Robust Two-Dimensional Ferromagnetism in Cr5Te8/CrTe2 Heterostructure with Curie Temperature above 400 K

The discovery of ferromagnetism in two-dimensional (2D) van der Waals crystals has generated widespread interest. The seeking of robust 2D ferromagnets with high Curie temperature (T_c) is vitally important for next-generation spintronic devices. However, owing to the enhanced spin fluctuation and weak exchange interaction upon the reduced dimensionalities, the exploring of robust 2D ferromagnets with T_c > 300 K is highly demanded but remains challenging. In this work, we fabricated air-stable 2D Cr₅Te₈/CrTe₂ vertical heterojunctions with T_c above 400 K by the chemical vapor deposition method. Transmission electron microscopy demonstrates a high-quality-crystalline epitaxial structure between tri-Cr₅Te₈ and 1T-CrTe₂ with striped moiré patterns and a superior ambient stability over six months. A built-in dual-axis strain together with strong interfacial coupling cooperatively leads to a record-high T_c for the Cr_xTe_y family. A temperature-dependent spin-flip process induces the easy axis of magnetization to rotate from the out-of-plane to the in-plane direction, indicating a phase-dependent proximity coupling effect, rationally interpreted by first-principles calculations of the magnetic anisotropy of a tri-Cr₅Te₈ and 1T-CrTe₂ monolayer. Our results provide a material realization of effectively enhancing the transition temperature of 2D ferromagnetism and manipulating the spin-flip of the easy axis, which will facilitate future spintronic applications.