Spin Dynamics in Hybrid Halide Perovskites - Effect of Dynamical and Permanent Symmetry Breaking.

Abstract

The hybrid organic-inorganic halide perovskite (HOIP), for example, MAPbBr₃, exhibits extended spin lifetime and apparent spin lifetime anisotropy in experiments. The underlying mechanisms of these phenomena remain illusive. By utilizing our first-principles density-matrix dynamics approach with quantum scatterings including electron-phonon and electron-electron interactions and self-consistent spin-orbit coupling, we present temperature- and magnetic field-dependent spin lifetimes in hybrid perovskites, in agreement with experimental observations. For centrosymmetric hybrid perovskite MAPbBr₃, the experimentally observed spin lifetime anisotropy is mainly attributed to the dynamic Rashba effect arising from the interaction between organic and inorganic components and the rotation of the organic cation. For noncentrosymmetric perovskites, such as MPSnBr₃, we found persistent spin helix texture at the conduction band minimum, which significantly enhances the spin lifetime anisotropy. Our study provides theoretical insight into spin dynamics in HOIP and strategies for controlling and optimizing spin transport.