The local atomic structures of amorphous Ge-Sb-Te phase-change materials have yet to be clarified and the rapid crystal-amorphous phase change resulting in distinct optical contrast is not well understood. We report the direct observation of local atomic structures in amorphous Ge_{2}Sb_{2}Te_{5} using "local" reverse Monte Carlo modeling dedicated to an angstrom-beam electron diffraction analysis. The results corroborated the existence of local structures with rocksalt crystal-like topology that were greatly distorted compared to the crystal symmetry. This distortion resulted in the breaking of ideal octahedral atomic environments, thereby forming local disordered structures that basically satisfied the overall amorphous structure factor. The crystal-like distorted octahedral structures could be the main building blocks in the formation of the overall amorphous structure of Ge-Sb-Te.
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http://dx.doi.org/10.1103/PhysRevLett.120.205502 | DOI Listing |
Chem Sci
December 2024
Shenzhen Grubbs Institute, Department of Chemistry, Guangdong Provincial Key Laboratory of Catalysis, Southern University of Science and Technology Shenzhen 518055 China
Distortion can play crucial roles in influencing structures and properties, as well as enhancing reactivity or selectivity in many chemical and biological systems. The distortion/interaction or activation-strain model is a popular and powerful method for deciphering the origins of activation energies, in which distortion and interaction energies dictate an activation energy. However, decomposition of local distortion energy at the atomic scale remains less clear and straightforward.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
Institut de Recherche sur les Céramiques (IRCER), UMR CNRS 7315-Université de Limoges, France.
A semi-automated workflow relying on atomic-scale modelling is introduced to explore and understand the yet-unsolved structure of the crystalline AsTe material, recently obtained from crystallization of the parent AsTe glass, which shows promising properties for thermoelectric applications. The seemingly complex crystal structure of AsTe is investigated with density functional theory, from the stand point of As/Te disorder, in a structural template derived from elemental-Te (Te), following experimental findings from combined X-ray total scattering and diffraction. Our workflow includes a combinatorial structure generation step followed by successive structure selection and relaxation steps with progressively-increasing accuracy levels and a multi-criterion evaluation procedure.
View Article and Find Full Text PDFSmall
January 2025
Department of Chemistry, Materials and Chemical Engineering "Giulio Natta", Politecnico di Milano, Piazza Leonardo da Vinci 32, Milano, 20133, Italy.
Single-atom catalysts (SACs) are gathering significant attention in chemistry due to their unique properties, offering uniform active site distribution and enhanced selectivity. However, their precise structure often remains unclear, with multiple models proposed in the literature. Understanding the coordination environment of the active site at the atomic level is crucial for explaining catalytic activity.
View Article and Find Full Text PDFJ Phys Chem A
January 2025
School of Physical Science and Technology, Southwest University, Chongqing 400715, China.
Searching for single-molecule magnets (SMM) with large effective blocking barriers, long relaxation times, and high magnetic blocking temperatures is vitally important not only for the fundamental research of magnetism at the molecular level but also for the realization of new-generation magnetic memory unit. Actinides (An) atoms possess extremely strong spin-orbit coupling (SOC) due to their 5 orbitals, and their ground multiplets are largely split into several sublevels because of the strong interplay between the SOC of An atoms and the crystal field (CF) formed by ligand atoms. Compared to TM-based SMMs, more dispersed energy level widths of An-based SMMs will give a larger total zero field splitting (ZFS) and thus provide a necessary condition to derive a higher .
View Article and Find Full Text PDFNature
January 2025
Department of Physics and Astronomy, University of California, Los Angeles, Los Angeles, CA, USA.
Microscopy and crystallography are two essential experimental methodologies for advancing modern science. They complement one another, with microscopy typically relying on lenses to image the local structures of samples, and crystallography using diffraction to determine the global atomic structure of crystals. Over the past two decades, computational microscopy, encompassing coherent diffractive imaging (CDI) and ptychography, has advanced rapidly, unifying microscopy and crystallography to overcome their limitations.
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