Ozone formation in ternary collisions: theory and experiment reconciled
The present Letter shows that the formation of ozone in ternary collisions O + O-2 + M-the primary mechanism of ozone formation in the stratosphere-at temperatures below 200 K (for M = Ar) proceeds through a formation of a temporary complex MO2, while at temperatures above similar to 700 K, the reac...
| Published in: | Physical Review Letters Vol. 128, № 10. P. 108501-1-108501-6 |
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| Other Authors: | , , , , |
| Format: | Article |
| Language: | English |
| Subjects: | |
| Online Access: | http://vital.lib.tsu.ru/vital/access/manager/Repository/koha:001002358 Перейти в каталог НБ ТГУ |
| Summary: | The present Letter shows that the formation of ozone in ternary collisions O + O-2 + M-the primary mechanism of ozone formation in the stratosphere-at temperatures below 200 K (for M = Ar) proceeds through a formation of a temporary complex MO2, while at temperatures above similar to 700 K, the reaction proceeds mainly through a formation of long-lived vibrational resonances of O-3*. 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 reaction O + O-2 + Ar because of extensive experimental data available. The rate coefficients for the forniation of O-3 in ternary collisions O + O-2 + Ar without 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 of O-3 molecules 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. |
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| Bibliography: | Библиогр.: 51 назв. |
| ISSN: | 0031-9007 |