Abstract
The influence of rotational energy transfers on the vibrational relaxation of the ν 2 and ν 4 modes of CH 4 are studied. The interaction matrix is built up in the framework of the semiclassical coupled-states approximation using the asymptotic expression of (3 j) symbols. It is assumed that the intermolecular potential is the sum of five exponential atom—atom interactions. The corresponding potential matrix is diagonalized by extending the approach of Billing to the case of spherical top molecule—atom collisions. The first-order perturbation calculation of rovibrational probabilities shows the strong influence of rotational energy transfers.
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