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Creators/Authors contains: "Singer, Andrej"

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  1. The ability to visualize crystalline defects and lattice distortions at the nanoscale holds profound implications for enhancing material properties and optimizing their design. Bragg coherent diffractive imaging (BCDI) emerged as a powerful technique due to its simplicity and high sensitivity to lattice strains. This review examines recent advancements in BCDI, highlighting its capability to uncover defects under various experimental conditions. It discusses fundamental principles and data analysis intricacies as well as BCDI's applications in characterizing structural and functional materials. Furthermore, it offers perspectives on the current limitations of BCDI and the potential implications of synchrotron upgrades. By providing these insights, the review aims to enhance the role of BCDI in advancing materials science and nanotechnology. 
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  2. Abstract Discontinuous solid-solid phase transformations play a pivotal role in determining the properties of rechargeable battery electrodes. By leveraging operando Bragg Coherent Diffractive Imaging (BCDI), we investigate the discontinuous phase transformation in LixNi0.5Mn1.5O4within an operational Li metal coin cell. Throughout Li-intercalation, we directly observe the nucleation and growth of the Li-rich phase within the initially charged Li-poor phase in a 500 nm particle. Supported by the microelasticity model, the operando imaging unveils an evolution from a curved coherent to a planar semi-coherent interface driven by dislocation dynamics. Our data indicates negligible kinetic limitations from interface propagation impacting the transformation kinetics, even at a discharge rate of C/2 (80 mA/g). This study highlights BCDI’s capability to decode complex operando diffraction data, offering exciting opportunities to study nanoscale phase transformations with various stimuli. 
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    Free, publicly-accessible full text available December 1, 2025
  3. Abstract Mott metal–insulator transitions possess electronic, magnetic, and structural degrees of freedom promising next‐generation energy‐efficient electronics. A previously unknown, hierarchically ordered, and anisotropic supercrystal state is reported and its intrinsic formation characterized in‐situ during a Mott transition in a Ca2RuO4thin film. Machine learning‐assisted X‐ray nanodiffraction together with cryogenic electron microscopy reveal multi‐scale periodic domain formation at and below the film transition temperature (TFilm ≈ 200–250 K) and a separate anisotropic spatial structure at and aboveTFilm. Local resistivity measurements imply an intrinsic coupling of the supercrystal orientation to the material's anisotropic conductivity. These findings add a new degree of complexity to the physical understanding of Mott transitions, opening opportunities for designing materials with tunable electronic properties. 
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  4. Unlike naturally occurring oxide crystals such as ruby and gemstones, there are no naturally occurring nitride crystals because the triple bond of the nitrogen molecule is one of the strongest bonds in nature. Here, we report that when the transition metal scandium is subjected to molecular nitrogen, it self-catalyzes to break the nitrogen triple bond to form highly crystalline layers of ScN, a semiconductor. This reaction proceeds even at room temperature. Self-activated ScN films have a twin cubic crystal structure, atomic layering, and electronic and optical properties comparable to plasma-based methods. We extend our research to showcase Sc’s scavenging effect and demonstrate self-activated ScN growth under various growth conditions and on technologically significant substrates, such as 6H–SiC, AlN, and GaN. Ab initio calculations elucidate an energetically efficient pathway for the self-activated growth of crystalline ScN films from molecular N2. The findings open a new pathway to ultralow-energy synthesis of crystalline nitride semiconductor layers and beyond. 
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  5. Bragg coherent X-ray diffractive imaging is a cutting-edge method for recovering three-dimensional crystal structure with nanoscale resolution. Phase retrieval provides an atomic displacement parallel to the Bragg peak reciprocal lattice vector. The derivative of the displacement along the same vector provides the normal strain field, which typically serves as a proxy for any structural changes. In this communication it is found that the other component of the displacement gradient, perpendicular to the reciprocal lattice vector, provides additional information from the experimental data collected from nanocrystals with mobile dislocations. Demonstration on published experimental data show how the perpendicular component of the displacement gradient adds to existing analysis, enabling an estimate for the external stresses, pinpointing the location of surface dislocations, and predicting the dislocation motion in in situ experiments. 
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  6. New properties and exotic quantum phenomena can form due to periodic nanotextures, including Moire patterns, ferroic domains, and topologically protected magnetization and polarization textures. Despite the availability of powerful tools to characterize the atomic crystal structure, the visualization of nanoscale strain-modulated structural motifs remains challenging. Here, we develop nondestructive real-space imaging of periodic lattice distortions in thin epitaxial films and report an emergent periodic nanotexture in a Mott insulator. Specifically, we combine iterative phase retrieval with unsupervised machine learning to invert the diffuse scattering pattern from conventional X-ray reciprocal-space maps into real-space images of crystalline displacements. Our imaging in PbTiO3/SrTiO3superlattices exhibiting checkerboard strain modulation substantiates published phase-field model calculations. Furthermore, the imaging of biaxially strained Mott insulator Ca2RuO4reveals a strain-induced nanotexture comprised of nanometer-thin metallic-structure wires separated by nanometer-thin Mott-insulating-structure walls, as confirmed by cryogenic scanning transmission electron microscopy (cryo-STEM). The nanotexture in Ca2RuO4film is induced by the metal-to-insulator transition and has not been reported in bulk crystals. We expect the phasing of diffuse X-ray scattering from thin crystalline films in combination with cryo-STEM to open a powerful avenue for discovering, visualizing, and quantifying the periodic strain-modulated structures in quantum materials. 
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