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ACS Nano. 2011 Jul 26;5(7):6069-76. doi: 10.1021/nn201978y. Epub 2011 Jul 1.

Role of hydrogen in chemical vapor deposition growth of large single-crystal graphene.

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Measurement Science & System Engineering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.


We show that graphene chemical vapor deposition growth on copper foil using methane as a carbon source is strongly affected by hydrogen, which appears to serve a dual role: an activator of the surface bound carbon that is necessary for monolayer growth and an etching reagent that controls the size and morphology of the graphene domains. The resulting growth rate for a fixed methane partial pressure has a maximum at hydrogen partial pressures 200-400 times that of methane. The morphology and size of the graphene domains, as well as the number of layers, change with hydrogen pressure from irregularly shaped incomplete bilayers to well-defined perfect single layer hexagons. Raman spectra suggest the zigzag termination in the hexagons as more stable than the armchair edges.

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