Unconventional Spintronics from Chiral Perovskites

Abstract Spintronic devices typically employ heterostructures with ferromagnets which break time‐reversal symmetry and have non‐vanishing magnetization. With the growing class of materials that support spin‐polarized carriers, current, and excitations, it is possible to envision emerging spintronic applications that are not limited to magnetoresistance. Here, chiral perovskites with no net magnetization are considered, where the space‐inversion and mirror symmetries are broken to induce chiral structure. The known importance of these perovskites is further expanded by the demonstration of the chiral‐induced spin selectivity (CISS). However, the generation of the spin‐polarized carriers across the interface with these chiral perovskites remains to be fully understood. These first‐principles studies for 2D PbBr ₄ ‐based chiral perovskites provide their electronic structure and an orbital‐based symmetry analysis, which allows to establish an effective Hamiltonian to elucidate the underlying origin of their chirality. The same analysis is used for the Edelstein effect, responsible for electrical generation of the nonequilibrium spin polarization in many materials, which in chiral perovskites can be a mechanism contributing to CISS. Furthermore, by examining optical properties of chiral perovskites and the opportunity to use them to realize tunable altermagnets, another class of zero‐magnetization spintronic materials, a versatile materials platform is put forth for unconventional spintronics.