Relativistic exchange interactions in CrX3 ( X=Cl , Br, I) monolayers

Abstract

It has been predicted theoretically and indirectly confirmed experimentally that single-layer CrX$_3$ (X=Cl, Br, I) might be the prototypes of topological magnetic insulators (TMI). In this work, by using first-principles calculations combined with atomistic spin dynamics we provide a complete picture of the magnetic interactions and magnetic excitations in CrX$_3$. The focus is here on the two most important aspects for the actual realization of TMI, namely the relativistic magnetic interactions and the finite-size (edge) effects. We compute the full interaction tensor, which includes both Kitaev and Dzyaloshinskii-Moriya terms, which are considered as the most likely mechanisms for stabilizing topological magnons. First, we instigate the properties of bulk CrI$_3$ and compare the simulated magnon spectrum with the experimental data [Phys. Rev. X 8, 041028 (2018)]. Our results suggest that a large size of topological gap, seen in experiment ($\approx$ 4 meV), can not be explained by considering pair-wise spin interactions only. We identify several possible reasons for this disagreement and suggest that a pronounced magneto-elastic coupling should be expected in this class of materials. The magnetic interactions in the monolayers of CrX$_3$ are also investigated. The strength of the anisotropic interactions is shown to scale with the position of halide atom in the Periodic Table, the heavier the element the larger is the anisotropy. Comparing the magnons for the bulk and single-layer CrI$_3$, we find that the size of the topological gap becomes smaller in the latter case. Finally, we investigate finite-size effects in monolayers and demonstrate that the anisotropic couplings between Cr atoms close to the edges are much stronger than those in ideal periodic structure. This should have impact on the dynamics of the magnon edge modes in this class of materials.