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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Rovibrational Energy Transfer in Methane Excited to 2v_3 in CH_4-N_4 Mixtures from Double-Resonance Measurements
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Rovibrational Energy Transfer in Methane Excited to 2v_3 in CH_4-N_4 Mixtures from Double-Resonance Measurements

机译：通过双共振测量在CH_4-N_4混合物中激发到2v_3的甲烷中的旋转振动能量传递

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摘要

The rovibrational energy transfer processes occurring in methane upon inelastic CH_4-N_4 collisions have been investigated by using time-resolved double-resonance (DR) measurements.The CH_4 molecules were excited at about 1.66#mu#m into selcted rotational levels of the 2v_3(F_2) state by an optical parametric oscillstor pumped by a Nd:YAG laster.The low power heam of a tunable diode laser emitting around 3.4#mu#m was used to probe the following transitions:(v_3+v_4)<-v_4,2v_3<-v_3,(v_3+v_4)<-2v_4,and 3v_3<-2v_3 transitions.Measurements were performed in CH_4-N_2 gas mixtures with various molar fractions of methane.Rate constants were deduced from the time evolution of the transient populations of the probed levels.N_2 has been found to be an efficient collision partner to deplete the laser-excited level through rotational energy transfer,with a rate constant of (13.0+-1.5)#mu#s~(-1) Torr~(-1) and through intermode transfer to equilibrate the populations among the states of the tetradecad,with a rate constant of (2.0+-0.6)#mu#s~(-1) Torr~(-1).These measurements have allowed as to determine the part played in the vibrational relaxation by intermode transfer processes,which occur between the strongly interacting states of the polyads upon CH_4-CH_4 as well as CH_4-N-2 collisions,and by near-resonant V-V energy transfer processes coupling coupling the tetradecad to lower polyads,which occut only upon CH_4-CH_4 collisions.
机译：通过时间分辨双共振（DR）测量研究了甲烷在非弹性CH_4-N_4碰撞时发生的旋转振动能量转移过程.CH_4分子在约1.66＃μ＃m的激发下被选择为2v_3（3）的旋转能级。 F_2）由Nd：YAG激光泵浦的光学参量振荡器进行振荡。可发射二极管激光器的低功率光束发射约3.4＃μ＃m，用于探测以下跃迁：（v_3 + v_4）<-v_4,2v_3 <-v_3，（v_3 + v_4）<-2v_4和3v_3 <-2v_3跃迁。在具有各种甲烷摩尔分数的CH_4-N_2气体混合物中进行测量。速率常数是从瞬态人口的时间演化推导出来的已发现N_2是通过旋转能量转移耗尽激光激发能级的有效碰撞伙伴，其速率常数为（13.0 + -1.5）＃mu＃s〜（-1）Torr〜（-1 ）并通过模式间转移来平衡十四进制各州之间的人口ad，其速率常数为（2.0 + -0.6）＃mu＃s〜（-1）Torr〜（-1）。这些测量值可以确定通过模间传递过程发生在振动弛豫中的部分CH_4-CH_4碰撞以及CH_4-N-2碰撞时，双胶体的强相互作用状态之间的相互作用，以及通过近共振VV能量转移过程将四面体耦合到较低的Polyad上，后者仅在CH_4-CH_4碰撞时才发生。

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