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The low evaporation temperature and carcinogen classification of commonly used molybdenum trioxide (MoO 3 ) precursor render it unsuitable for the safe and practical synthesis of molybdenum disulfide (MoS 2 ). Furthermore, as evidenced by several experimental findings, the associated reaction constitutes a multistep process prone to the formation of uncontrolled amounts of intermediate MoS 2-y O y phase mixed with the MoS 2 crystals. Here, molybdenum dioxide (MoO 2 ), a chemically more stable and safer oxide than MoO 3 , was utilized to successfully grow cm-scale continuous films of monolayer MoS 2 . A high-resolution optical image stitching approach and Raman line mapping were used to confirm the composition and homogeneity of the material grown across the substrate. A detailed examination of the surface morphology of the continuous film revealed that, as the gas flow rate increased by an order of magnitude, the grain-boundary separation dramatically reduced, implying a transition from a kinetically to thermodynamically controlled growth. Importantly, the single-step vapor-phase sulfurization (VPS) reaction of MoO 2 was shown to suppress intermediate state formations for a wide range of experimental parameters investigated and is completely absent, provided that the global S:Mo loading ratio is set higher than the stoichiometric ratio of 3:1 required by the VPS reaction.

CVD Synthesis of Intermediate State-Free, Large-Area and Continuous MoS2 via Single-Step Vapor-Phase Sulfurization of MoO2 Precursor