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The transition metal selenides M_1+ySe₂(M = V, Ti) have intriguing quantum properties, which make them target materials for controlling properties by thinning them to the ultrathin limit. An appropriate approach for the synthesis of such ultrathin films is by molecular beam epitaxy. Here, it is shown that such synthesized V‐ and Ti‐Se₂films can undergo a compositional change by vacuum annealing. Combined scanning tunneling and photoemission spectroscopy is used to determine compositional and structural changes of ultrathin films as a function of annealing temperature. Loss of selenium from the film is accompanied by a morphology change of monolayer height islands to predominantly bilayer height. In addition, crystal periodicity and atomic structure changes are observed. These changes are consistent with a transition from a layered transition metal dichalcogenide (TMDC) to ordered intercalation compounds with V or Ti intercalated in between two layers of their respective TMDCs. These observations may clear up misconception of the nature of previously reported high‐temperature grown transition metal selenides. More significantly, the demonstrated control of the formation of intercalation compounds is a key step toward modifying properties in van der Waals systems and toward expanding material systems for van der Waals heterostructures.

Post‐synthesis doping of 2D materials is demonstrated by incorporation of vapor‐deposited transition metals into a MoTe₂lattice. Using this approach, vanadium doping of 2H‐MoTe₂produces a 2D ferromagnetic semiconductor with a Curie temperature above room temperature (RT). Surprisingly, ferromagnetic properties can be induced with very low vanadium concentrations, down to ≈0.2%. The vanadium species introduced at RT are metastable, and annealing to above ≈500 K results in the formation of a thermodynamically favored impurity configuration that, however, exhibits reduced ferromagnetic properties. Doping with titanium, instead of vanadium, shows a similar incorporation behavior, but no ferromagnetism is induced in MoTe₂. This indicates that the type of impurities in addition to their atomic configuration is responsible for the induced magnetism. The interpretation of the experimental results is consistent with ab initio calculations, which confirm that the proposed vanadium impurity configurations exhibit magnetic moments, in contrast to the same configurations with titanium impurities. This study illustrates the possibility to induce ferromagnetic properties in layered van der Waals semiconductors by controlled magnetic impurity doping and thus to add magnetic functionalities to 2D materials.