Artificial Multiferroics and Enhanced Magnetoelectric Effect in van der Waals Heterostructures

Abstract: Multiferroic materials with coupled ferroelectric and ferromagnetic properties are important for multifunctional devices due to their potential ability of controlling magnetism via electric field, and vice versa. The recent discoveries of two-dimensional ferromagnetic and ferroelectric materials have ignited tremendous research interest and aroused hope to search for two-dimensional multiferroics. However, intrinsic two-dimensional multiferroic materials and, particularly, those with strong magnetoelectric couplings are still rare to date. In this paper, using first-principles simulations, we propose artificial two-dimensional multiferroics via a van der Waals heterostructure formed by ferromagnetic bilayer chromium triiodide (CrI3) and ferroelectric monolayer Sc2CO2. In addition to the coexistence of ferromagnetism and ferroelectricity, our calculations show that, by switching the electric polarization of Sc2CO2, we can tune the interlayer magnetic couplings of bilayer CrI3 between ferromagnetic and antiferromagnetic states. We further reveal that such a strong magnetoelectric effect is from a dramatic change of the band alignment induced by the strong build-in electric polarization in Sc2CO2 and the subsequent change of the interlayer magnetic coupling of bilayer CrI3. These artificial multiferroics and enhanced magnetoelectric effect give rise to realizing multifunctional nanoelectronics by van der Waals heterostructures.