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Using first-principles calculations within density functional theory, westudy the energetics and kinetics of carbon nucleation in the early stages ofepitaxial graphene growth on three representative stepped metal surfaces:Ir(111), Ru(0001), and Cu(111). We find that on the flat surfaces of Ir(111)and Ru(0001), two carbon atoms repel each other, while they prefer to form adimer on Cu(111). Moreover, the step edges on Ir and Ru surfaces cannot serveas effective trapping centers for single carbon adatoms, but can readilyfacilitate the formation of carbon dimers. These contrasting behaviors areattributed to the delicate competition between C-C bonding and C-metal bonding,and a simple generic principle is proposed to predict the nucleation sites of Cadatoms on many other metal substrates with the C-metal bond strengths as theminimal inputs.

Contrasting Behavior of Carbon Nucleation in the Initial Stages of Graphene Epitaxial Growth on Stepped Metal Surfaces