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Using density functional theory calculations with van der Waals corrections, we investigated how the interlayer orientation affects the structure and electronic properties of MoS-graphene bilayer heterostructures. Changing the orientation of graphene with respect to MoS strongly influences the type and the value of the electronic bandgap in MoS, while not significantly altering the binding energy between the layers or the interlayer spacing. We show that the physical origin of this tunable bandgap arises from variations in the S–S interplanar distance (MoS thickness) with the interlayer orientation, variations which are caused by electron transfer away from the Mo–S bonds.


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