Magnetoelectric Coupling in Multiferroic Bilayer VS2

Based on the first-principles prediction, we report the magnetoelectric coupling effect in two-dimensional multiferroic hilayer VS2. The ground-state 3R-type stacking breaks space inversion symmetry, therefore introducing a spontaneous polarization perpendicular to the layer plane. We further reveal that the out-of-plane ferroelectric polarization of bilayer VS2 can be reversed upon interlayer sliding of an in-plane translation. Each VS2 layer has a ferromagnetic state with an opposite magnetic moment between two antiferromagnetically ordered layers. We found that ferroelectricity and antiferromagnetism can be coupled together by a ferrovalley in bilayer VS2 to realize electronic control of magnetism. Remarkably, a net magnetic moment is generated by reducing the interlayer distance, and an electric field is able to achieve linear and second-order nonlinear magnetoelectric coupling in bilayer VS2.