Epitaxial growth of large-area single-layer graphene over Cu(1 1 1)/sapphire by atmospheric pressure CVD

We report the atmospheric pressure chemical vapor deposition (CVD) growth of single-layer graphene over a crystalline Cu(1 1 1) film heteroepitaxially deposited on c-plane sapphire. Orientation-controlled, epitaxial single-layer graphene is achieved over the Cu(1 1 1) 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 °C gives high-quality epitaxial single-layer graphene whose orientation of hexagonal lattice matches with the Cu(1 1 1) lattice which is determined by the sapphire’s crystallographic direction. At lower CVD temperature of 900 °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°. 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(1 1 1) lattice.