Anisotropic Defect Diffusion in Layered CsPbBr$_\mathrm{x}$I$_\mathrm{3-x}$ Perovskites

Abstract

Mixed-halide perovskites offer a route to enhance phase stability and modify optoelectronic properties. Here, we use large-scale molecular dynamics simulations with a reactive force field to investigate defects in CsPbBr$_\mathrm{x}$I$_\mathrm{3-x}$ perovskites, focusing on how defect mobility can be controlled and the stability of the material may be improved by layered ordering of Br and I anions in layers. Our results show that layered halide ordering induces strongly anisotropic defect diffusion: migration proceeds readily along the layers, whereas diffusion across them is strongly suppressed. For Cs defects, this anisotropy originates from directional lattice strain and the associated octahedral tilting, while halide migration is governed by an interplay between strain and preferential local halide bonding configurations.