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Growing large-area single-crystal monolayers is the holy grail of graphenesynthesis. In this work, the efficiency of graphene growth and the quality oftheir continuous films are explored through the time evolution of individualdomains and their surface coverage on the substrate. Our phase-field modelingresults and experimental characterization clearly demonstrate the criticalroles of the deposition flux, edge-reaction kinetics and the surface diffusionof active carbon sources in modulating the pattern evolution and rate ofgrowth. The contrast in edge-kinetics-limited and surface-diffusion-limitedregimes is remarkable, which can be characterized by the evolution of domainpatterns and considered as an indicator of the growth regime. Common featuresexist in these two regimes, showing that the growth rate scales with time as t2in the early stage of growth and is regime-independent, which is explained bythe coarsen profiles of carbon concentration for both the compact and dendriticdomains. The rate decays rapidly in the final stage of growth due to thecompetition between neighboring domains on the limited carbon sources diffusingon the substrate, which is highly regime-sensitive and extremely low in thesurface-diffusion-limited regime with narrow gaps between the domains to befilled. Based on these findings, synthesis strategies to improve the growthefficiency and film quality are discussed.

Pattern Evolution Characterizes the Mechanism and Efficiency of CVD Graphene Growth