Understanding the microscopic mechanisms for the nucleation and growth of two-dimensional molybdenum diselenide (2D MoSe) via chemical vapor deposition (CVD) is crucial towards the precisely controlled growth of the 2D material. In this work, we employed a joint use of transmission electron microscopy and CVD, in which the 2D MoSe were directly grown on a graphene membrane based on grids, that enables the microstructural characterization of as-grown MoSe flakes. We further explore the role of hydrogen gas and find: in an argon ambient, the primary products are few-layer MoSe flakes, along with MoO nanoparticles; while with the introduction of H, single-layer MoSe became the dominant product during the CVD growth. Quantitative analysis of the effects of H flow rate on the flake sizes, and areal coverage was also given. Nevertheless, we further illuminated the evolution of shape morphology and edge structures of single-layer MoSe, and proposed the associated growth routes during a typical CVD process.
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