Theoretical Study on the Contacting Interface-Dependent Band Alignments of CsPbBr3@MoS2 van der Waals Heterojunctions: Spin–Orbit Coupling Does MatterClick to copy article linkArticle link copied!
- Dong-Hui XuDong-Hui XuCollege of Chemistry and Material Science, Sichuan Normal University, Chengdu 610068, ChinaMore by Dong-Hui Xu
- Jun-Feng LiuJun-Feng LiuCollege of Chemistry and Material Science, Sichuan Normal University, Chengdu 610068, ChinaMore by Jun-Feng Liu
- Xu-Jiang WanXu-Jiang WanCollege of Chemistry and Material Science, Sichuan Normal University, Chengdu 610068, ChinaMore by Xu-Jiang Wan
- Xiang-Yang Liu*Xiang-Yang Liu*Email: [email protected]College of Chemistry and Material Science, Sichuan Normal University, Chengdu 610068, ChinaMore by Xiang-Yang Liu
- Ganglong CuiGanglong CuiKey Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University, Beijing 100875, ChinaMore by Ganglong Cui
- Laicai Li*Laicai Li*Email: [email protected]College of Chemistry and Material Science, Sichuan Normal University, Chengdu 610068, ChinaMore by Laicai Li
Abstract
Van der Waals heterojunctions formed by all-inorganic cesium lead halide perovskites and two-dimensional transition-metal dichalcogenides (TMDs) have received much attention in recent years due to their outstanding optoelectronic properties. However, several fundamental issues such as band alignments and carrier dynamics in these novel heterojunctions remain unclear. Herein, we have first exploited static electronic structure calculations in combination with non-adiabatic dynamics simulations to investigate the interfacial properties of the heterojunctions formed by monolayer MoS2 and CsPbBr3 nanosheets. Our results indicate that the interfacial properties are closely related to the contacting interfaces during the formation of the heterojunctions. First, the planar-average charge-density difference and charge-density difference analyses indicate that the charge-transfer properties during the formation of heterojunctions are different with different contacting interfaces. Second, the band alignment alters from type-I to type-II, while the contacting facet of CsPbBr3 changes from PbBr2- to CsBr-terminated one. Moreover, the spin–orbit coupling effects are indispensable for correctly predicting such contacting interface-dependent band alignments of CsPbBr3@MoS2 heterojunctions. Finally, the non-adiabatic dynamics simulations reveal that the electron transfer from CsPbBr3 to MoS2 takes place within 100 fs in type-II CsPbBr3–CsPb@MoS2 due to the small adjacent energy differences. Based on these results, we propose that such contacting interface-dependent band alignments might be responsible for the experimentally observed weakened instead of totally vanished photoluminescence. Our present work not only provides a reasonable microscopic mechanism for interpreting previous experimental results but can also be helpful for the future design of novel devices based on two-dimensional TMD and perovskite heterojunctions with better optoelectronic performance.
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