First-principles study of perpendicular magnetic anisotropy of CrI3/In2Se3 Van der Waals heterostructure

Two-dimensional multiferroic van der Waals (vdW) heterostructures are promising for nanoscale and multifunctional spintronic devices. Controllable perpendicular magnetic anisotropy in vdW heterostructure often plays a central role in stabilizing ferromagnetic order and lowering energy consumption. Here, we carry out first-principles calculations for CrI3/In2Se3 vdW heterostructure and investigate how its magnetic anisotropy is interrelated to the electronic structure. We show that the semiconducting nature of CrI3 is preserved but band gap decreases in monolayer-CrI3/In2Se3 and bilayer-CrI3/In2Se3 vdW heterostructures. The magnetoelectric effect of CrI3/In2Se3 vdW heterostructure enhances the magnetic moment of CrI3, but decreases the perpendicular magnetic anisotropy of CrI3. I-p orbital coupling matrix element is noteworthy in regard to the modulation of magnetic anisotropy. The MAE contribution of Cr atom slightly enhances but is still negligible by the reason of countervailing contribution of d-orbital coupling matrix element. By reversing the ferroelectric polarization of In2Se3, the easy magnetization axis of monolayer CrI3 can be switched. These results will help to understand the magnetic anisotropy of multiferroic vdW heterostructure and may enable the development of nonvolatile memory devices.