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Abstract Edges and point defects in layered dichalcogenides are important for tuning their electronic and magnetic properties. By combining scanning tunneling microscopy (STM) with density functional theory (DFT), the electronic structure of edges and point defects in 2D‐PtSe₂are investigated where the 1.8 eV bandgap of monolayer PtSe₂facilitates the detailed characterization of defect‐induced gap states by STM. The stoichiometric zigzag edge terminations are found to be energetically favored. STM and DFT show that these edges exhibit metallic 1D states with spin polarized bands. Various native point defects in PtSe₂are also characterized by STM. A comparison of the experiment with simulated images enables identification of Se‐vacancies, Pt‐vacancies, and Se‐antisites as the dominant defects in PtSe₂. In contrast to Se‐ or Pt‐vacancies, the Se‐antisites are almost devoid of gap states. Pt‐vacancies exhibit defect induced states that are spin polarized, emphasizing their importance for inducing magnetism in PtSe₂. The atomic‐scale insights into defect‐induced electronic states in monolayer PtSe₂provide the fundamental underpinning for defect engineering of PtSe₂‐monolayers and the newly identified spin‐polarized edge states offer prospects for engineering magnetic properties in PtSe₂nanoribbons. 

Abstract 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.