Giant Spin Splitting and its Origin in Methylhydrazinium Lead Halide Perovskites

Abstract

Spin splitting, or removal of spin degeneracy in the electronic energy band/level is often a measure of spin-orbit coupling strength and a way to manipulate spin degrees of freedom. We use first-principles simulations to predict giant spin splitting in methylhydrazinium lead halide (MHyPbX${}_3$, MHy = CH${}_3$NH${}_2$NH${}_2$, X = Br and Cl) hybrid organic-inorganic perovskites. The values can reach up to 408.0~meV at zero Kelvin and 281.6~meV at room temperature. The origin of the effect is traced to the large distortion of PbX${}_3$ framework, driven primarily by Pb ions in the ferroelectric ${\Gamma }^{3-}$ mode. The Pb displacements consist of combination of polar and antipolar arrangements and result in up to 39.2~meV/atom enhancement of the spin-orbit coupling energy in the polar phase of the materials. The spin-orbit coupling gives origin to highly persistent spin textures in MHyPbX${}_3$, which are desirable for applications in spintronics and quantum computing. Our findings reveal an additional functionality for hybrid organic-inorganic perovskite and open a way for the design of more materials with giant spin splitting.