Graphene growth through a recrystallization process in plasma enhanced chemical vapor deposition

Thermal chemical vapour deposition (TCVD) is the current method of choice to fabricate high quality, large area graphene films on catalytic copper substrates. In order to obtain sufficiently high growth rates at reduced growth temperatures an efficient dissociation of the precursor molecules already in the gas phase is required. We used plasma enhanced chemical vapour deposition (PECVD) to fabricate high quality graphene films at various temperatures. The efficient, plasma-induced dissociation of the precursor molecules results in an activation energy of 2.2 eV for the growth rate in PECVD, which is reduced by almost a factor of 2 as compared to TCVD growth in the same reactor. By varying the growth time, we demonstrate that crystalline graphene grains surrounded by amorphous carbon formed during the early stage of growth merge into an almost defect-free graphene film with growth time via a recrystallization process. Almost defect-free graphene is prepared with negligible (IlsubgDl/subg/IlsubgGl/subg l 0.1) contributions of the D peak in Raman spectroscopy and with a sheet resistance down to 470 Ω/sq.