Edge-controlled growth and kinetics of single-crystal graphene domains by chemical vapor deposition

Controlled synthesis of wafer-sized single crystalline high-quality graphene is a great challenge of graphene growth by chemical vapor deposition because of the complicated kinetics at edges that govern the growth process. Here we report the synthesis of single-crystal graphene domains with tunable edges from zigzag to armchair via a growth-etching-regrowth process. Both growth and etching of graphene are strongly dependent on the edge structure. This growth/etching behavior is well explained at the atomic level, given the concentrations of kinks on various edges, and allows control of graphene edges and morphology according to the classical kinetic Wulff construction theory. This work provides a deep understanding of the fundamental problems that limit graphene growth by chemical vapor deposition.