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Molybdenum disulfide (MoS₂) films, which are only a single atomic layer thick, have been synthesized by chemical vapor deposition (CVD) and have gained significant attention due to their band-gap semiconducting properties. However, in order for them to be useful for the fabrication of practical devices, patterning processes that can be used to form specific MoS₂ structures must be integrated with the existing synthetic approaches. Here, we report a method for the synthesis of centimeter-scale, high-quality single-layer MoS₂ that can be directly patterned during CVD, so that postpatterning processes can be avoided and device fabrication can be streamlined. Utilizing X-ray photoelectron spectroscopic imaging, we characterize the chemical states of these CVD-synthesized single-layer MoS₂ films and demonstrate that the triangular-shaped MoS₂ are single-crystalline single-domain monolayers. We also …