How Spin Relaxes and Dephases in Bulk Halide Perovskites

TL;DR

This paper uses first-principles calculations to analyze spin relaxation and dephasing in halide perovskites, providing insights into spin dynamics crucial for spintronics and quantum technologies.

Contribution

It introduces an ab initio density-matrix dynamics framework to predict spin lifetimes and dephasing times in CsPbBr3, accounting for spin-orbit coupling and scattering processes.

Findings

Fr{"o}hlich interaction negligibly affects spin relaxation

Persistent spin helix can enhance spin lifetime with large spin-split

Rashba SOC does not realize persistent spin helix

Abstract

Spintronics in halide perovskites has drawn significant attention in recent years, due to highly tunable spin-orbit fields and intriguing interplay with lattice symmetry. Spin lifetime -- a key parameter that determines the applicability of materials for spintronics and spin-based quantum information applications -- has been extensively measured in halide perovskites, but not yet assessed from first-principles calculations. Here, we leverage our recently-developed \emph{ab initio} density-matrix dynamics framework to compute the spin relaxation time ($T_{1}$) and ensemble spin dephasing time ($T_{2}^{*}$) in a prototype halide perovskite, namely CsPbBr$_{3}$ with self-consistent spin-orbit coupling (SOC) and quantum descriptions of the electron scattering processes. We also implement the Land\'e $g$-factor for solids from first principles and take it into account in our dynamics, which is required to accurately capture spin dephasing at external magnetic fields. We thereby predict intrinsic spin lifetimes as an upper bound for experiments, identify the dominant spin relaxation pathways, and evaluate the dependence on temperature, external fields, carrier density,and impurities. Importantly, we find that the Fr{\"o}hlich interaction that dominates carrier relaxation contributes negligibly to spin relaxation, consistent with the spin-conserving nature of this interaction. We investigated the effect of spin-orbit field with inversion asymmetry on spin lifetime, and we demonstrated from our calculation, persistent spin helix can enhance spin lifetime when the spin-split is large, but it can not be realized by Rashba SOC. Our theoretical approach may lead to new strategies to optimize spin and carrier transport properties in spintronics and quantum information applications.