Exploitable Magnetic Anisotropy of the Two-Dimensional Magnet CrI3

Magnetic anisotropy often plays a central role in various static and dynamic properties of magnetic materials. In particular, for two-dimensional (2D) van der Waals materials, as inferred from the Mermin–Wagner theorem, it is an essential prerequisite for stabilizing ferromagnetic order. In this work, we carry out first-principles calculations for a CrI 3 monolayer and investigate how its magnetic anisotropy is interrelated to adjustable parameters governing the underlying electronic structure. We explore various routes for controlled manipulation of magnetic anisotropy: chemical adsorption, substitutional doping, optical excitation, and charge transfer through a heterostructure. In particular, the vertical stacking of CrI 3 and graphene is noteworthy in regard to controlling magnetic anisotropy: the spin anisotropy axis is switchable between the out-of-plane and in-plane directions, which is accompanied by a variation in the anisotropy energy of up to 500%. Our results show the possibility that dynamic control of the anisotropy of the 2D magnet CrI 3 may enable the development of an advanced spintronic device with enhanced energy efficiency and high operation speed.