Unraveling the Defect-Dominated Broadband Emission Mechanisms in (001)-Preferred Two-Dimensional Layered Antimony-Halide Perovskite Film

Zichen Yang; Weiwei Meng; Jiaxing Kang; Xiang Wang; Xin Shu; Teng Chen; Run Xu; Fei Xu; Feng Hong

doi:10.1021/acs.jpclett.2c03151

Unraveling the Defect-Dominated Broadband Emission Mechanisms in (001)-Preferred Two-Dimensional Layered Antimony-Halide Perovskite Film

J Phys Chem Lett. 2022 Dec 22;13(50):11736-11744. doi: 10.1021/acs.jpclett.2c03151. Epub 2022 Dec 14.

Authors

Zichen Yang¹, Weiwei Meng², Jiaxing Kang¹, Xiang Wang¹, Xin Shu¹, Teng Chen³, Run Xu^{4

5}, Fei Xu^{1

5

6}, Feng Hong^{1

5}

Affiliations

¹ SHU-Solar E R&D Lab, Department of Physics, College of Sciences, Shanghai Key Laboratory of High Temperature Superconductors, Shanghai Frontiers Science Center of Quantum and Superconducting Matter States, Shanghai University, Shanghai200444, China.
² School of Physics and Technology, Center for Electron Microscopy, MOE Key Laboratory of Artificial Micro- and Nano-structures, and Institute for Advanced Studies, Wuhan University, Wuhan430072, China.
³ Shanghai Key Laboratory of Mechanics in Energy Engineering, Shanghai Institute of Applied Mathematics and Mechanics, School of Mechanics and Engineering Science, Shanghai University, Shanghai200444, China.
⁴ Department of Electronic Information Materials, School of Materials Science and Engineering, Shanghai University, Shanghai200444, China.
⁵ Zhejiang Institute of Advanced Materials, Shanghai University, Jiashan314113, China.
⁶ State Key Laboratory of Surface Physics, Department of Physics, Fudan University, Shanghai200433, China.

PMID: 36515687
DOI: 10.1021/acs.jpclett.2c03151

Abstract

By adding molar-controlled SbCl₃ in a Cs₃Sb₂Cl₉ precursor, we employed a low-temperature solution-processed approach to prepare high-quality (001)-preferred Cs₃Sb₂Cl₉ thin film, which demonstrates a stable defect-dominated broadband emission at room temperature. Density functional theory calculations reveal that the defect emission originates from the donor-acceptor pair (DAP) recombination between chlorine vacancy (V_Cl) and cesium vacancy (V_Cs). Furthermore, V_Cl + V_Cs DAP is more stable on the (001) surface. The improved film quality and the more stable V_Cl + V_Cs DAP increase the activation energy related to defect states, resulting in an enhancement of the defect emission for the high-quality (001)-preferred film. This work provides deep insight into the key role of the (001) surface in defect emission and a feasible strategy to enhance the defect emission in 2D halide perovskites A₃B₂X₉ (A = CH₃NH₃, Cs, Rb; B = Bi, Sb; X = Cl, Br, I) by control of the thin film preferred orientation.