Stacking order has a strong influence on the coupling between the two layers of twisted bilayer graphene (BLG), which in turn determines its physical properties. Here, we report the investigation of the interlayer coupling of the epitaxially grown single-crystal 30°-twisted BLG on Cu(111) at the atomic scale. The stacking order and morphology of BLG is controlled by a rationally designed two-step growth process, that is, the thermodynamically controlled nucleation and kinetically controlled growth. The crystal structure of the 30°-twisted bilayer graphene (30°-tBLG) is determined to have quasicrystal-like symmetry. The electronic properties and interlayer coupling of the 30°-tBLG are investigated using scanning tunneling microscopy and spectroscopy. The energy-dependent local density of states with in situ electrostatic doping shows that the electronic states in two graphene layers are decoupled near the Dirac point. A linear dispersion originated from the constituent graphene monolayers is discovered with doubled degeneracy. This study contributes to controlled growth of twist-angle-defined BLG and provides insights on the electronic properties and interlayer coupling in this intriguing system.
Keywords: electronic structure; epitaxial growth; interlayer coupling; quasicrystal; twisted bilayer graphene.