Large Variations of the Raman Signal in the Spectra of Twisted Bilayer Graphene on a BN Substrate

We report an unusual enhancement of the Raman signal of the G mode in a twisted graphene bilayer (2-LG) on a hexagonal single-crystalline boron nitride substrate. We used an isotopically engineered 2-LG, where the top layer was composed of C-13 atoms and the bottom layer of C-12 atoms. Consequently, it was possible by Raman spectroscopy to distinguish between the enhancement coming from the top and bottom layers. The enhancement of the G mode was, however, found to be similar for the top and bottom layers, and this enhancement effect was observed only at certain locations on the substrate. The experiment with two different laser excitation energies showed that the location of the enhanced spots is dependent on the laser excitation energy. Therefore our results suggest that the enhancement comes from new states in the electronic structure, which are a consequence of a local specific rotation of the grains in graphene layers.