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Graphene has recently attracted a great deal of interest in both academia andindustry because of its unique electronic and optical properties [1,2], as wellas its chemical, thermal, and mechanical properties. The superb characteristicsof graphene make this material one of the most promising candidates for variousapplications, such as ultrafast electronic circuits [1] and photodetectors [2],clean and renewable energy [3], and rapid single-molecule DNA sequencing [4,5].The electronic properties of the graphene system rely heavily on the number ofgraphene layers [6] and effects on the coupling with the underlying substrate.Graphene can be produced by mechanical exfoliation of graphite, solutionapproaches [7,8], thermal decomposition of SiC [9,10], and chemical vapordeposition/segregation on catalytic metals [11-17]. Despite significantprogress in graphene synthesis, production with fine control over the thicknessof the film remains a considerable challenge. Here, we report on the synthesisof nearly 100% coverage of single-layer graphene on a Ni(111) surface withcarbon atoms diffused from a highly orientated pyrolytic graphite (HOPG)substrate. Our results demonstrate how fine control of thickness and structurecan be achieved by optimization of equilibrium processes of carbon diffusionfrom HOPG, segregation from Ni, and carbon diffusion at a Ni surface. Ourmethod represents a significant step toward the scalable synthesis of graphenefilms with high structural qualities and finely controlled thicknesses andtoward realizing the unique properties of graphene.

Single-layer Graphene Nearly 100% Covering an Entire Substrate