A variational method is developed to treat rotational excitations of molecules and polyatomic ions in crystals. The theory is applicable for all potential strengths and is exact in the limits of weak and strong potentials. Rotational motion with one, two, and three degrees of freedom are treated in a unified manner. Explicit calculations are performed for the one-dimensional rotation of a CH3 group in a C6 potential and the three-dimensional reorientational motion of a methane molecule in Td and D2d potentials. The results are compared with recent neutron scattering experiments.
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Hüller et al. (1975) studied this question.
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