Ozone Formation in Ternary Collisions: Theory and Experiment Reconciled
| Autor: | Marjan Mirahmadi, Jesús Pérez-Ríos, Oleg Egorov, Vladimir Tyuterev, Viatcheslav Kokoouline |
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| Rok vydání: | 2021 |
| Předmět: | |
| Zdroj: | Physical Review Letters Physical Review Letters. 2022. Vol. 128, № 10. P. 108501-1-108501-6 |
| ISSN: | 1079-7114 |
| Popis: | Absorbing UV radiation, ozone protects life on Earth and plays a fundamental role in Earth's temperature balance. The formation of ozone occurs through the ternary recombination reaction: O$_2$+O+M $\rightarrow$ O$_3$+M, where M can be N$_2$, O$_2$ or Ar. Here, we developed a theoretical approach capable of modeling the formation of ozone molecules in ternary collisions, and applied it to the reaction with M=Ar because of extensive experimental data available. The rate coefficients for the direct formation of O$_3$ in ternary collisions O+O$_2$+Ar were computed for the first time as a function of collision energy, and thermally-averaged coefficients were derived for temperatures 5-900~K leading to a good agreement with available experimental data for temperatures 100-900~K. The present study shows that the formation of ozone in ternary collisions O+O$_2$+Ar at temperatures below 200~K proceeds through a formation of a temporary complex ArO$_2$, while at temperatures above 1000~K, the reaction proceeds mainly through a formation of long-lived vibrational resonances of O$_3^*$. At intermediate temperatures 200~K-1000~K, the process cannot be viewed as a two-step mechanism. In addition, it is found that the majority of O$_3$ molecules formed initially are weakly bound. 6 pages, 5 figures |
| Databáze: | OpenAIRE |
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