Ultrafast Transition of Nonuniform Graphene to High-Quality Uniform Monolayer Films on Liquid Cu

It is essentially important to synthesize uniform graphene films with a controlled number of layers because their properties strongly depend on the number of layers. Although chemical vapor deposition (CVD) on Cu has been widely used to synthesize large-area graphene films, the growth on solid and liquid Cu (L-Cu) suffers from poor thickness uniformity with a great number of adlayers and difficulty in forming continuous films even after a long growth time of hours, respectively. Here, we found that nonuniform graphene films initially grown on solid Cu (S-Cu) foil can rapidly transform into continuously uniform monolayer graphene film on L-Cu within 3 min. Moreover, the films obtained show larger grain size, higher quality, better optical and electrical properties, and better performance in organic light-emitting diode applications than the original films grown on S-Cu foil. By using carbon isotope labeling, we revealed that the multilayer-to-monolayer transition of graphene on L-Cu experiences etching-"self-aligning"-coalescence processes. This two-step CVD method not only opens up a new way for the rapid growth of uniform monolayer graphene films but also provides helpful information for the controlled growth of uniform monolayers of other 2D materials such as monolayer h-BN.