Hole-Doping-Induced Perpendicular Magnetic Anisotropy and High Curie Temperature in a CrSX (X = Cl, Br, I) Semiconductor Monolayer

A large perpendicular magnetic anisotropy and a high Curie temperature (TC) are crucial for the application of two-dimensional (2D) intrinsic ferromagnets to spintronic devices. Here, we investigated the electronic and magnetic properties of carrier-doped Van der Waals layered CrSX (X = Cl, Br, I) ferromagnets using first-principles calculations. It was found that hole doping can increase the magnitude of the magnetic anisotropy energy (MAE) and change the orientation of the easy magnetization axis at small doping amounts of 2.37 × 1013, 3.98 × 1012, and 3.33 × 1012/cm2 for CrSCl, CrSBr, and CrSI monolayers, respectively. The maximum values of the MAE reach 57, 133, and 1597 μeV/u.c. for the critical hole-doped CrSCl, CrSBr, and CrSI with spin orientation along the (001) direction, respectively. Furthermore, the Fermi energy level of lightly hole-doped CrSX (X = Cl, Br, I) moves into the spin-up valence band, leading to the CrSX (X = Cl, Br, I) magnetic semiconductor monolayer becoming first a half-metal and then a metal. In addition, the TC can also be increased up to 305, 317, and 345 K for CrSCl, CrSBr, and CrSI monolayers at doping amounts of 5.94 × 1014, 5.78 × 1014, and 5.55 × 1014/cm2, respectively. These properties suggest that the hole-doping process can render 2D CrSX (X = Cl, Br, I) monolayers remarkable materials for application to electrically controlled spintronic devices.