Multiple modulation of magnetism in two-dimensional FeCl2/In2Se3 van der Waals heterostructure

The effective modulation of magnetism for two-dimensional (2D) materials not only has potential applications in nanoscale spintronic devices but also has urgent demands in modern industries. In this work, we report the discovery of ferroelectrically (FE) tunable orbital reconstruction in FeCl2/In2Se3 2D van der Waals (vdWs) heterostructures (HSs), which leads to a transition from ferromagnetic (FM) order to ferrimagnetic order (intra-layer magnetic coupling is AFM3 arrangement). The reversible FE polarization not only enables the easy magnetization axis to be tuned from the out-of-plane to in-plane direction but also reduces the net magnetization strength from 31.87 to −0.18 μB/f.u. Based on the charge density differences and the density of states analysis, the preference of FM and AFM3 arrangement can be reasonably explained by the Goodenough–Kanamori–Anderson rule. The ferroelectric switching enables nonvolatile electric control of magnetic order and anisotropy, offering significant potential for high-efficiency nanodevices and nonvolatile information storage. Moreover, modulation of magnetism (magnetic moment from −0.18 to 0.18 μB/f.u.) can also be achieved through interlayer sliding in the −P case, providing a way to control magnetism in 2D vdWs HSs.