Electronic Hybridization of Large-Area Stacked Graphene Films

Direct, tunable coupling between individually assembled graphene layers is a next step toward designer two-dimensional 2D crystal systems, with relevance for fundamental studies and technological applications. Here we describe the fabrication and characterization of large-area cm2, coupled bilayer graphene on SiO2Si substrates. Stacking two graphene films leads to direct electronic interactions between layers, where the resulting film properties are determined by the local twist angle. Polycrystalline bilayer films have a stained-glass window appearance explained by the emergence of a narrow absorption band in the visible spectrum that depends on twist angle. Direct measurement of layer orientation via electron diffraction together with Raman and optical spectroscopy, confirms the persistence of clean interfaces over large areas. Finally, we demonstrate that interlayer coupling can be reversibly turned off through chemical modification, enabling optical-based chemical detection schemes. Together, these results suggest that 2D crystals can be individually assembled to form electronically coupled systems suitable for large-scale applications.