Epitaxial growth of large-area single-layer graphene over Cu(111)/sapphire by atmospheric pressure CVD

We report the atmospheric pressure chemical vapor deposition (CVD) growth of single-layer graphene over a crystalline Cu(111) film heteroepitaxially deposited on c-plane sapphire. Orientation-controlled, epitaxial single-layer graphene is achieved over the Cu(111) film on sapphire, while a polycrystalline Cu film deposited on a Si wafer gives non-uniform graphene with multi-layer flakes. Moreover, the CVD temperature is found to affect the quality and orientation of graphene grown on the Cu/sapphire substrates. The CVD growth at 1000 degrees C gives high-quality epitaxial single-layer graphene whose orientation of hexagonal lattice matches with the Cu(111) lattice which is determined by the sapphire's crystallographic direction. At lower CVD temperature of 900 degrees C, low-quality graphene with enhanced Raman D band is obtained, and it showed two different orientations of the hexagonal lattice; one matches with the Cu lattice and another rotated by 30 degrees. Carbon isotope-labeling experiment indicates rapid exchange of the surface-adsorbed and gas-supplied carbon atoms at the higher temperature, resulting in the highly crystallized graphene with energetically most stable orientation consistent with the underlying Cu(111) lattice. (C) 2011 Elsevier Ltd. All rights reserved.