Abstract

Two-dimensional molybdenum disulfide (MoS2) has emerged as a promising candidate for next-generation electronics and optoelectronics; however, its scalable synthesis with precise control over domain size and film continuity remains challenging. Herein, we report a physical vapor deposition (PVD)-assisted chemical vapor deposition (CVD) strategy for the controllable growth of high-quality monolayer MoS2. By thermally evaporating an ultrathin (3 nm) MoO3 precursor film, spontaneous post-deposition dewetting yields a porous honeycomb morphology that significantly enhances vapor–solid reaction kinetics during subsequent sulfurization. Crucially, by modulating the argon carrier gas flow rate to regulate the local sulfur chemical potential, we achieve distinct growth regimes: a high flow rate (70 sccm) suppresses nucleation density, enabling isolated triangular and hexagonal single crystals with lateral dimensions up to 500 μm, whereas a reduced flow rate (50 sccm) promotes high-density nucleation and coalescence into continuous centimeter-scale polycrystalline films. Comprehensive structural and optical characterizations, including atomic force microscopy, Raman spectroscopy, photoluminescence, and X-ray photoelectron spectroscopy, confirm that the synthesized MoS2 exhibits prototypical monolayer thickness (~0.7 nm), well-defined local crystallinity and a direct bandgap emission at 1.84 eV. This work establishes a robust, scalable, and highly tunable route for synthesizing large-area 2D TMDs tailored for advanced device integration.

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