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Experimental study demonstrates temperature-independent vibrational transfer in nitrous oxide-carbon monoxide collisions, highlighting limitations of standard theoretical models at low temperatures.
Vibrational deactivation of N2O(001) by N2O, CO, and Ar has been studied from 144 to 405 °K using the laser fluorescence method. The probability of vibration to vibration energy transfer, N2O(001) + CO(v=0) ? N2O(000) + CO(v=1) + ΔE = 81 cm−1, is 0.025 and is independent of temperature from 144 to 405 °K. We have performed theoretical calculations on this rate using the modified Sharma–Brau theory developed by Tam. The present results, together with previous experimental work at higher temperatures, suggest a good theoretical fit above room temperature, but not below. The deactivation of N2O(001) in collisions with N2O, CO, and Ar, N2O(001) + M → N2O(mnl0) + M + ΔE, has been determined to be 102 to 104 times slower than observed for the V→V exchange process. The N2O(001) intramolecular rates become smaller with decreasing temperature with the exception of the N2O self-relaxation rate. Below 250 °K this rate increases rapidly with decreasing temperature.
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Starr et al. (1975) studied this question.
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