Two-dimensional (2D) transition-metal dichalcogenides (TMDCs) and their Janus derivatives have emerged as promising platforms for next-generation spintronic and quantum technologies. In this work, we present a comprehensive first-principles investigation of 155 intrinsic defect configurations in MoS2, MoSe2, WS2, and Janus MoSSe and WSSe monolayers. Our results reveal that intrinsic point defects can induce robust magnetism in WSSe without requiring transition-metal doping—an important contrast to earlier studies that focused primarily on extrinsic substitutions. We find that magnetic moments as high as 6 in MoS₂ and up to 4 in Janus TMDCs arise from symmetry breaking and the formation of localized mid-gap defect states. Furthermore, by mapping out the stability windows of vacancies, antisites, and vacancy complexes over a wide range of chemical potentials, we establish clear mechanistic connections between defect energetics and spin ordering. Importantly, several strong magnetic defects drive semiconductor-to-half-metal transitions, enabling spin-polarized electronic transport, while other configurations exhibiting weaker magnetism retain semiconducting character but with appreciably reduced bandgaps. Overall, this study provides a benchmark dataset and a defect-engineering roadmap for tailoring magnetic responses in 2D TMDCs. These insights offer actionable design strategies for realizing defect-driven spin functionality in future 2D spintronic and quantum devices.
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