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A master-equation formalism is applied to the problem of overtone-induced isomerization of CH3NC to CH3CN. The results are compared to the experiments of Reddy and Berry, who measured the yield of isomerization as a function of pressure after excitation to the fourth and fifth overtones of the CH stretching mode. The master-equation model predicts the yield and the curvature in the yield−1 vs pressure plots observed in the experiments. For the lower overtone (5←0) the results are consistent with a simple strong-collider model. However, even under strong-collider conditions the yield is very sensitive to the parameters in the master equation. For the upper overtone (6←0) the data do not fit a strong collider model and multistep deactivation dominates. We are able to determine from the data the average energy transferred in a collision by assuming a particular form for the energy-transfer function. In addition, the effect of changing the shape of the energy-transfer function is investigated.
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Miller et al. (1986) studied this question.
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