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Graphene was reported as the first-discovered two-dimensional material, and the thermal decomposition of SiC is a feasible route to prepare graphene films. However, it is difficult to obtain a uniform single-layer graphene avoiding the coexistence of multilayer graphene islands or bare substrate holes, which give rise to the degradation of device performance and becomes an obstacle for the further applications. Here, with the assistance of nitrogen plasma, we successfully obtained high-quality single-layer and bilayer graphene with large-scale and uniform surface via annealing 4H-SiC(0001) wafers. The highly flat surface and ordered terraces of the samples were characterized using in situ scanning tunneling microscopy. The Dirac bands in single-layer and bilayer graphene were measured using angle-resolved photoemission spectroscopy. X-ray photoelectron spectroscopy combined with Raman spectroscopy were used to determine the composition of the samples and to ensure no intercalation or chemical reaction of nitrogen with graphene. Our work has provided an efficient way to obtain the uniform single-layer and bilayer graphene films grown on a semiconductive substrate, which would be an ideal platform for fabricating two-dimensional devices based on graphene.

Epitaxial Growth of Uniform Single-Layer and Bilayer Graphene with Assistance of Nitrogen Plasma