authors. For APT specimen preparation in situ chromium deposition on the region of interest (ROI) was performed, followed by an additional platinum deposition. After tip sharpening, an additional chromium coating was applied. SEI tips were sharpened under cryogenic conditions to reduce bending of the graphite particles containing numerous cracks, while CEI tips were prepared at room temperature. TEM lamellas were prepared at both room and cryogenic temperatures and transferred via different routes – ambient atmosphere, vacuum and argon to compare stability and beam sensitivity. TEM analysis including bright-field (BF), high-angle annular dark-field (HAADF) and energy-dispersive X-ray spectroscopy (EDS) mapping under both room-temperature and cryogenic conditions for differently aged battery cells. In this presentation, the specimen preparation workflow as well as results of the SEI and CEI layer composition in differently aged commercial pouch cells are presented using APT and TEM revealing a deeper insight into the aging mechanism behind the layer formation.

This study explores whether the diffusion of Re in the gamma-phase of Ni-base superalloy single crystals is accelerated along fine dislocation networks that have formed at gamma/gamma'-interfaces during high-temperature and low-stress creep. Diffusion couples of Re-enriched superalloy thin films were sputter deposited onto (100) planes of two Re-free single-crystalline nickel-base superalloys with different microstructures. One consisted of an as-processed microstructure with cuboidal gamma'-particles separated by thin gamma-channels, with a low dislocation density. The other featured continuous gamma'-rafts parallel to the [100] direction with fine dislocation networks at the gamma/gamma'-interfaces. The rafted structure was produced by 2 % creep deformation along the [001] direction at 1000 degrees C and 240 MPa. Analytical transmission electron microscopy and atom probe tomography revealed that the diffusion of Re into the gamma-phase was not accelerated by the presence of dislocation networks at the gamma/gamma'-interfaces of the rafted microstructure.

Linear phase-contrast scanning transmission electron microscopy (STEM) techniques compatible with high-throughput 4D-STEM acquisition are widely used to enhance phase contrast in weakly scattering and beam-sensitive materials. In these modalities, contrast transfer is often suppressed at low spatial frequencies, resulting in a characteristic contrast gap that limits contrast. Approaches that retain low-frequency phase contrast exist but typically require substantially increased experimental complexity, restricting routine use. Dark-field STEM imaging captures this missing low-frequency information through electrons scattered outside the bright-field disk, but discards a large fraction of the scattered signal and is therefore dose-inefficient. Fused Full-field STEM (FF-STEM) is introduced as a 4D-STEM imaging modality that overcomes these limitations by combining ptychographic phase reconstruction with tilt-corrected dark-field imaging within a single acquisition. Bright-field data are used to estimate probe aberrations and reconstruct a high-resolution phase image, while dark-field data provide complementary low-frequency contrast. The two channels are fused in Fourier space using Wiener-band weighting based on the spectral signal-to-noise ratio, yielding transfer-gap-free images with high contrast. FF-STEM preserves the upsampling and depth-sectioning capabilities of ptychography, adds robust low-frequency contrast characteristic of dark-field imaging, and enables dose-efficient, near-real-time reconstruction.

Probing the mechanical behavior of liquids at the nanoscale-especially under hydrostatic stress with various strain rates and extreme temperature conditions-holds significant potential for advancing microfluidic, biomedical, and energy systems. However, it remains experimentally challenging due to the inherent difficulties in encapsulation of liquid at micro/nanoscale and in accurately applying and measuring stress within confined microscale environments. In this work, we present a novel single-step method for liquid encapsulation at the microscale and subsequent in situ micromechanical testing at extreme dynamic thermomechanical conditions. Localized electrodeposition in the liquid process enables the direct formation of hollow copper microarchitectures containing picoliters of liquid. The presence of the encapsulated liquid was verified via structural analysis at cryogenic and elevated temperatures. We investigated the mechanical role of the confined liquid through compressive tests, demonstrating its incompressibility at room temperature and its enhanced load-bearing capacity in the ice phase at -160°C. These results reveal enhanced energy dissipation due to the size-dependent strength of ice. Additionally, we evaluated the tensile response of copper-ice composites at -160°C using microfabricated push-to-pull structures. Our findings outline a new pathway for encapsulation of liquids in metal microarchitectures that could aid and impact fields of microelectronics, pharmaceuticals, and energy storage.

