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Two-dimensional dilute magnetic semiconductors has been recently reported insemiconducting transition metal dichalcogenides by the introduction ofspin-polarized transition metal atoms as dopants. This is the case ofvanadium-doped WS$_2$ and WSe$_2$ monolayers, which exhibits a ferromagneticordering even above room temperature. However, a broadband characterization oftheir electronic band structure and its dependence on vanadium concentration isstill lacking. Therefore, here we perform power-dependent photoluminescence,resonant four-wave mixing, and differential reflectance spectroscopy to studythe optical transitions close to the A exciton energy of vanadium-doped WS$_2$monolayers with distinct concentrations. Instead of a single A exciton peak,vanadium-doped samples exhibit two photoluminescence peaks associated withtransitions to occupied and unoccupied bands. Moreover, resonant Ramanspectroscopy and resonant second-harmonic generation measurements revealed ablueshift in the B exciton but no energy change in the C exciton as vanadium isintroduced in the monolayers. Density functional theory calculations showedthat the band structure is sensitive to the Hubbard $U$ correction forvanadium and several scenarios are proposed to explain the twophotoluminescence peaks around the A exciton energy region. Our work providesthe first broadband optical characterization of these two-dimensional dilutemagnetic semiconductors, shedding light on the novel electronic features ofWS$_{2}$ monolayers which are tunable by the vanadium concentration.

Effects of Vanadium Doping on the Optical Response and Electronic Structure of WS$_{2}$ Monolayers