Out-of-plane polarization and topological magnetic vortices in multiferroic CrPSe3

Two-dimensional multiferroic materials are ideal systems for exploring new coupling mechanisms between different ferroic orders and producing novel quantum phenomena with potential applications. We employ first-principles density functional theory calculations to discover intrinsic ferroelectric and antiferroelectric phases of CrPSe3, which show ferromagnetic order and compete with the centrosymmetric phase with an antiferromagnetic order. Our analysis shows that the electrical dipoles of such type-I multiferroic phases come from the out-of-plane displacements of phosphorus ions due to the stereochemically active lone pairs. The coupling between polar and magnetic orders creates the opportunity for tuning the magnetic ground state by switching from the centrosymmetric to the ferroelectric phase using an out-of-plane electric field. In ferroelectric and antiferroelectric phases, the combination of easy-plane anisotropy and Dzyaloshinskii-Moriya interactions indicates that they can host topological magnetic vortices such as meron pairs.