title: Oxidation-assisted graphene heteroepitaxy on copper foil.
abstract: We propose an innovative, easy-to-implement approach to synthesize aligned large-area single-crystalline graphene flakes by chemical vapor deposition on copper foil. This method doubly takes advantage of residual oxygen present in the gas phase. First, by slightly oxidizing the copper surface, we induce grain boundary pinning in copper and, in consequence, the freezing of the thermal recrystallization process. Subsequent reduction of copper under hydrogen suddenly unlocks the delayed reconstruction, favoring the growth of centimeter-sized copper (111) grains through the mechanism of abnormal grain growth. Second, the oxidation of the copper surface also drastically reduces the nucleation density of graphene. This oxidation/reduction sequence leads to the synthesis of aligned millimeter-sized monolayer graphene domains in epitaxial registry with copper (111). The as-grown graphene flakes are demonstrated to be both single-crystalline and of high quality.
authors: Research Group on Carbon Nanostructures (CARBONNAGe), University of Namur, Rue de Bruxelles 61, 5000 Namur, Belgium. nicolas.reckinger@unamur.be nicolas.reckinger@gmail.com and Department of Physics, Research Center in Physics of Matter and Radiation (PMR), University of Namur, Rue de Bruxelles 61, 5000 Namur, Belgium.
authors: Nicolas
authors: N
authors: Reckinger
authors: ICTEAM, Université catholique de Louvain (UCL), Place du Levant 3, 1348 Louvain-la-Neuve, Belgium.
authors: Xiaohui
authors: X
authors: Tang
authors: Research Group on Carbon Nanostructures (CARBONNAGe), University of Namur, Rue de Bruxelles 61, 5000 Namur, Belgium. nicolas.reckinger@unamur.be nicolas.reckinger@gmail.com and Department of Physics, Research Center in Physics of Matter and Radiation (PMR), University of Namur, Rue de Bruxelles 61, 5000 Namur, Belgium.
authors: Frédéric
authors: F
authors: Joucken
authors: Laboratorio de Microscopías Avanzadas (LMA), Instituto de Nanociencia de Aragón (INA), Universidad de Zaragoza, 50018 Zaragoza, Spain.
authors: Luc
authors: L
authors: Lajaunie
authors: Laboratorio de Microscopías Avanzadas (LMA), Instituto de Nanociencia de Aragón (INA), Universidad de Zaragoza, 50018 Zaragoza, Spain and ARAID Foundation, 50018 Zaragoza, Spain.
authors: Raul
authors: R
authors: Arenal
authors: UMR CNRS 8520, IEMN/ISEN, Avenue Poincaré, BP 60069, 59652 Villeneuve d'Ascq Cedex, France.
authors: Emmanuel
authors: E
authors: Dubois
authors: Institute of Condensed Matter and Nanosciences/Nanoscopic Physics, Université catholique de Louvain (UCL), Chemin du Cyclotron 2, 1348 Louvain-la-Neuve, Belgium.
authors: Benoît
authors: B
authors: Hackens
authors: Research Group on Carbon Nanostructures (CARBONNAGe), University of Namur, Rue de Bruxelles 61, 5000 Namur, Belgium. nicolas.reckinger@unamur.be nicolas.reckinger@gmail.com and Department of Physics, Research Center in Physics of Matter and Radiation (PMR), University of Namur, Rue de Bruxelles 61, 5000 Namur, Belgium.
authors: Luc
authors: L
authors: Henrard
authors: Research Group on Carbon Nanostructures (CARBONNAGe), University of Namur, Rue de Bruxelles 61, 5000 Namur, Belgium. nicolas.reckinger@unamur.be nicolas.reckinger@gmail.com and Department of Physics, Research Center in Physics of Matter and Radiation (PMR), University of Namur, Rue de Bruxelles 61, 5000 Namur, Belgium.
authors: Jean-François
authors: JF
authors: Colomer