Structural Disorder by Octahedral Tilting in Inorganic Halide Perovskites: New Insight with Bayesian Optimization
Structural disorder is common in metal‐halide perovskites and important for understanding the functional properties of these materials. First‐principles methods can address structure variation on the atomistic scale, but they are often limited by the lack of structure‐sampling schemes required to ch...
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| Format: | Article |
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Wiley-VCH
2024-11-01
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| Series: | Small Structures |
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| Online Access: | https://doi.org/10.1002/sstr.202400268 |
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| author | Jingrui Li Fang Pan Guo‐Xu Zhang Zenghui Liu Hua Dong Dawei Wang Zhuangde Jiang Wei Ren Zuo‐Guang Ye Milica Todorović Patrick Rinke |
| author_facet | Jingrui Li Fang Pan Guo‐Xu Zhang Zenghui Liu Hua Dong Dawei Wang Zhuangde Jiang Wei Ren Zuo‐Guang Ye Milica Todorović Patrick Rinke |
| author_sort | Jingrui Li |
| collection | DOAJ |
| description | Structural disorder is common in metal‐halide perovskites and important for understanding the functional properties of these materials. First‐principles methods can address structure variation on the atomistic scale, but they are often limited by the lack of structure‐sampling schemes required to characterize the disorder. Herein, structural disorder in the benchmark inorganic halide perovskites CsPbI3 and CsPbBr3 is computationally studied in terms of the three octahedral‐tilting angles. The subsequent variations in energetics and properties are described by 3D potential‐energy surfaces (PESs) and property landscapes, delivered by Bayesian optimization as implemented in the Bayesian optimization structure search code sampling density functional theory (DFT) calculations. The rapid convergence of the PES with about 200 DFT data points in 3D searches demonstrates the power of active learning and strategic sampling with Bayesian optimization. Further analysis indicates that disorder grows with increasing temperature and reveals that the material bandgap at finite temperatures is a statistical mean over disordered structures. |
| format | Article |
| id | doaj-art-b53711afebd54fa0b8d64df19cc31ba2 |
| institution | OA Journals |
| issn | 2688-4062 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Small Structures |
| spelling | doaj-art-b53711afebd54fa0b8d64df19cc31ba22025-08-20T02:12:29ZengWiley-VCHSmall Structures2688-40622024-11-01511n/an/a10.1002/sstr.202400268Structural Disorder by Octahedral Tilting in Inorganic Halide Perovskites: New Insight with Bayesian OptimizationJingrui Li0Fang Pan1Guo‐Xu Zhang2Zenghui Liu3Hua Dong4Dawei Wang5Zhuangde Jiang6Wei Ren7Zuo‐Guang Ye8Milica Todorović9Patrick Rinke10State Key Laboratory for Manufacturing Systems Engineering Electronic Materials Research Laboratory Key Laboratory of the Ministry of Education School of Electronic Science and Engineering Xi'an Jiaotong University Xi'an 710049 ChinaState Key Laboratory for Manufacturing Systems Engineering Electronic Materials Research Laboratory Key Laboratory of the Ministry of Education School of Electronic Science and Engineering Xi'an Jiaotong University Xi'an 710049 ChinaMIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin 150001 ChinaState Key Laboratory for Manufacturing Systems Engineering Electronic Materials Research Laboratory Key Laboratory of the Ministry of Education School of Electronic Science and Engineering Xi'an Jiaotong University Xi'an 710049 ChinaKey Laboratory for Physical Electronics and Devices of the Ministry of Education and Shaanxi Key Lab of Information Photonic Technique School of Electronic Science and Engineering Xi'an Jiaotong University Xi'an 710049 ChinaSchool of Microelectronics and Key Lab of Micro‐Nano Electronics and System Integration of Xi'an City Xi'an Jiaotong University Xi'an 710049 ChinaState Key Laboratory for Manufacturing Systems Engineering & International Joint Laboratory for Micro/Nano Manufacturing and Measurement Technology Xi'an Jiaotong University Xi'an 710049 ChinaState Key Laboratory for Manufacturing Systems Engineering Electronic Materials Research Laboratory Key Laboratory of the Ministry of Education School of Electronic Science and Engineering Xi'an Jiaotong University Xi'an 710049 ChinaDepartment of Chemistry and 4D LABS Simon Fraser University Burnaby British Columbia V5A 1S6 CanadaDepartment of Mechanical and Materials Engineering University of Turku FI‐20014 Turku FinlandDepartment of Applied Physics Aalto University P.O.Box 11100, AALTO FI‐00076 Espoo FinlandStructural disorder is common in metal‐halide perovskites and important for understanding the functional properties of these materials. First‐principles methods can address structure variation on the atomistic scale, but they are often limited by the lack of structure‐sampling schemes required to characterize the disorder. Herein, structural disorder in the benchmark inorganic halide perovskites CsPbI3 and CsPbBr3 is computationally studied in terms of the three octahedral‐tilting angles. The subsequent variations in energetics and properties are described by 3D potential‐energy surfaces (PESs) and property landscapes, delivered by Bayesian optimization as implemented in the Bayesian optimization structure search code sampling density functional theory (DFT) calculations. The rapid convergence of the PES with about 200 DFT data points in 3D searches demonstrates the power of active learning and strategic sampling with Bayesian optimization. Further analysis indicates that disorder grows with increasing temperature and reveals that the material bandgap at finite temperatures is a statistical mean over disordered structures.https://doi.org/10.1002/sstr.202400268Bayesian optimizationscesium lead halide perovskitesfirst‐principles calculationsmultidimensional potential‐energy surfacesstructural disorders |
| spellingShingle | Jingrui Li Fang Pan Guo‐Xu Zhang Zenghui Liu Hua Dong Dawei Wang Zhuangde Jiang Wei Ren Zuo‐Guang Ye Milica Todorović Patrick Rinke Structural Disorder by Octahedral Tilting in Inorganic Halide Perovskites: New Insight with Bayesian Optimization Small Structures Bayesian optimizations cesium lead halide perovskites first‐principles calculations multidimensional potential‐energy surfaces structural disorders |
| title | Structural Disorder by Octahedral Tilting in Inorganic Halide Perovskites: New Insight with Bayesian Optimization |
| title_full | Structural Disorder by Octahedral Tilting in Inorganic Halide Perovskites: New Insight with Bayesian Optimization |
| title_fullStr | Structural Disorder by Octahedral Tilting in Inorganic Halide Perovskites: New Insight with Bayesian Optimization |
| title_full_unstemmed | Structural Disorder by Octahedral Tilting in Inorganic Halide Perovskites: New Insight with Bayesian Optimization |
| title_short | Structural Disorder by Octahedral Tilting in Inorganic Halide Perovskites: New Insight with Bayesian Optimization |
| title_sort | structural disorder by octahedral tilting in inorganic halide perovskites new insight with bayesian optimization |
| topic | Bayesian optimizations cesium lead halide perovskites first‐principles calculations multidimensional potential‐energy surfaces structural disorders |
| url | https://doi.org/10.1002/sstr.202400268 |
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