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

Abstract

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.