Magnetic Anisotropy Control with Curie Temperature above 400 K in a van der Waals Ferromagnet for Spintronic Device

Abstract The technological appeal of van der Waals ferromagnetic materials is the ability to control magnetism under external fields with desired thickness toward novel spintronic applications. For practically useful devices, ferromagnetism above room temperature or tunable magnetic anisotropy is highly demanded but remains challenging. To date, only a few layered materials exhibit unambiguous ferromagnetic ordering at room temperature via gating techniques or interface engineering. Here, it is demonstrated that the magnetic anisotropy control and dramatic modulation of Curie temperature (T_c) up to 400 K are realized in layered Fe₅GeTe₂ via the high‐pressure diamond‐anvil‐cell technique. Magnetic phases manifesting with in‐plane anisotropic, out‐of‐plane anisotropic and nearly isotropic magnetic states can be tuned in a controllable way, depicted by the phase diagram with a maximum T_c up to 360 K. Remarkably, the T_c can be gradually enhanced to above 400 K owing to the Fermi surface evolution during a pressure loading–deloading process. Such an observation sheds light on the understanding and control of emergent magnetic states in practical spintronic applications.