Above-Room-Temperature Ferromagnetism Regulation in Two-Dimensional Heterostructures by van der Waals Interfacial Magnetochemistry.

Most methods for regulating physical and chemical properties of materials involve the breaking and formation of chemical bonds, which inevitably change local structures. Two-dimensional (2D) ferromagnets are critical for spintronic memory and quantum devices, but most of them maintain ferromagnetism at low temperature, and multiaspect control of 2D ferromagnetism at room temperature or above is still missing. Here, we report a nondestructive, van der Waals (vdW) interfacial magnetochemistry strategy for above-room-temperature, multiaspect 2D ferromagnetism regulation. By vdW coupling nonmagnetic MoS, WSe, or BiSbTeSe with 2D vdW ferromagnet FeGaTe, the Curie temperature is enhanced up to 400 K, best for 2D ferromagnets, with 26.8% tuning of room-temperature perpendicular magnetic anisotropy and an unconventional anomalous Hall effect up to 340 K. These phenomena originate from changes in magnetic exchange interactions and magnetic anisotropy energy by interfacial charge transfer and spin-orbit coupling. This work opens a pathway for engineering multifunctional 2D heterostructures by vdW interfacial magnetochemistry.