Enhancing Optoelectronic Properties of Quasi-2D Ruddlesden–Popper Perovskites via Pseudo–Halogen Doping: A First–Principles Study on Cs₂Pb(SCN)₂Br₂
Year: 2025
Author: Peng Xiong, Jia-Ming Li, Zhi-Mi Zhang, Zhong-Yuan Wang, Jian Wu, Chuan-Jia Tong
Communications in Computational Chemistry, Vol. 1 (2025), Iss. 1 : pp. 81–87
Abstract
Two-dimensional (2D) Ruddlesden-Popper (RP) perovskites have been intensively investigated due to their superior stability and outstanding optoelectronic properties. Although A-site doping in quasi-2D RP-phase perovskites has been extensively studied, the effect of X-site doping remains unknown. Using first-principles calculations, this work demonstrates that $SCN^-$ substitution in Cs₂Pb(SCN)₂Br₂ induces a structural transformation from isotropic to anisotropic through octahedral tilting along the b-axis, reducing octahedral spacing from 5.17 to 4.88 Å. This structural modification enhances carrier mobility, dramatically increases exciton binding energy from 30.47 to 145.39 meV, and improves defect tolerance compared to pristine Cs₂PbBr₄. These modifications synergistically suppress non-radiative recombination pathways while promoting radiative processes, so that improve its performance as a promising light-emitting diode (LED) material. These findings establish pseudo-halogen substitution as a promising strategy for optimizing carrier transport and radiative efficiency in low-dimensional perovskite LED devices.
Journal Article Details
Publisher Name: Global Science Press
Language: English
DOI: https://doi.org/10.4208/cicc.2025.84.02
Communications in Computational Chemistry, Vol. 1 (2025), Iss. 1 : pp. 81–87
Published online: 2025-01
AMS Subject Headings: Global Science Press
Copyright: COPYRIGHT: © Global Science Press
Pages: 7
Keywords: Ruddlesden-Popper (RP) perovskites LED exciton binding energy carrier mobility.