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首页> 外文期刊>The Journal of Chemical Physics >RESONANT VIBRATION-VIBRATION ENERGY TRANSFER BETWEEN HIGHLY VIBRATIONALLY EXCITED O-2(X (3)SIGMA(G)(-),V=15-26) AND CO2, N2O, N-2, AND O-3
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RESONANT VIBRATION-VIBRATION ENERGY TRANSFER BETWEEN HIGHLY VIBRATIONALLY EXCITED O-2(X (3)SIGMA(G)(-),V=15-26) AND CO2, N2O, N-2, AND O-3

机译：高振动激发的O-2（X（3）SIGMA（G）（-），V = 15-26）与CO2，N2O，N-2和O-3之间的共振振动-能量传递

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摘要

Vibrational-state-specific total-removal relaxation rate constants, k(v)(M), for O-2(X (3) Sigma(g)(-), v = 15 to 26) by M=CO2, N2O, and N-2 have been obtained using the stimulated emission pumping (SEP) method in a pump-dump and probe configuration. Relaxation by O-3 was Studied using the chemical activation method, where the reaction: O(P-3)+O-3-->O-2(v)+O-2, was employed to produce highly vibrationally excited O-2 in an excess of ozone. Efficient (1%-2% of the gas kinetic limit) near-resonant 2-1 and/or 1-1 vibration-to-vibration (V-V) energy exchange was observed whenever the energy resonant condition was fulfilled and the transition in the quench partner would have been an allowed infrared transition in the isolated molecule. For M=CO2 and N2O, the temperature dependence of the 2-1 near-resonant energy transfer rate constants was found to be inverted. In contrast, the temperature dependence of the V-R, T relaxation rate constants for M=O-2 was normal. For M=N-2, a weak but positive temperature dependence was found. By extrapolating the temperature dependence to mesospheric temperatures (200 K) the effect of highly vibrationally excited O-2 On the thermal budget can be discussed. The rate constant for the reaction of O(P-3)+O-3 was determined for an elevated collision energy of similar to 10 kcal/mol and was found to be 5000 times larger than the room temperature rate constant. (C) 1996 American Institute of Physics. [References: 65]
机译：对于O-2（X（3）Sigma（g）（-），v = 15至26），M = CO2，N2O的振动状态特定的总去除弛豫速率常数k（v）（M）， N-1和N-2已使用激发-发射泵浦（SEP）方法以泵浦-转储和探头配置获得。使用化学活化方法研究了O-3的弛豫，其中使用了以下反应：O（P-3）+ O-3-> O-2（v）+ O-2，以产生高度振动激发的O- 2过量的臭氧。每当满足能量共振条件且淬灭转变时，均观察到有效的（气体动力学极限的1％-2％）近共振2-1和/或1-1振动-振动（VV）能量交换。伴侣在分离出的分子中可能是允许的红外跃迁。对于M = CO2和N2O，发现2-1近共振能量传输速率常数的温度依赖性是相反的。相反，对于M ＝ O-2，V-R，T弛豫速率常数的温度依赖性是正常的。对于M ＝ N-2，发现弱但正的温度依赖性。通过将温度依赖性推算到中层温度（200 K），可以讨论高度振动激发的O-2对热预算的影响。确定O（P-3）+ O-3反应的速率常数，使其具有约10 kcal / mol的提高的碰撞能量，并且发现其比室温速率常数大5000倍。 （C）1996年美国物理研究所。 [参考：65]

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