Spin Dynamics in Hybrid Halide Perovskites - Effect\nof Dynamical and Permanent Symmetry Breaking

The hybrid organic–inorganic\nhalide perovskite (HOIP), for\nexample, MAPbBr<sub>3</sub>, exhibits extended spin lifetime and apparent\nspin lifetime anisotropy in experiments. The underlying mechanisms\nof these phenomena remain illusive. By utilizing our first-principles\ndensity-matrix dynamics approach with quantum scatterings including\nelectron–phonon and electron–electron interactions and\nself-consistent spin–orbit coupling, we present temperature-\nand magnetic field-dependent spin lifetimes in hybrid perovskites,\nin agreement with experimental observations. For centrosymmetric hybrid\nperovskite MAPbBr<sub>3</sub>, the experimentally observed spin lifetime\nanisotropy is mainly attributed to the dynamic Rashba effect arising\nfrom the interaction between organic and inorganic components and\nthe rotation of the organic cation. For noncentrosymmetric perovskites,\nsuch as MPSnBr<sub>3</sub>, we found persistent spin helix texture\nat the conduction band minimum, which significantly enhances the spin\nlifetime anisotropy. Our study provides theoretical insight into spin\ndynamics in HOIP and strategies for controlling and optimizing spin\ntransport.