文献类型：期刊文献

英文题名：Defect and carrier characteristics of chalcogenide perovskite BaZrS3 under thermodynamic stability: a first-principles study for photovoltaic application

作者：Chen, Qinmiao[1];Ni, Yi[1];Wang, Yufei[2,3]

机构：[1]East China Univ Sci & Technol, Sch Phys, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Chinese Acad Sci, Inst Semicond, Lab Solid State Optoelect Informat Technol, Beijing 100083, Peoples R China;[3]Univ Chinese Acad Sci, Coll Future Technol, Beijing 101408, Peoples R China

年份：2026

卷号：16

期号：7

起止页码：6677

外文期刊名：RSC ADVANCES

收录：;EI(收录号：20260720072924);WOS:【SCI-EXPANDED(收录号:WOS:001677909800001)】；

基金：The project is supported by the National Natural Science Foundation of China (No. 11604097).

语种：英文

外文关键词：Barium zirconate - Carrier concentration - Conversion efficiency - Defects - Film preparation - Perovskite solar cells - Photoelectricity - Photovoltaics - Semiconductor doping - Thermodynamic stability

摘要：BaZrS3 is reported to be an exceptional chalcopyrite perovskite with remarkable stability, making it a key material for the next-generation perovskite-inspired technologies. In this study, the thermodynamic stability of BaZrS3 was investigated while referencing all potential secondary phases in the Materials Project database. Furthermore, the influence of element doping on both the bands and thermodynamic stability of BaZrS3 was also studied, the band adjustment efficiency was validated, and experimental synthesis challenges were elucidated. Based on a large supercell, Heyd-Scuseria-Ernzerhof hybrid functional and finite-size effect correction, the concentration properties of defects and charge carriers of BaZrS3 were then determined in the thermodynamically stable region, from the characteristics of defect formation energy with varied Fermi levels. The results indicate that degenerated semiconductor characteristics exist in BaZrS3 in the thermodynamically stable region, which should be avoided. The defect transition energy level characteristics of BaZrS3 were also calculated and identified. Additionally, the properties of deep-level defects Si with high concentration were analyzed. While Si (+2/0) exhibits deep-level defect states, Si (+1/0) does not. The non-radiative and radiative capture coefficients of deep-level defect Si (+2/0) were calculated at 1.28682 x 10-25 and 3.51 x 10-15 cm3 s-1, respectively. The obtained defect and carrier qualities of BaZrS3 were applied to evaluate its photoelectric conversion efficiency. The manuscript investigates, for the first time, how defects evolve with changes in chemical potential in stable BaZrS3, providing valuable guidance for the experimentally controllable preparation of high-quality BaZrS3 films or devices.