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Magnetic transition metal dichalcogenide (TMD) films have recently emerged aspromising candidates to host novel magnetic phases relevant to next-generationspintronic devices. However, systematic control of the magnetizationorientation, or anisotropy, and its thermal stability, characterized by Curietemperature (Tc) remains to be achieved in such films. Here we presentself-intercalated epitaxial Cr1+{\delta}Te2 films as a platform for achievingsystematic/smooth magnetic tailoring in TMD films. Using a molecular beamepitaxy (MBE) based technique, we have realized epitaxial Cr1+{\delta}Te2 filmswith smoothly tunable over a wide range (0.33-0.82), while maintainingNiAs-type crystal structure. With increasing {\delta}, we found monotonicenhancement of Tc from 160 to 350 K, and the rotation of magnetic anisotropyfrom out-of-plane to in-plane easy axis configuration for fixed film thickness.Contributions from conventional dipolar and orbital moment terms areinsufficient to explain the observed evolution of magnetic behavior with{\delta}. Instead, ab initio calculations suggest that the emergence ofantiferromagnetic interactions with {\delta}, and its interplay withconventional ferromagnetism, may play a key role in the observed trends. To ourknowledge, this constitutes the first demonstration of tunable Tc and magneticanisotropy across room temperature in TMD films, and paves the way forengineering novel magnetic phases for spintronic applications.

Tailoring Magnetism in Self-intercalated Cr1+{\delta}Te2 Epitaxial Films