Hole doping as an efficient route to increase the Curie temperature in monolayer CrI3

Abstract Two-dimensional van der Waals (vdW) magnets offer unprecedented opportunities to control magnetism at the atomic scale. Through charge carrier doping---realized by electrostatic gating, intercalation/adsorption, or interfacial charge transfer---one can efficiently tune exchange interactions and spin-orbit-induced effects in these systems. In this work, through a multi-scale theoretical framework combining density functional theory, spin Hamiltonian modeling, and Wannier-function analysis, we choose monolayer CrI 3 to unravel how carrier doping affects the isotropic as well as anisotropic exchange interactions in this prototypical vdW ferromagnet. The remarkable efficiency of hole doping in enhancing ferromagnetic exchange and magnetic anisotropy found in our study was explained through orbital-resolved analysis. Crucially, we demonstrated that unlike the undoped system -- where isotropic exchange interactions govern magnetic long-range order -- the hole-doped CrI 3 exhibits anisotropic terms comparable in magnitude to isotropic ones. In particular, the magnetic anisotropy energy increases from 0.65 meV in undoped to 4.43 meV in strongly hole-doped CrI 3 , with the second-neighbor Dzyaloshinskii-Moriya interaction increasing from 0.12 meV to 2.01 meV. Finally, we show that a high concentration of holes can increase the Curie temperature from 56 K all the way up to 228 K. This work advances our understanding of doping-controlled magnetism in semiconducting 2D materials, demonstrating how anisotropy engineering can stabilize high-temperature magnetic order.