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Title: Cooperative Island Growth of Large Area Single-Crystal Graphene by Chemical Vapor Deposition on Cu

We describe a two-step approach for suppressing nucleation of graphene on Cu using chemical vapor deposition. In the first step, as received Cu foils are oxidized in air at temperatures up to 500 C to remove surface impurities and to induce the regrowth of Cu grains during subsequent annealing in H2 flow at 1040 C prior to graphene growth. In the second step, transient reactant cooling is performed by using a brief Ar pulse at the onset of growth to induce collisional deactivation of the carbon growth species. The combination of these two steps results in a three orders of magnitude reduction in the graphene nucleation density, enabling the growth of millimeter-size single crystal graphene grains. A kinetic model shows that suppressing nucleation promotes a cooperative island growth mode that favors the formation of large area single crystal graphene, and it is accompanied by a roughly 3 orders of magnitude increase in the reactive sticking probability of methane compared to that in random nucleation growth.
 [1] ;  [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [3] ;  [2]
  1. Oak Ridge National Laboratory (ORNL)
  2. ORNL
  3. Argonne National Laboratory (ANL)
Publication Date:
OSTI Identifier:
DOE Contract Number:
Resource Type:
Journal Article
Resource Relation:
Journal Name: ACS Nano; Journal Volume: 8; Journal Issue: 6
Research Org:
Oak Ridge National Laboratory (ORNL); Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org:
SC USDOE - Office of Science (SC)
Country of Publication:
United States
graphene; nucleation; kinetics; chemical vapor deposition