Synchronous growth of AB-stacked bilayer graphene on Cu by simply controlling hydrogen pressure in CVD process

AB-stacked bilayer graphene has attracted considerable attention due to its feasibility of band gap tuning. Although synthesis of bilayer graphene on Cu has been reported using chemical vapor deposition (CVD) through a layer-by-layer growth mechanism, the process is long and complicated due to lack of catalytic assistance of Cu to the second graphene layer growth. Here we show that theoretical modeling demonstrates an alternative synchronous growth of bilayer graphene on Cu is possible by passivating the top graphene nuclei edges with hydrogen to allow carbon diffusion underneath the top graphene nuclei for bottom graphene layer formation. Moreover, such a growth mechanism has been achieved experimentally in a facile CVD method by simply controlling the H₂ pressure. Bilayer graphene with high coverage of over ∼95% and a high AB stacking ratio of up to ∼90% has been obtained within a short growth time of 30 min. Also, graphene with single, double and multiple layers can be obtained by simply controlling the hydrogen pressure. This result represents the demonstration of the fast synchronous AB-stacked bilayer graphene growth, which is important to scalable manufacture of graphene with controllable layer number and stacking required for practical applications.