Thermally Induced Graphene Rotation on Hexagonal Boron Nitride

In this Letter, we report the observation of thermally induced rotation of graphene on hexagonal boron nitride (h-BN). After the rotation, two thermally stable configurations of graphene on h-BN with a relative lattice twisting angle of 0 degrees (most stable) and 30 degrees (metastable), respectively, were found. Graphene on h-BN with a twisting angle below (above) a critical angle of similar to 12 +/- 2 degrees tends to rotate towards 0 degrees (30 degrees) at a temperature of >100 degrees C, which is in line with our theoretical simulations. In addition, by manipulating the annealing temperature and the flake sizes of graphene, moire superlattices with large spatial periods of graphene on h-BN are achieved. Our studies provide a detailed understanding of the thermodynamic properties of graphene on h-BN and a feasible approach to obtaining van der Waals heterostructures with aligned lattices.