Mechanical, Electronic, and Magnetic Properties of NiX2 (X = Cl, Br, I) Layers

Since the recent experimental discovery of the CrI3 and CrGeTe3 monolayers, van der Waals (vdW) layered transition metal compounds have been recognized as promising candidates to realize 2D ferromagnetic (FM) semiconductors. However, until now, only limited compounds have been proposed to be ferromagnetic semiconductors. Here, on the basis of first-principles calculations, we report that the monolayer, Janus monolayer, and bilayer of NiX2 (X = Cl, Br, I) are intrinsic 2D FM semiconductors. Our results show that exfoliation energy of the NiX2 monolayer is smaller than that of graphene, and all studied NiX2 layers show semiconducting band gaps. The predicted Curie temperature values for NiX2 (X = Cl, Br, I) monolayers ranged from 120 to 170 K with Monte Carlo simulations. For the Janus monolayer, we found that the spin interaction shows a very strong magnetoelectric coupling under an external electric field. Furthermore, for the bilayer of NiX2, our results show that the interlayer coupling is quite weak, indicating the possibility of tuning the magnetic coupling through external manipulations.