Angle Dependence of Interlayer Coupling in Twisted Transition Metal Dichalcogenide Heterobilayers

We reveal by first-principles calculations that the interlayer binding in a twisted MoS2/MoTe2 heterobilayer decreases with the increasing twist angle, due to the increase of the interlayer overlapping degree, a geometric quantity describing well the interlayer steric effect. The binding energy is found to be a Gaussian-type function of the twist angle. The resistance to rotation, an analogue to the interlayer sliding barrier, can also be defined accordingly. In sharp contrast to the case of the MoS2 homobilayer, here the energy band gap reduces with the increasing twist angle. We find a remarkable interlayer charge transfer from MoTe2 to MoS2, which enlarges the band gap, but this charge transfer weakens with greater twisting and interlayer overlapping degree. Our discovery provides a solid basis in twistronics and a practical instruction in band structure engineering of van der Waals heterostructures.