Ferroelectric Control of Spin Textures in Layered Hybrid Perovskites

Abstract

Hybrid organic--inorganic perovskites with broken inversion symmetry provide a fertile ground for uncovering coupled spin-orbit and ferroelectric phenomena. Here, we investigate the layered family (PA)$_2$CsY$_2$X$_7$ (Y = Pb, Sn; X = I, Br) using density functional theory, Berry-phase polarization analysis, and effective $\boldsymbol{k \cdot p}$ modeling. Across all four members, we find indirect bandgaps with extrema near $\Gamma$, sizable spin splittings at both band edges, and robust in-plane ferroelectric polarization that stabilizes out-of-plane persistent spin textures (PSTs). Crucially, polarization reversal switches the spin orientation, enabling electrical control of PSTs and thereby non-volatile manipulation of spin states. These results establish (PA)$_2$CsY$_2$X$_7$ as a versatile materials platform where compositional design and ferroelectric switching jointly enable spintronic functionality.