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Two-dimensional (2D) layered semiconductor materials, such as transition metal dichalcogenides (TMDCs), have attracted considerable interests because of their intriguing optical and electronic properties. Controlled growth of TMDC crystals with large grain size and atomically smooth surface is indeed desirable but remains challenging due to excessive nucleation. Here, we have synthesized high-quality monolayer, bilayer MoSe 2 triangular crystals, and continuous thin films with controlled nucleation density via reverse-flow chemical vapor deposition (CVD). High crystallinity and good saturated absorption performance of MoSe 2 have been systematically investigated and carefully demonstrated. Optimized nucleation and uniform morphology could be achieved via fine-tuning reverse-flow switching time, growth time and temperature, with corresponding growth kinetics proposed. Our work opens up a new approach for controllable synthesis of monolayer TMDC crystals with high yield and reliability, which promote surface/interface engineering of 2D semiconductors towards van der Waals heterostructure device applications.

Synthesis of Monolayer MoSe2 with Controlled Nucleation via Reverse-Flow Chemical Vapor Deposition