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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Statistical theory of collisional energy transfer in molecular collisions. trans-Stilbene deactivation by argon, carbon dioxide, and n-fleptane
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Statistical theory of collisional energy transfer in molecular collisions. trans-Stilbene deactivation by argon, carbon dioxide, and n-fleptane

机译：分子碰撞中碰撞能量转移的统计理论。氩气，二氧化碳和正庚烷使反-Stilbene失活

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摘要

Recent advances in experimental techniques have made it possible to measure the full conditional probability density P(E, E') of the energy transfer between two colliding molecules in the gas phase, one of which is highly energized and the other in thermal equilibrium at a given temperature. Data have now become available for trans-stilbene deactivation by the three bath gas molecules Ar, CO2, and n-heptane (C7H16). The initial energies of trans-stilbene are set to 10 000, 20 000, 30 000, and 40 000 cm (-1). The results show that exceptionally large amounts of energy are transferred in each collision. By application of our partially ergodic collision theory (PECT), we find that the energy transfer efficiency beta(E) ranges from a rather normal value of 0.15 for n-heptane at the highest excitation energy to 0.93-nearly in the ergodic collision limit-for the argon bath gas at high excitation energy. Generally, the PECT produces a good fit of the data except for the nearly elastic peak in the case of n-heptane, where PECT produces a rounded and downshifted peak in contrast to a sharply defined elastic maximum of the monoexponential functional fit produced from the original experimental data obtained by kinetically controlled selective ionization in the work of the group of Luther in Gottingen. This problem is analyzed and found to be related partly to the lack of treatment of glancing collisions in the theory with a remaining uncertainty due to the weak dependence of energy transfer efficiency on nearly elastic collisions. A summary of the present state of understanding shows that collisional activation and deactivation of reactant molecules is more efficient and more statistical than has been previously realized.
机译：实验技术的最新进展使得有可能测量气相中两个碰撞分子之间能量转移的全部条件概率密度P（E，E'），其中一个处于高能状态，另一个处于热平衡状态。给定温度。现已有了通过三个浴气分子Ar，CO2和正庚烷（C7H16）进行反式二苯乙烯减活化的数据。反式二苯乙烯的初始能量设置为10000、20000、30000和40 000 cm（-1）。结果表明，每次碰撞都传递了异常大量的能量。通过应用我们的部分遍历碰撞理论（PECT），我们发现能量传递效率β（E）的范围从正庚烷在最高激发能量下的正常值0.15到遍历碰撞极限的0.93几乎不等。用于高激发能的氩浴气体。通常，PECT产生了很好的数据拟合，但在正庚烷的情况下几乎是弹性峰，而PECT则产生了一个圆角和下移峰，而原始峰产生的单指数函数拟合的弹性最大值被清晰定义哥廷根路德小组通过动力学控制的选择性电离获得的实验数据。分析此问题后发现，该问题部分与理论中缺乏对扫视碰撞的处理有关，由于能量传输效率对近乎弹性的碰撞的依赖性较弱，因此仍然存在不确定性。对当前理解状态的总结表明，反应物分子的碰撞活化和失活比以前已经认识到的更为有效和统计。

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