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Ultrathin transition metal dichalcogenides (TMDCs) of Mo and W show greatpotential for digital electronics and optoelectronic applications. Whereasearly studies were limited to mechanically exfoliated flakes, the large-areasynthesis of 2D TMDCs has now been realized by chemical vapor deposition (CVD)based on a sulfurization reaction. Since then, the optoelectronic properties ofCVD grown monolayer MoS$_{2}$ have been heavily investigated, but the influenceof stoichiometry on the electrical and optical properties has been largelyoverlooked. Here we systematically vary the stoichiometry of monolayerMoS$_{2}$ during CVD via controlled sulfurization and investigate theassociated changes in photoluminescence and electrical properties. X-rayphotoelectron spectroscopy is employed to measure relative variations instoichiometry and the persistence of MoO$_{x}$ species. As MoS$_{2-{\delta}}$is reduced (increasing {\delta}), the field-effect mobility of monolayertransistors increases while the photoluminescence yield becomes non-uniform.Devices fabricated from monolayers with the lowest sulfur content havenegligible hysteresis and a threshold voltage of ~0 V. We conclude that theelectrical and optical properties of monolayer MoS$_{2}$ crystals can be tunedvia stoichiometry engineering to meet the requirements of various applications.

Influence of Stoichiometry on the Optical and Electrical Properties of Chemical Vapor Deposition Derived MoS$_{2}$