Structural Dynamics Descriptors for Metal Halide Perovskites
- 주제(기타) Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary
- 설명문(일반) [Liang, Xia; Klarbring, Johan; Li, Zhenzhu; Walsh, Aron] Imperial Coll London, Dept Mat, London SW7 2AZ, England; [Klarbring, Johan] Linkoping Univ, Dept Phys Chem & Biol IFM, SE-58183 Linkoping, Sweden; [Baldwin, William J.; Csanyi, Gabor] Univ Cambridge, Dept Engn, Cambridge CB2 1PZ, England; [Walsh, Aron] Ewha Womans Univ, Dept Phys, Seoul 03760, South Korea
- 등재 SCIE, SCOPUS
- OA유형 hybrid, Green Submitted
- 발행기관 AMER CHEMICAL SOC
- 발행년도 2023
- 총서유형 Journal
- URI http://www.dcollection.net/handler/ewha/000000211566
- 본문언어 영어
- Published As https://doi.org/10.1021/acs.jpcc.3c03377
- PubMed 37791100
초록/요약
Metal halide perovskites have shown extraordinary performance in solar energy conversion technologies. They have been classified as "soft semiconductors" due to their flexible corner-sharing octahedral networks and polymorphous nature. Understanding the local and average structures continues to be challenging for both modeling and experiments. Here, we report the quantitative analysis of structural dynamics in time and space from molecular dynamics simulations of perovskite crystals. The compact descriptors provided cover a wide variety of structural properties, including octahedral tilting and distortion, local lattice parameters, molecular orientations, as well as their spatial correlation. To validate our methods, we have trained a machine learning force field (MLFF) for methylammonium lead bromide (CH3NH3PbBr3) using an on-the-fly training approach with Gaussian process regression. The known stable phases are reproduced, and we find an additional symmetry-breaking effect in the cubic and tetragonal phases close to the phase-transition temperature. To test the implementation for large trajectories, we also apply it to 69,120 atom simulations for CsPbI3 based on an MLFF developed using the atomic cluster expansion formalism. The structural dynamics descriptors and Python toolkit are general to perovskites and readily transferable to more complex compositions.
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