Designing tailored stationary phase materials is essential for extending chromatographic techniques from conventional molecular systems to the separation of (nano)particles. In this work, we investigate key aspects of the design of stationary phase materials using silica supraparticles. Supraparticles are defined spherical aggregates of sub-micron sized primary particles, which provide tunable pore sizes and thus form a variable model system to elucidate structure-property relations for the size-exclusion chromatography of colloidal nanoparticles. We fabricate supraparticles with tunable pore sizes (70-200 nm) and particle sizes (13-25 μm) and systematically enhance their mechanical stability through high-temperature sintering and binder reinforcement to ensure stability upon packing. Using gold nanoparticles (5-100 nm) as model analytes, we demonstrate pore size-dependent elution behavior, quantify accessible pore volume via the dimensionless distribution coefficient, and investigate the role of pore size and supraparticle size on column efficiency. We further demonstrate effective separation of nanoparticles from molecular impurities and agglomerates, as well as partial to near-complete separation of binary nanoparticle mixtures depending on their size differences. Moreover, we analyze the packing structure inside columns using X-ray micro-computed tomography, revealing packing defects as a key cause of moderate performance, underscoring the importance of optimized packing protocols. Using supraparticles as a versatile model system, our work offers practical insights into the design of tunable stationary phase materials for efficient nanoparticle separation via chromatography.

Solid-state nuclear magnetic resonance spectroscopy under Magic Angle Spinning (MAS) is one of the most powerful analytic techniques and in principle the method of choice to elucidate with molecular detail all components of complex solid or solid-liquid samples. MAS NMR under light irradiation is yet little developed, with technical solutions and first applications just emerging. We present the first operando observation of photoreforming of methanol to formaldehyde in a transparent rotor, irradiated at 365 nm by four LEDs, at spinning rates up to 11.5 kHz. The photon flux inside the rotor is quantified by an actinometric reaction. Efficient light penetration into the entire rotor volume is crucial. Therefore, we introduce silica monoliths with a continuous network of macropores, coated with TiO2 (anatase) as supported heterogeneous catalyst. These monoliths provide a large pore volume to accommodate the liquid substrate and a high surface area. Centrally, the network of pores larger than the visible light enhances light penetration into the material by a factor of two compared to a powder. Silica monoliths may be easily decorated with various photocatalysts and thus provide a versatile platform for observing in real time photocatalytic reactions by solid-state NMR.

Superalloys are renowned for their exceptional high-temperature strength and are essential in gas turbine engines. Much research has focused on solute partitioning to defects, leading to local phase transformations (LPT) that impact mechanical properties. This study investigates five single-crystalline CoNi-based alloys derived from polycrystalline CoWAlloy1, with variations in Nb, Re, Ta, Ti, and W. Their performance is compared with established Ni-based alloys (NA1, NA6, ME3, RRHT5) using constant strain rate (CSR) compression and compression creep tests. Deformation mechanisms were investigated utilizing transmission electron microscopy (TEM) and atomic resolution X-ray energy dispersive spectroscopy (EDS). Thermodynamic calculations were also employed to rationalize alloy behavior in the context of LPT. Results showed CSR testing at 850 °C ( ε̇=10^-4 s^-1 ) parallels creep testing in predicting alloy performance within deformation regimes dominated by γ′ shearing via planar defects. Nb and Ta were highlighted as critical in enhancing LPT by increasing η and χ ordering, unlike Ti, which showed significantly less influence. Although theoretical models suggested Re and W would enhance LPT, they exhibited poor behavior in creep tests due to low diffusivity. These findings validated using η-ordering tendency to estimate high-temperature performance and establish the groundwork for computationally driven LPT design in CoNi-based superalloys for disk applications.

Metallic micrometamaterials exhibit exceptional specific strength and energy dissipation capacity, yet their mechanical behavior under extreme thermomechanical conditions remains poorly understood. Here, we uncover deformation mechanisms in metallic microlattices subjected to combined thermal and mechanical extremes. Copper microlattices were fabricated via a localized electrodeposition process with submicron spatial resolution and, for the first time, compressed at cryogenic (-150 degrees C) and room temperatures under high strain rates up to 100 s-1. The copper microlattices, characterized by micron-sized grains and randomly oriented growth twins, exhibit distinct temperature- and strain rate-dependent deformation responses that lead to enhanced energy dissipation. Compression tests on copper micropillars, which are dimensionally equivalent to the microlattice struts, reveal substantial shifts in deformation mechanisms from dislocation slip to mechanical twinning as a function of temperature and strain rate. Together, these results provide a comprehensive framework for designing metallic micrometamaterials optimized for extreme thermomechanical environments.

