Suppression of Graphene Nucleation by Turning Off Hydrogen Supply Just before Atmospheric Pressure Chemical Vapor Deposition Growth

To exploit the extraordinary property of graphene in practical electrical and optical devices, it is necessary to produce large-sized, single-crystal graphene. Atmospheric pressure chemical vapor deposition (APCVD) on polycrystalline Cu surface is a promising scalable route of graphene synthesis but the unavoidable multiple nucleation limits their reachable domain size. Here, we report that effective suppression of nucleation was achieved by only turning off hydrogen supply before introduction of the carbon source for graphene growth. The density of graphene decreased from 72.0 to 2.2 domains/cm2 by turning off hydrogen for 15 min. X-ray photoelectron spectroscopy and Raman spectroscopy studies show that the Cu surface was covered with 3–4 nm thick highly crystalline Cu2O, which would be caused by oxidation by residual oxidative gasses in the chamber during the turning off period. It was also revealed that elevating the temperature in Ar followed by annealing in H2/Ar before turning off hydrogen led to the enlargement of the Cu domain, resulting in the further suppression of nucleation. By optimizing such growth parameters in the CVD process, a single-crystal graphene with ~2.6 mm in diameter was successfully obtained.