Interlayer ferromagnetism and insulator-metal transition in element-doped CrI3 thin films

Abstract: The exploration of magnetism in two-dimensional layered materials has attracted extensive research interest. For the monoclinic phase CrI3 with interlayer antiferromagnetism, finding a static and robust way of realizing the intrinsic interlayer ferromagnetic coupling is desirable. In this Letter, we study the electronic structure and magnetic properties of the nonmagnetic element (e.g., O, S, Se, N, P, As and C) doped bi- and triple-layer CrI3 systems via first-principles calculations. Our results demonstrate that O, P, S, As, and Se doped CrI3 bilayer can realize interlayer ferromagnetism. Further analysis shows that the interlayer ferromagnetic coupling in the doped few-layer CrI3 is closely related to the formation of localized spin-polarized state. This finding indicates that insulated interlayer ferromagnetism can be realized at high doping concentration (larger than 8.33%). When the doping concentration is less than 8.33%, but larger than 2.08%, an insulator-metal phase transition can occur since the localized spin-polarized states percolate to form contiguous grids in few-layer CrI3.