Two-stage rotational disordering of a molecular crystal surface: C60

We propose a two-stage mechanism for the rotational surface disordering phase transition of a molecular crystal, as realized in C60 fullerite. Our study, based on Monte Carlo simulations, uncovers the existence of a new intermediate regime, between a low-temperature ordered (2x2) state, and a high-temperature (1x1) disordered phase. In the intermediate regime there is partial disorder, strongest for a subset of particularly frustrated surface molecules. These concepts and calculations provide a coherent understanding of experimental observations, with possible extension to other molecular crystal surfaces.