Two-dimensional and van der Waals ferromagnets are ideal platform to study low-dimensional magnetism and proximity effects in van der Waals heterostructures. Their ultimate two-dimensional character also offers the opportunity to easily adjust their magnetic properties using strain or electric fields. Among 2D ferromagnets, the Te2 compounds with x = 0–1 are very promising because their magnetic properties depend on the amount of self-intercalated Cr atoms between pure CrTe2 layers and the Curie temperature ( ) can reach room temperature for certain compositions. Here, we investigate the evolution of the composition as well as the structural and magnetic properties of thin Cr1.33Te2 (Cr2Te3) films epitaxially grown on graphene upon annealing. We observe a transition above 450 °C from the Cr1.33Te2 phase with perpendicular magnetic anisotropy and a of 180 K to a composition close to Te2 with in-plane magnetic anisotropy and a of 240–250 K. This phase remains stable up to 650 °C above which a pure Cr film starts to form. This work demonstrates the complex interplay between intercalated Cr, lattice parameters, and magnetic properties in Te2 compounds.
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