Twisting Dynamics of Large Lattice-Mismatch van der Waals Heterostructures

van der Waals (vdW) homo/heterostructures are ideal systems for studying interfacial tribological properties such as structural superlubricity. Previous studies concentrated on the mechanism of translational motion in vdW interfaces. However, detailed mechanisms and general properties of the rotational motion are barely explored. Here, we combine experiments and simulations to reveal the twisting dynamics of the MoS₂/graphite heterostructure. Unlike the translational friction falling into the superlubricity regime with no twist angle dependence, the dynamic rotational resistances highly depend on twist angles. Our results show that the periodic rotational resistance force originates from structural potential energy changes during the twisting. The structural potential energy of MoS₂/graphite heterostructure increases monotonically from 0° to 30° twist angles, and the estimated relative energy barrier is (1.43 ± 0.36) × 10^-3 J/m². The formation of Moiré superstructures in the graphene layer is the key to controlling the structural potential energy of the MoS₂/graphene heterostructure. Our results suggest that in twisting 2D heterostructures, even if the interface sliding friction is negligible, the evolving potential energy change results in a nonvanishing rotational resistance force. The structural change of the heterostructure can be an additional pathway for energy dissipation in the rotational motion, further enhancing the rotational friction force.