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Sliding ferroelectricity is widely existed in van der Waals (vdW)two-dimensional (2D) multilayers, exhibiting great potential on low-dissipationnon-volatile memories. However, in a vdW heterostructure, interlayer slidingusually fails to reverse or distinctly change the electric polarization, whichmakes the electrical control difficult in practice. Here we propose that in avdW magnetic system, the interlayer spin interaction could provide an extradegree-of-freedom to remarkably tune the electric polarization. Combiningtight-binding model analysis and first-principles calculations, we show that inthe CrI3/MnSe2 and other vdW magnetic heterobilayers, the switching of theinterlayer magnetic order can greatly change, even reverse the off-planeelectronic polarization. Furthermore, interlayer sliding causes a non-volatileswitching of the magnetic order and, thus, reverses the electric polarization,suggesting a non-volatile magnetoelectric coupling effect. These findings willsignificantly advances the development of 2D ferroelectrics and multiferroicsfor spintronic applications.

Interlayer-spin-interaction-driven Sliding Ferroelectricity in a van der Waals Magnetic Heterobilayer