Microscopic origin of magnetoferroelectricity in monolayer NiBr$_{2}$ and NiI$_{2}$

Abstract

We investigate the magnetoelectric properties of the monolayer NiX$_{2}$ (X = Br, I) through first-principles calculations. Our calculations predict that the NiBr$_{2}$ monolayer exhibits a cycloidal magnetic ground state. For the NiI$_{2}$ monolayer, a proper-screw helical magnetic ground state with modulation vector \(\boldsymbol{Q} = (q, 0, 0)\) is adopted, approximated based on experimental observations. The electric polarization in NiBr$_{2}$ shows a linear dependence on the spin-orbit coupling strength \(\lambda_{\text{SOC}}\), which can be adequately described by the generalized Katsura-Nagaosa-Balatsky (gKNB) model, considering contributions from up to the third nearest-neighbor spin pairs. In contrast, the electric polarization in NiI$_{2}$ exhibits a distinct dependence on \(q\) and \(\lambda_{\text{SOC}}\), which cannot be fully explained by the gKNB mechanism alone. To address this, the \(p\)-\(d\) hybridization mechanism is extended to NiI$_{2}$ to explain the observed behavior. The respective contributions from the \(p\)-\(d\) hybridization and the gKNB mechanism in NiI$_{2}$ are then quantitatively evaluated. Overall, our work elucidates the microscopic mechanisms underlying multiferroicity in NiBr$_{2}$ and NiI$_{2}$ monolayers, with the conclusions readily applicable to their bulk forms.