Intelligent self-correcting growth of uniform Bernal-stacked bi-/trilayer graphene

State-of-the-art synthesis strategies of two-dimensional (2D) materials have been designed following the nucleation-dominant pattern for structure control. However, this classical methodology fails to achieve the precise layer- and stacking-resolved growth of wafer-scale few-layer 2D materials due to its intrinsically low energy resolution. Here, we present an intelligent self-correcting method for the high-resolution growth of uniform few-layer graphene. We demonstrate the layer-resolved growth of wafer-scale bilayer and trilayer graphene (BLG and TLG) with selective Bernal stacking through spontaneous correction of the single-layer graphene film with disordered multilayer graphene islands. Theoretical calculations reveal that the self-correcting growth is driven by the stepwise energy minimization of the closed system and kinetically activated by forming a low-barrier pathway for the carbon detachment-diffusion-attachment. Such uniform Bernal-stacked BLG and TLG films show high quality with distinct quantum Hall effect being observed. Our work opens an avenue for developing an intelligent methodology to realize the precise synthesis of diverse 2D materials.