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Engineering electronic bandgaps is crucial for applications in information technology, sensing, and renewable energy. Transition metal dichalcogenides (TMDCs) offer a versatile platform for bandgap modulation through alloying, doping, and heterostructure formation. Here, the synthesis of a 2D Mo_xW_1‐xS₂graded alloy is reported, featuring a Mo‐rich center that transitions to W‐rich edges, achieving a tunable bandgap of 1.85 to 1.95 eV when moving from the center to the edge of the flake. Aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy showed the presence of sulfur monovacancy, V_S, whose concentration varied across the graded Mo_xW_1‐xS₂layer as a function of Mo content with the highest value in the Mo‐rich center region. Optical spectroscopy measurements supported by ab initio calculations reveal a doublet electronic state of V_S, which is split due to the spin‐orbit interaction, with energy levels close to the conduction band or deep in the bandgap depending on whether the vacancy is surrounded by W atoms or Mo atoms. This unique electronic configuration of V_Sin the alloy gave rise to four spin‐allowed optical transitions between the V_Slevels and the valence bands. The study demonstrates the potential of defect and optical engineering in 2D monolayers for advanced device applications.

The capacity to manipulate magnetization in 2D dilute magnetic semiconductors (2D‐DMSs) using light, specifically in magnetically doped transition metal dichalcogenide (TMD) monolayers (M‐dopedTX₂, whereM = V, Fe, and Cr;T = W, Mo;X = S, Se, and Te), may lead to innovative applications in spintronics, spin‐caloritronics, valleytronics, and quantum computation. This Perspective paper explores the mediation of magnetization by light under ambient conditions in 2D‐TMD DMSs and heterostructures. By combining magneto‐LC resonance (MLCR) experiments with density functional theory (DFT) calculations, we show that the magnetization can be enhanced using light in V‐doped TMD monolayers (e.g., V‐WS₂, V‐WSe₂). This phenomenon is attributed to excess holes in the conduction and valence bands, and carriers trapped in magnetic doping states, mediating the magnetization of the semiconducting layer. In 2D‐TMD heterostructures (VSe₂/WS₂, VSe₂/MoS₂), the significance of proximity, charge‐transfer, and confinement effects in amplifying light‐mediated magnetism is demonstrated. We attributed this to photon absorption at the TMD layer that generates electron–hole pairs mediating the magnetization of the heterostructure. These findings will encourage further research in the field of 2D magnetism and establish a novel design of 2D‐TMDs and heterostructures with optically tunable magnetic functionalities, paving the way for next‐generation magneto‐optic nanodevices.

The field of photovoltaics is revolutionized in recent years by the development of two–dimensional (2D) type‐II heterostructures. These heterostructures are made up of two different materials with different electronic properties, which allows for the capture of a broader spectrum of solar energy than traditional photovoltaic devices. In this study, the potential of vanadium (V)‐doped WS₂is investigated, hereafter labeled V‐WS₂, in combination with air‐stable Bi₂O₂Se for use in high‐performance photovoltaic devices. Various techniques are used to confirm the charge transfer of these heterostructures, including photoluminescence (PL) and Raman spectroscopy, along with Kelvin probe force microscopy (KPFM). The results show that the PL is quenched by 40%, 95%, and 97% for WS₂/Bi₂O₂Se, 0.4 at.% V‐WS₂/Bi₂O₂Se, and 2 at.% V‐WS₂/Bi₂O₂Se, respectively, indicating a superior charge transfer in V‐WS₂/Bi₂O₂Se compared to pristine WS₂/Bi₂O₂Se. The exciton binding energies for WS₂/Bi₂O₂Se, 0.4 at.% V‐WS₂/Bi₂O₂Se and 2 at.% V‐WS₂/Bi₂O₂Se heterostructures are estimated to be ≈130, 100, and 80 meV, respectively, which is much lower than that for monolayer WS₂. These findings confirm that by incorporating V‐doped WS₂, charge transfer in WS₂/Bi₂O₂Se heterostructures can be tuned, providing a novel light‐harvesting technique for the development of the next generation of photovoltaic devices based on V‐doped transition metal dichalcogenides (TMDCs)/Bi₂O₂Se.