The dynamic surface evolution of halide perovskites induced by external energy stimulation

Feiyu Cheng; Pengdong Wang; Chenzhe Xu; Qingliang Liao; Suicai Zhang; Haochun Sun; Wenqiang Fan; Guodong Liu; Zhiyun Li; Yaping Kong; Li Wang; Fangsen Li; Zhuo Kang; Yue Zhang

doi:10.1093/nsr/nwae042

The dynamic surface evolution of halide perovskites induced by external energy stimulation

Natl Sci Rev. 2024 Feb 2;11(4):nwae042. doi: 10.1093/nsr/nwae042. eCollection 2024 Apr.

Authors

Feiyu Cheng^{1

2}, Pengdong Wang³, Chenzhe Xu^{1

2}, Qingliang Liao^{1

2}, Suicai Zhang^{1

2}, Haochun Sun^{1

2}, Wenqiang Fan^{1

2}, Guodong Liu⁴, Zhiyun Li³, Yaping Kong³, Li Wang³, Fangsen Li³, Zhuo Kang^{1

2}, Yue Zhang^{1

2}

Affiliations

¹ Academy for Advanced Interdisciplinary Science and Technology, State Key Laboratory for Advanced Metals and Materials, University of Science and Technology Beijing, Beijing 100083, China.
² Beijing Key Laboratory for Advanced Energy Materials and Technologies, Key Laboratory of Advanced Materials and Devices for Post-Moore Chips, Ministry of Education, Beijing Advanced Innovation Center for Materials Genome Engineering, School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China.
³ Vacuum Interconnected Nanotech Workstation (Nano-X), Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, China.
⁴ Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.

Abstract

Tracking the dynamic surface evolution of metal halide perovskite is crucial for understanding the corresponding fundamental principles of photoelectric properties and intrinsic instability. However, due to the volatility elements and soft lattice nature of perovskites, several important dynamic behaviors remain unclear. Here, an ultra-high vacuum (UHV) interconnection system integrated by surface-sensitive probing techniques has been developed to investigate the freshly cleaved surface of CH₃NH₃PbBr₃ in situ under given energy stimulation. On this basis, the detailed three-step chemical decomposition pathway of perovskites has been clarified. Meanwhile, the evolution of crystal structure from cubic phase to tetragonal phase on the perovskite surface has been revealed under energy stimulation. Accompanied by chemical composition and crystal structure evolution, electronic structure changes including energy level position, hole effective mass, and Rashba splitting have also been accurately determined. These findings provide a clear perspective on the physical origin of optoelectronic properties and the decomposition mechanism of perovskites.

Keywords: external energy stimulation; metal halide perovskite; surface dynamic evolution; surface electronic structure; ultra-high vacuum interconnection system.