Moire Superlattice Effects and Band Structure Evolution in Near-30-Degree Twisted Bilayer Graphene

In stacks of two-dimensional crystals, mismatch of their lattice constants and misalignment of crystallographic axes lead to formation of moire patterns. We show that moire superlattice effects persist in twisted bilayer graphene (tBLG) with large twists and short moire periods. Using angle-resolved photoemission, we observe dramatic changes in valence band topology across large regions of the Brillouin zone, including the vicinity of the saddle point at M and across 3 eV from the Dirac points. In this energy range, we resolve several moire minibands and detect signatures of secondary Dirac points in the reconstructed dispersions. For twists theta > 21.8 degrees, the low-energy minigaps are not due to cone anticrossing as is the case at smaller twist angles but rather due to moire scattering of electrons in one graphene layer on the potential of the other which generates intervalley coupling. Our work demonstrates the robustness of the mechanisms which enable engineering of electronic dispersions of stacks of two-dimensional crystals by tuning the interface twist angles. It also shows that large-angle tBLG hosts electronic minigaps and van Hove singularities of different origin which, given recent progress in extreme doping of graphene, could be explored experimentally.