Orientational order and phase transitions in deuterated methane: a neutron total scattering and reverse Monte Carlo study

Abstract

We report a study of the orientational order and phase transitions in crystalline deuterated methane, carried out using neutron total scattering and the Reverse Monte Carlo (RMC) method. The resultant atomic configurations are consistent with the average structures obtained from Rietveld refinement of the powder diffraction data, but additionally enable us to determine the C–D bond orientational distribution functions (ODF) for the disordered molecules in the high-temperature phase, and for both ordered and disordered molecules in the intermediate-temperature phase. We show that this approach gives more accurate information than can been obtained from fitting a bond ODF to diffraction data. Given the resurgence of interest in orientationally-disordered crystals, we argue that the approach of total scattering with the RMC method provides a unique quantification of orientational order and disorder.