Synthesis of sub-millimeter Bi-/multi-layer graphene by designing a sandwiched structure using copper foils

Bernal-stacked (AB-stacked) bilayer graphene has been receiving significant attention because it has a tunable band-gap under an applied vertical electric field. Herein, we designed a sandwiched structure simply by embedding one piece of Cu sheet into a Cu pocket to establish an environment that suppresses Cu evaporation and ensures that both surfaces of Cu sheet are smooth to grow large-size bilayer graphene (BLG) and multilayer graphene (MLG). Single-diffusion and double-diffusion mechanisms help explain graphene growth on both the Cu pocket and the Cu sheet, respectively. On the basis of the double-diffusion mechanism, we prepared AB-stacked sub-millimeter BLG and MLG with diameters up to 603 μm and 793 μm, respectively. Our work regarding the improvement of the quality and single-crystal size of graphene domains helps broaden the potential applications in materials chemistry and microelectronic devices.