Bilayer graphene has attracted significant interest due to its unique properties, including fascinating electrical behavior when one layer is slightly rotated relative to the other. However, the quality of large-area bilayer graphene is often limited by the layer-plus-island growth mode in which islands of thicker graphene present as unavoidable impurities. Here, we report the observation of the layer-by-layer, Frank-van der Merwe (FM) growth mode in bilayer graphene where multilayer impurities are suppressed. Instead of the conventional surface adhesive energy, it is found that interface adhesive energy is possible to be tuned with an oxidative pretreatment. The FM-grown bilayer graphene is of AB-stacking or with small-twisting-angle (θ = 0-5°), which is more mechanically robust compared to monolayer graphene, facilitating a free-standing wet transfer technology.
Revisions are made based on reviewers' comments.