Substrate screening for superclean graphene growth using first-principles calculations

Suppressing the formation of amorphous surface carbon and contaminants during the preparation of graphene by chemical vapor deposition remains an ongoing issue. Herein, we analyzed how substrate characteristics affect graphene quality by simulating margin extension, the nucleation process, and defect pegging configurations on mono-crystalline oriented metal substrates with the aim of enhancing graphene cleanliness. Defect formation energy and nucleation potential, which are indirect substrate–graphene interaction features, were found to appropriately evaluate graphene quality. The crystallographic orientation of the metal substrate was discovered to be critical for producing superclean graphene. A low graphene defect density and high nucleation rate on the Cu (100) facet guarantee growth of high-quality graphene, especially in terms of suppressing the formation of amorphous carbon. In addition, rapid kink growth and self-healing on the Cu (100) facet facilitate rapid graphene synthesis, which is also promoted by rapid kink splicing and margin self-repair on this facet. This study provides theoretical insight useful for the synthesis of superclean graphene.