Spin-Driven Ferroelectricity in Two-Dimensional Magnetic Heterostructures.

Achieving magnetic control of ferroelectricity or electric control of magnetism is usually challenging in material systems as their magnetism and ferroelectricity have distinct fundamental origins and are subject to different symmetry constraints. However, such control has significant promise for a wide range of device applications. In this work, we employ first-principles density functional theory calculations to demonstrate the emergence of spin-driven ferroelectricity in a vertically stacked two-dimensional (2D) van der Waals magnetic heterostructure, formed by two ferromagnetic (FM) CrBr layers separated by an antiferromagnetic (AFM) MnPSe layer, delicately designed to be structurally inversion symmetric but magnetically asymmetric. The spin-induced out-of-plane electric polarization of the entire heterostructure can be reversibly controlled by an external magnetic field. We further validate the effectiveness of this design strategy in several other lattice-matched FM/AFM/FM heterostructures, thereby providing a novel family of multiferroic systems based on 2D materials.