title: Interdependency of subsurface carbon distribution and graphene-catalyst interaction.
abstract: The dynamics of the graphene-catalyst interaction during chemical vapor deposition are investigated using in situ, time- and depth-resolved X-ray photoelectron spectroscopy, and complementary grand canonical Monte Carlo simulations coupled to a tight-binding model. We thereby reveal the interdependency of the distribution of carbon close to the catalyst surface and the strength of the graphene-catalyst interaction. The strong interaction of epitaxial graphene with Ni(111) causes a depletion of dissolved carbon close to the catalyst surface, which prevents additional layer formation leading to a self-limiting graphene growth behavior for low exposure pressures (10(-6)-10(-3) mbar). A further hydrocarbon pressure increase (to ∼10(-1) mbar) leads to weakening of the graphene-Ni(111) interaction accompanied by additional graphene layer formation, mediated by an increased concentration of near-surface dissolved carbon. We show that growth of more weakly adhered, rotated graphene on Ni(111) is linked to an initially higher level of near-surface carbon compared to the case of epitaxial graphene growth. The key implications of these results for graphene growth control and their relevance to carbon nanotube growth are highlighted in the context of existing literature.
authors.affiliation: Department of Engineering, University of Cambridge , Cambridge CB3 0FA, United Kingdom.
authors.forename: Robert S
authors.initials: RS
authors.lastname: Weatherup
authors.forename: Hakim
authors.initials: H
authors.lastname: Amara
authors.forename: Raoul
authors.initials: R
authors.lastname: Blume
authors.forename: Bruno
authors.initials: B
authors.lastname: Dlubak
authors.forename: Bernhard C
authors.initials: BC
authors.lastname: Bayer
authors.forename: Mamadou
authors.initials: M
authors.lastname: Diarra
authors.forename: Mounib
authors.initials: M
authors.lastname: Bahri
authors.forename: Andrea
authors.initials: A
authors.lastname: Cabrero-Vilatela
authors.forename: Sabina
authors.initials: S
authors.lastname: Caneva
authors.forename: Piran R
authors.initials: PR
authors.lastname: Kidambi
authors.forename: Marie-Blandine
authors.initials: MB
authors.lastname: Martin
authors.forename: Cyrile
authors.initials: C
authors.lastname: Deranlot
authors.forename: Pierre
authors.initials: P
authors.lastname: Seneor
authors.forename: Robert
authors.initials: R
authors.lastname: Schloegl
authors.forename: François
authors.initials: F
authors.lastname: Ducastelle
authors.forename: Christophe
authors.initials: C
authors.lastname: Bichara
authors.forename: Stephan
authors.initials: S
authors.lastname: Hofmann