Voltage-Controllable Colossal Magnetocrystalline Anisotropy In Single-Layer Transition Metal Dichalcogenides

Materials with large magnetocrystalline anisotropy and strong electric field effects are highly needed to develop new types of memory devices based on electric field control of spin orientations. Instead of using modified transition metal films, we propose that certain monolayer transition metal dichalcogenides are the ideal candidate materials for this purpose. Using density functional calculations, we show that they exhibit not only a large magnetocrystalline anisotropy (MCA), but also colossal voltage modulation under an external field. Notably, in some materials such as CrSe2 and FeSe2, where spins show a strong preference for in-plane orientation, they can be switched to an out-of-plane direction. This effect is attributed to the large band character alteration that the transition metal d states undergo around the Fermi energy due to the electric field. We further demonstrate that strain can also greatly change MCA, and can help to improve the modulation efficiency when combined with an electric field.