Detailed numerical results are presented for the time dependent vibrational relaxation process in the rapid expansion of anharmonic oscillators in nonequilibrium nozzle flows. Calculations for the expansion of CO, CO/Ar, and CO/N2 mixtures from high stagnation temperatures, in the range 2000–4500°K, are compared with previously reported experimental results. It is concluded that the effects of the anharmonicity of the molecules are unlikely to lead to an increase of more than a factor of 2 in the vibrational energy relaxation rate. A simple analytical result is derived in terms of the molecular constants and the expansion temperature ratio to predict the degree of distortion of the low level ``vibrational temperature'' which results from the anharmonicity.
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