Making solution-cast organic solar cells industrially available generally comes at the cost of significant performance losses compared to device prototypes manufactured under laboratory conditions. Adjusting solvent evaporation kinetics is postulated to recover efficiency. Yet, a comprehensive characterization of their effect, independently of other property-defining parameters, is lacking. Thus, the present objective is to isolate the influence of the solvent drying rate on solution-deposited organic active layer nanomorphologies and performances. To this end, a specially designed gas quenching technique is employed to fabricate PM6:Y6 donor-acceptor films under systematic variations of evaporation conditions. Using an extensive investigation protocol that combines insights from numerical simulations and experimental measurements, process-structure-performance relationships are unraveled. It is found that higher drying rates imply finer and more dispersed nanomorphologies with increased fractions of amorphous material. This enhances electric charge generation, thereby improving short-circuit current density and overall cell performance. The open-circuit voltage is also boosted under accelerated evaporation due to changes in the aggregation mode of the Y6 small molecule that induce higher effective bandgaps. The results demonstrate that the developed gas-quenching technique is a valuable tool for optimizing the performance of upscaled organic photovoltaics, as it is readily compatible with high-throughput equipment, such as roll-to-roll coating machines.

We present the first multiscale identical location tomography of a porous transport electrode (PTE) of a proton exchange membrane water electrolyzer. The tomogram encompasses length scales between micrometer-thick fibers to nanopores in the catalyst layer (CL) with nanometer-thin binder coatings on the iridium-oxide particles. It was recorded using micro-computed tomography, focused ion beam scanning electron microscopy tomography, scanning transmission electron microscopy and spectroscopy, nitrogen adsorption, and supplemented by a modeling approach. The reconstruction of the PTE reveals a porosity of around 51% of the porous transport layer (PTL) and 61% of the CL. A thorough analysis of the CL allows a comparison with the pristine catalyst powder and a realistic prediction of the transport parameters by modeling the binder thickness to a mean of 7 to 10.5 nm. Further, the overall transport parameters of the PTE are determined. The PTL has a higher permeability in the through-plane direction, whereas the CL shows isotropic transport properties. This study offers a comprehensive picture of the multiscale structure and properties of a PTE, which allows for a comparison with catalyst-coated membranes and computer-aided optimization of future PTEs.

Recently, it has been reported that the formation of B2 crystals in CuPdAgRu alloys leads to a notable increase in strength and conductivity. Here, we investigate the microstructural evolution associated with the formation of the ordered B2 phase: Correlative X-ray and electron diffraction analysis confirms the partial transformation of the initial fcc structure of the alloy into B2; the distribution of alloying elements within the latter phase is revealed by atomic-scale energy-dispersive X-ray spectroscopy. 4D-STEM virtual dark-field imaging uncovers a finely and homogeneously distributed B2 phase. High-resolution STEM imaging directly reveals few-nanometer thin plate-like regions of fcc remaining embedded coherently in the B2 matrix with a specific orientation relationship; these regions correlate with an enrichment of Ag and depletion of Cu, contributing to the large lattice misfit between both phases. These observations provide insights into microscopic-level structural changes and their possible influence on macroscopic properties of advanced functional alloys.

The required energy for shearing γʹ precipitates and generating planar faults in the L12-crystal structure has a significant effect on the overall strength of γ / γʹ superalloys. To reveal the influence of the crucial alloying elements Ta and Cr on the planar defect energies in the γʹ Co3(Al,W) phase of Co-based superalloys, compression testing of single freestanding cubes was conducted. For comparison, the γʹ Co3(Ti,Cr) phase, an alternate strengthening precipitate phase, was tested. Atomistic simulations of compression tests on Ni3Al nanocubes with varying compositions confirmed a direct correlation between the required stresses for nucleation of partial dislocations at the γʹ cube surface and the unstable and stable complex stacking fault energies of the γʹ phase. Hence, the effect of the alloying elements on the mechanical properties could be ascribed to their impact on the complex stacking fault energy. High-resolution scanning transmission electron microscopy revealed the presence of intrinsic and extrinsic stacking faults during compression of the γʹ cubes by glide of a/6 <112>(111) Shockley partial dislocations and anti-phase boundaries. No segregation of solutes to the planar defects was detected with energy-dispersive X-ray spectroscopy, as expected for room temperature deformation. The overall resistance against shearing of the Co3(Al,W) phase seems to be higher compared to the Co3(Ti,Cr) phase. Ta increases the resistance of Co3(Al,W) precipitates against shearing by Shockley partial dislocations, while Cr reduces it. Accordingly, the results indicate that Ta increases and Cr decreases the complex stacking fault energies in Co3(Al,W)-based superalloys.

