Anisotropic Defect Diffusion in Layered CsPbBr x I3– x Perovskites

Abstract

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 CsPbBrxI3–x perovskites, focusing on how defect mobility can be controlled and the stability of the material improved by layered ordering of Br and I anions. 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, whereas halide migration is governed by an interplay between strain and preferential local halide bonding configurations.