Screening and Design of Novel 2D Ferromagnetic Materials with High Curie Temperature above Room Temperature

Two-dimensional (2D) intrinsic ferromagnets with high Curie temperature ( T C ) are desirable for spintronic applications. Using systematic first-principles calculations, we investigate the electronic and magnetic properties of 22 monolayer 2D materials with layered bulk phases. From these candidates, we screen out five ferromagnetic monolayer materials belonging to three types of structures: type i (ScCl, YCl, LaCl), type ii (LaBr 2 ), and type iii (CrSBr). Type i is a kind of metallic ferromagnetic material, whereas LaBr 2 and CrSBr of type ii and iii are small-bandgap ferromagnetic semiconductors with T C near room temperature. Moreover, the ferromagnetic CrSBr monolayer possesses a large magnetic moment of ∼3 μ B per Cr atom, originating from its distorted octahedron coordination. The robust ferromagnetism of the CrSBr monolayer is ascribed to the halogen-mediated (Cr–Br–Cr) and chalcogen-mediated (Cr–S–Cr) superexchange interactions; then, an isoelectronic substitution strategy is proposed to tailor the magnetic coupling strength. Hence, monolayer structures of CrSI, CrSCl, and CrSeBr with notably enhanced Curie temperature up to 500 K as well as favorable formation energy are designed. The moderate interlayer binding energy and high T C make these monolayer ferromagnetic materials feasible for experimental synthesis and attractive as 2D spintronic devices.