{"title":"无机卤化物包光体中八面体倾斜造成的结构紊乱:贝叶斯优化的新见解","authors":"Jingrui Li, Fang Pan, Guo-Xu Zhang, Zenghui Liu, Hua Dong, Dawei Wang, Zhuangde Jiang, Wei Ren, Zuo-Guang Ye, Milica Todorović, Patrick Rinke","doi":"10.1002/sstr.202400268","DOIUrl":null,"url":null,"abstract":"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 CsPbI<sub>3</sub> and CsPbBr<sub>3</sub> 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.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":"164 1","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2024-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Structural Disorder by Octahedral Tilting in Inorganic Halide Perovskites: New Insight with Bayesian Optimization\",\"authors\":\"Jingrui Li, Fang Pan, Guo-Xu Zhang, Zenghui Liu, Hua Dong, Dawei Wang, Zhuangde Jiang, Wei Ren, Zuo-Guang Ye, Milica Todorović, Patrick Rinke\",\"doi\":\"10.1002/sstr.202400268\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"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 CsPbI<sub>3</sub> and CsPbBr<sub>3</sub> 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.\",\"PeriodicalId\":21841,\"journal\":{\"name\":\"Small Structures\",\"volume\":\"164 1\",\"pages\":\"\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-07-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Small Structures\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1002/sstr.202400268\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Small Structures","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1002/sstr.202400268","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
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 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.