In situ observations of gas phase dynamics during graphene growth using solid-state carbon sources.

A single-layer graphene has been uniformly grown on a Cu surface at elevated temperatures by thermal processing of a poly(methyl methacrylate) (PMMA) film in a rapid thermal annealing (RTA) system under vacuum. The detailed chemistry of the transition from solid-state carbon to graphene on the catalytic Cu surface was investigated by performing in situ residual gas analysis while PMMA/Cu-foil samples were being heated, in conjunction with interrupted growth studies to reconstruct ex situ the heating process. The data clearly show that the formation of graphene occurs by vaporizing hydrocarbon molecules from PMMA, such as methane and/or methyl radicals, which act as precursors, rather than by the direct graphitization of solid-state carbon. We also found that the temperature for vaporizing hydrocarbon molecules from PMMA and the length of time the gaseous hydrocarbon atmosphere is maintained, which are dependent on both the heating temperature profile and the amount of a solid carbon feedstock, are the dominant factors that determine the crystalline quality of the resulting graphene film. Under optimal growth conditions, the PMMA-derived graphene was found to have a carrier (hole) mobility as high as ∼2700 cm(2) V(-1) s(-1) at room temperature, which is superior to common graphene converted from solid carbon.

Facile synthesis of few-layer graphene with a controllable thickness using rapid thermal annealing.

Few-layer graphene films with a controllable thickness were grown on a nickel surface by rapid thermal annealing (RTA) under vacuum. The instability of nickel films in air facilitates the spontaneous formation of ultrathin (<2-3 nm) carbon- and oxygen-containing compounds on a nickel surface; thus, the high-temperature annealing of the nickel samples without the introduction of intentional carbon-containing precursors results in the formation of graphene films. From annealing temperature and ambient studies during RTA, it was found that the evaporation of oxygen atoms from the surface is the dominant factor affecting the formation of graphene films. The thickness of the graphene layers is strongly dependent on the RTA temperature and time, and the resulting films have a limited thickness (<2 nm), even for an extended RTA time. The transferred films have a low sheet resistance of ~0.9 ± 0.4 kΩ/sq, with ~94% ± 2% optical transparency, making them useful for applications as flexible transparent conductors.