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

TL;DR

This study uses first-principles simulations to explore spin lifetimes and anisotropy in hybrid halide perovskites, revealing the roles of symmetry breaking and organic-inorganic interactions in spin dynamics.

Contribution

It introduces a comprehensive first-principles approach to analyze spin dynamics in HOIPs, highlighting mechanisms behind spin lifetime anisotropy and effects of symmetry breaking.

Findings

Dynamical Rashba effect causes spin lifetime anisotropy in centrosymmetric MAPbBr3.

Persistent spin helix texture enhances spin lifetime in noncentrosymmetric MPSnBr3.

Theoretical insights enable strategies to control spin transport in hybrid perovskites.

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 densitymatrix dynamics approach with quantum scatterings including electron-phonon and electronelectron interactions and self-consistent spinorbit 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 dynamical Rashba effect arising from the interaction between organic and inorganic components and the rotation of the organic cation. For noncentrosymmetric perovskite, 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 to spin dynamics in HOIP and strategies for controlling and optimizing spin transport.