Electrically-Tunable High Curie Temperature Two-Dimensional Ferromagnetism in Van der Waals Layered Crystals

Abstract: Identifying intrinsic low-dimensional ferromagnets with high transition temperature and electrically tunable magnetism is crucial for the development of miniaturized spintronics and magnetoelectrics. Recently long-range 2D ferromagnetism was observed in van der Waals crystals CrI$_3$ and Cr$_2$Ge$_2$Te$_6$, however their Curie temperature is significantly lowered when reducing down to monolayer/few layers. Herein, using renormalized spin-wave theory and first-principles electronic structure theory, we present a theoretical study of electrically tunable 2D ferromagnetism in van der Waals layered CrSBr and CrSeBr semiconductors with high Curie temperature of ~150K and sizable band gap. High transition temperature is attributed to strong anion-mediated superexchange interaction and a sizable spin-wave excitation gap due to large exchange and single-ion anisotropy. Remarkably, hole and electron doping can switch magnetization easy axis from in-plane to out-of-plane direction. These unique characteristics establish monolayer CrSBr and CrSeBr as promising platform for realizing 2D spintronics and magnetoelectrics such as 2D spin field effect transistor.