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We directly measure the electronic structure of twisted graphene/MoS2 van derWaals heterostructures, in which both graphene and MoS2 are monolayers. We usecathode lens microscopy and microprobe angle-resolved photoemissionspectroscopy measurements to image the surface, determine twist angle, and mapthe electronic structure of these artificial heterostructures. For monolayergraphene on monolayer MoS2, the resulting band structure reveals the absence ofhybridization between the graphene and MoS2 electronic states. Further, thegraphene-derived electronic structure in the heterostructures remains intact,irrespective of the twist angle between the two materials. In contrast,however, the electronic structure associated with the MoS2 layer is found to betwist-angle dependent; in particular, the relative difference in the energy ofthe valence band maximum at {\Gamma} and K of the MoS2 layer varies fromapproximately 0 to 0.2 eV. Our results suggest that monolayer MoS2 within theheterostructure becomes predominantly an indirect bandgap system for all twistangles except in the proximity of 30 degrees. This result enables potentialbandgap engineering in van der Waals heterostructures comprised of monolayerstructures.

Tuning the Electronic Structure of Monolayer Graphene/MoS2 van der Waals Heterostructures via Interlayer Twist