Mis-orientation controlled cross-plane thermoelectricity in twisted bilayer graphene

The introduction of 'twist' or relative rotation between two atomically thin van der Waals (vdW) membranes gives rise to periodic Moire potential, leading to a substantial altercation of the band structure of the planar assembly. While most of the recent experiments primarily focus on the electronic-band hybridization by probing in-plane transport properties, here we report out-of-plane thermoelectric measurements across the van der Waals gap in twisted bilayer graphene (tBLG), which exhibits an interplay of twist-dependent inter-layer electronic and phononic hybridization. We show that at a large twist angle, the thermopower is entirely driven by a novel phonon drag effect at the sub-nanometer scale, while the electronic component of the thermopower is recovered only when the misorientation between the layers is reduced to less than two degrees. Our experiment shows that cross-plane thermoelectricity at a low angle is exceptionally sensitive to the nature of band dispersion and may provide fundamental insights into the coherence of electronic states in twisted bilayer graphene.