Layer-by-layer synthesis of large-area graphene films by thermal cracker enhanced gas source molecular beam epitaxy

A thermal cracker enhanced gas source molecular beam epitaxy system was used to synthesize large-area graphene. Hydrocarbon gas molecules were broken by thermal cracker at very high temperature of 1200 °C and then impinged on a nickel substrate. High-quality, large-area graphene films were achieved at 800 °C, and this was confirmed by both Raman spectroscopy and transmission electron microscopy. A rapid cooling rate was not required for few-layer graphene growth in this method, and a high-percentage of single layer and bilayer graphene films was grown by controlling the growth time. The results suggest that in this method, carbon atoms migrate on the nickel surface and bond with each other to form graphene. Few-layer graphene is formed by subsequent growth of carbon layers on top of existing graphene layers. This is completely different from graphene formation through carbon dissolving in nickel and then precipitating from the nickel during rapid substrate cooling in the chemical vapor deposition method.