Nonvolatile ferroelectric manipulation of magnetoelectric coupling and band alignment in two-dimensional CrI3/In2Se3 multiferroic van der Waals heterostructures

The coexistence of magnetic and ferroelectric properties in two-dimensional (2D) van der Waals (vdW) multiferroic heterostructures have attracted increasing interest in the development of multifunctional devices. Here, we report a new strategy to tune the magnetic ordering and electronic properties of 2D CrI₃/In₂Se₃ multiferroic heterostructures by the ferroelectric polarization based on the density-functional theory calculations. Our results demonstrate that the upward polarization state contributes to the enhancement of ferromagnetic coupling and Curie temperature of CrI₃ layer in the heterostructures. Moreover, the reverse of ferroelectric polarization can drive the transition from the ferromagnetic coupling to antiferromagnetic one in the heterostructures with a bilayer CrI₃, while the intralayer magnetic ordering is still ferromagnetic. Moreover, the ferroelectric polarization of In₂Se₃ layer creates a non-volatile build-in electric field that can modulate the band alignment and carrier spatial distribution. These findings suggest a large potential of 2D multiferroic heterostructures in data storage and spintronics devices.