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The introduction of 'twist' or relative rotation between two atomically thinvan der Waals (vdW) membranes gives rise to periodic Moire potential, leadingto a substantial altercation of the band structure of the planar assembly.While most of the recent experiments primarily focus on the electronic-bandhybridization by probing in-plane transport properties, here we reportout-of-plane thermoelectric measurements across the van der Waals gap intwisted bilayer graphene (tBLG), which exhibits an interplay of twist-dependentinter-layer electronic and phononic hybridization. We show that at a largetwist angle, the thermopower is entirely driven by a novel phonon drag effectat the sub-nanometer scale, while the electronic component of the thermopoweris recovered only when the misorientation between the layers is reduced to lessthan two degrees. Our experiment shows that cross-plane thermoelectricity at alow angle is exceptionally sensitive to the nature of band dispersion and mayprovide fundamental insights into the coherence of electronic states in twistedbilayer graphene.

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