Abstract Fused filament fabrication (FFF) 3D printing provides an accessible route to fabricating retrievable photocatalytic architectures with tunable geometry and composition. Here, we address the limited recoverability and reusability of conventional powder-based photocatalysts by translating a metal-free semiconductor catalyst to 3D printed electrodes. Graphitic carbon nitride (g-C3N4) was functionalized with carbonized polydopamine (cPDA) to create a modified photocatalyst with improved photophysical behavior, consistent, more effective charge separation, and longer-lived photoexcited states, which correlates with enhanced photocatalytic activity. The optimized formulation was compounded into an extrudable PLA-based composite filament and printed into electrodes containing either g-C3N4 or g-C3N4/cPDA. The printed g-C3N4/cPDA electrodes show enhanced photocatalytic rhodamine B degradation under simulated sunlight compared with unmodified printed electrodes. In contrast to suspended powders, the electrodes enable straightforward retrieval, improved operational stability, and reuse without postseparation steps. Furthermore, we demonstrate that electrode performance can be increased by scaling the surface area, highlighting geometry as a simple handle for upscaling. This work demonstrates the potential of photocatalytic 3D printed electrodes made from abundant materials via low-energy processing as a scalable and sustainable route for wastewater treatment.

Abstract The multilevel assembly of conjugated polymers critically determines their electronic performance. However, establishing a direct correlation from molecular-level interactions to macroscopic morphology and charge transport properties remains challenging. In this work, advanced characterization techniques were employed to identify and visualize two distinct assembly processes of a representative n-type conjugated polymer, F4BDOPV-2T, in both solution and thin film states, allowing for a structural correlation between solvent affinities and assembly structures. In 1-chloronaphthalene, strong solvation of the conjugated backbones promoted sidechain-dominated growth of nanoscale assemblies and ordered lamellar packing, resulting in compact 3D cluster aggregates in solution and well-oriented, large-scale ordered crystalline grains in the solid state. Conversely, toluene favored sidechain solvation, leading to backbone-dominated assembly growth that formed fiber networks and interconnected crystalline grains. The superior grain connectivity during backbone-dominated growth outweighed the effect of smaller grain size, yielding a three-fold enhancement in electron mobility (μe = 2.05 cm2 V–1 s–1). Through real-space electron microscopy visualization, this work bridges intermolecular interactions with multilevel assembly structures of conjugated polymers, providing fundamental insights into rational solvent regulation and morphological control for high-performance organic electronics.

Despite centuries of advancement, the synthesis of carbon materials remains heavily reliant on energy-intensive thermal processes. Conventional methods require external heating for prolonged periods to overcome high energy barriers, posing challenges for sustainable large-scale production. Here we show an energy-autonomous synthesis pathway that utilizes the intrinsic chemical energy stored within a polyaniline-HClO4 composite. Triggered by mild thermal, microwave, or mechanical stimulation, the precursor undergoes a rapid exothermic self-propagation driven by the explosive decomposition of perchlorate species. This single-step process, completed in ≈0.4 s, simultaneously generates intense localized heat and a massive volume of gas, which forcibly exfoliates and carbonizes the polymer into interconnected 2D amorphous carbon nanosheets. We demonstrate that this energy-efficient method achieves carbon conversion efficiencies comparable to traditional pyrolysis. Furthermore, the reaction intensity is precisely tunable via the precursor water content, ensuring potential for safe industrial scale-up. This approach also enables the atomic-level incorporation of transition metals, creating a versatile platform for the design of catalysts for oxygen and carbon dioxide reduction reactions. This work provides a scalable, energy-autonomous pathway for carbon synthesis and offers a platform for the precise construction of catalytic architectures.

Reducing iridium loading in proton exchange membrane water electrolyzer anodes is essential to meet cost targets for large‐scale green hydrogen production. Here, we report a photodeposition‐based synthesis of TiO 2 @IrO 2 core‐shell catalysts with iridium contents as low as 10 wt%. The influence of annealing temperature, iridium content, and iridium loading on structural and electrochemical properties is systematically investigated. An annealing temperature of 450 °C provides the best compromise between activity, conductivity, and stability. Remarkably, even at 10 wt% Ir (≈4.5 vol% IrO 2 ), the core‐shell architecture maintains high electronic conductivity and mass activity. The low iridium content results in ~18 μm thick catalyst layers at a loading of 0.35 mg Ir cm −2 , corresponding to a high thickness factor of 52.0 ± 0.8 μm (mg Ir cm −2 ) −1 . Two‐dimensional, two‐phase performance modeling reveals that these thick catalyst layers improve electronic connectivity at low loadings, leading to higher catalyst utilization than a commercial reference. As a result, the core‐shell catalyst outperforms the reference in single‐cell measurements, achieving 1.77 V at 2 A cm −2 at a low loading of 0.31 mg Ir cm −2 . During 200 h durability testing, reversible degradation is observed, while irreversible losses remain on par with the reference and the core–shell structure is preserved.