American Institute of Physics, The Journal of Chemical Physics, 22(135), p. 224509
DOI: 10.1063/1.3664726
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Transitions within the tunneling multiplet of CH(4) in phase II have been measured in an experiment at the backscattering instrument BASIS of the Neutron Source SNS. They all involve transitions from or to T-states. A statistical model is put forward which accounts for local departures from tetrahedral symmetry at the sites of ordered molecules. Different from previous work, in which discrete sets of overlap matrix elements have been studied, now large numbers of elements as well as the ensemble of T-states are considered. The observed neutron spectra can be explained rather well, all based on the pocket state formalism of A. Hüller [Phys. Rev. B 16, 1844 (1977)]. A completely new result is the observation and simulation of transitions between T-states, which give rise to a double peaked feature close to the elastic position and which reflect the disorder in the system. CH(2)D(2) molecules in the CH(4) matrix are largely responsible for the disorder and an interesting topic for their own sake. The simple model presented may lend itself to a broader application.