Quantum-mechanical calculations on pressure and temperature dependence of three-body recombination reactions: application to ozone formation rates.
A quantum-mechanical model is designed for the calculation of termolecular association reaction rate coefficients in the low-pressure fall-off regime. The dynamics is set up within the energy transfer mechanism and the kinetic scheme is the steady-state approximation. We applied this model to the fo...
| Main Authors: | , |
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| Format: | Journal article |
| Language: | English |
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2004
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| _version_ | 1826259423706742784 |
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| author | Charlo, D Clary, D |
| author_facet | Charlo, D Clary, D |
| author_sort | Charlo, D |
| collection | OXFORD |
| description | A quantum-mechanical model is designed for the calculation of termolecular association reaction rate coefficients in the low-pressure fall-off regime. The dynamics is set up within the energy transfer mechanism and the kinetic scheme is the steady-state approximation. We applied this model to the formation of ozone O + O2 + M --> O3 + M for M = Ar, making use of semiquantitative potential energy surfaces. The stabilization process is treated by means of the vibrational close-coupling infinite order sudden scattering theory. Major approximations include the neglect of the O3 vibrational bending mode and rovibrational couplings. We calculated individual isotope-specific rate constants and rate constant ratios over the temperature range 10-1000 K and the pressure fall-off region 10(-7)-10(2) bar. The present results show a qualitative and semiquantitative agreement with available experiments, particularly in the temperature region of atmospheric interest. |
| first_indexed | 2024-03-06T18:49:39Z |
| format | Journal article |
| id | oxford-uuid:0fca6be0-7868-4bbe-a701-7b08efeab9a4 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-06T18:49:39Z |
| publishDate | 2004 |
| record_format | dspace |
| spelling | oxford-uuid:0fca6be0-7868-4bbe-a701-7b08efeab9a42022-03-26T09:52:55ZQuantum-mechanical calculations on pressure and temperature dependence of three-body recombination reactions: application to ozone formation rates.Journal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:0fca6be0-7868-4bbe-a701-7b08efeab9a4EnglishSymplectic Elements at Oxford2004Charlo, DClary, DA quantum-mechanical model is designed for the calculation of termolecular association reaction rate coefficients in the low-pressure fall-off regime. The dynamics is set up within the energy transfer mechanism and the kinetic scheme is the steady-state approximation. We applied this model to the formation of ozone O + O2 + M --> O3 + M for M = Ar, making use of semiquantitative potential energy surfaces. The stabilization process is treated by means of the vibrational close-coupling infinite order sudden scattering theory. Major approximations include the neglect of the O3 vibrational bending mode and rovibrational couplings. We calculated individual isotope-specific rate constants and rate constant ratios over the temperature range 10-1000 K and the pressure fall-off region 10(-7)-10(2) bar. The present results show a qualitative and semiquantitative agreement with available experiments, particularly in the temperature region of atmospheric interest. |
| spellingShingle | Charlo, D Clary, D Quantum-mechanical calculations on pressure and temperature dependence of three-body recombination reactions: application to ozone formation rates. |
| title | Quantum-mechanical calculations on pressure and temperature dependence of three-body recombination reactions: application to ozone formation rates. |
| title_full | Quantum-mechanical calculations on pressure and temperature dependence of three-body recombination reactions: application to ozone formation rates. |
| title_fullStr | Quantum-mechanical calculations on pressure and temperature dependence of three-body recombination reactions: application to ozone formation rates. |
| title_full_unstemmed | Quantum-mechanical calculations on pressure and temperature dependence of three-body recombination reactions: application to ozone formation rates. |
| title_short | Quantum-mechanical calculations on pressure and temperature dependence of three-body recombination reactions: application to ozone formation rates. |
| title_sort | quantum mechanical calculations on pressure and temperature dependence of three body recombination reactions application to ozone formation rates |
| work_keys_str_mv | AT charlod quantummechanicalcalculationsonpressureandtemperaturedependenceofthreebodyrecombinationreactionsapplicationtoozoneformationrates AT claryd quantummechanicalcalculationsonpressureandtemperaturedependenceofthreebodyrecombinationreactionsapplicationtoozoneformationrates |