Ozone Formation in Ternary Collisions: Theory and Experiment Reconciled
Ozone Formation in Ternary Collisions: Theory and Experiment Reconciled
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三元碰撞中臭氧的形成：理论与实验的协调
DOI：
10.1103/physrevlett.128.108501
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发表时间：
2022
影响因子：
8.6
通讯作者：
Kokoouline, Viatcheslav
中科院分区：
文献类型：
--
作者：
Mirahmadi, Marjan;Pérez-Ríos, Jesús;Egorov, Oleg;Tyuterev, Vladimir;Kokoouline, Viatcheslav
本信表明，臭氧的形成在三元碰撞臭氧形成的主要机制在平流层臭氧形成的温度低于200 K（为）通过形成一个临时的复合物进行，而在温度以上，反应进行主要是通过形成长寿命的振动共振。在200-700 K的中间温度下，该过程不能被视为两步机制，通常用于简化和近似三个原子或分子的碰撞。发展的理论方法适用于reactionbecause广泛的实验数据。在不采用两步近似的情况下，首次计算了三重碰撞中形成的速率系数随碰撞能量的变化。导出了5-900 K温度范围内的热平均系数。结果表明，初始形成的大部分分子是弱结合的。考虑到新生粒子数的振动猝灭过程，在100-900 K的温度范围内得到了与实验数据的良好一致性。
The present Letter shows that the formation of ozone in ternary collisions—the primary mechanism of ozone formation in the stratosphere—at temperatures below 200 K (for) proceeds through a formation of a temporary complex, while at temperatures above, the reaction proceeds mainly through a formation of long-lived vibrational resonances of. At intermediate temperatures 200–700 K, the process cannot be viewed as a two-step mechanism, often used to simplify and approximate collisions of three atoms or molecules. The developed theoretical approach is applied to the reactionbecause of extensive experimental data available. The rate coefficients for the formation ofin ternary collisionswithout using two-step approximations were computed for the first time as a function of collision energy. Thermally averaged coefficients were derived for temperatures 5–900 K. It is found that the majority ofmolecules formed initially are weakly bound. Accounting for the process of vibrational quenching of the nascent population, a good agreement with available experimental data for temperatures 100–900 K is obtained.