The potential impact of ClOx radical complexes on polar stratospheric ozone loss processes
The importance of radical-molecule complexes for atmospheric chemistry has been discussed in recent years. In particular, the existence of a ClO·O2 and ClOx water radical complexes like ClO·H2O, OClO·H2O, OClO·(H2O)2, and ClOO·H2O could play a role in enhancing the ClO dimer (Cl2O2) formation and th...
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ftgfzpotsdam:oai:gfzpublic.gfz-potsdam.de:item_331295 2023-05-15T15:14:45+02:00 The potential impact of ClOx radical complexes on polar stratospheric ozone loss processes Vogel, B. Feng, W. Streibel, M. Müller, R. 2006 https://gfzpublic.gfz-potsdam.de/pubman/item/item_331295 unknown info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-6-3099-2006 info:eu-repo/semantics/altIdentifier/urn/http://doi.crossref.org/servlet/query?format=unixref&pid=bib@gfz-potsdam.de&id=10.5194/acp-6-3099-2006 https://gfzpublic.gfz-potsdam.de/pubman/item/item_331295 Atmospheric Chemistry and Physics info:eu-repo/semantics/article 2006 ftgfzpotsdam https://doi.org/10.5194/acp-6-3099-2006 2022-09-14T05:54:42Z The importance of radical-molecule complexes for atmospheric chemistry has been discussed in recent years. In particular, the existence of a ClO·O2 and ClOx water radical complexes like ClO·H2O, OClO·H2O, OClO·(H2O)2, and ClOO·H2O could play a role in enhancing the ClO dimer (Cl2O2) formation and therefore may constitute an important intermediate in polar stratospheric ozone loss cycles. Model simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS) will be presented to study the role of radical complexes on polar stratospheric ozone loss processes. The model simulations are performed for the Arctic winter 2002/2003 at a level of 500 K potential temperature and the results are compared to observed ozone loss rates determined by the Match technique. Moreover, recently reported values for the equilibrium constant of the ClO dimer formation are used to restrict the number of possible model results caused by large uncertainties about radical complex chemistry. Our model simulations show that the potential impact of ClO·O2 on polar ozone loss processes is small (dO3/dt≪0.5 ppb/sunlight h) provided that the ClO·O2 complex is only weakly stable. Assuming that the binding energies of the ClOx water complexes are much higher than theoretically predicted an enhancement of the ozone loss rate by up to ≈0.5 ppb/sunlight h is simulated. Because it is unlikely that the ClOx water complexes are much more stable than predicted we conclude that these complexes have no impact on polar stratospheric ozone loss processes. Although large uncertainties about radical complex chemistry exist, our findings show that the potential impact of ClOx radical molecule complexes on polar stratospheric ozone loss processes is very small considering pure gas-phase chemistry. However the existence of ClOx radical-molecule complexes could possibly explain discrepancies for the equilibrium constant of the ClO dimer formation found between recent laboratory and stratospheric measurements. Article in Journal/Newspaper Arctic GFZpublic (German Research Centre for Geosciences, Helmholtz-Zentrum Potsdam) Arctic Atmospheric Chemistry and Physics 6 10 3099 3114 |
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Open Polar |
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GFZpublic (German Research Centre for Geosciences, Helmholtz-Zentrum Potsdam) |
op_collection_id |
ftgfzpotsdam |
language |
unknown |
description |
The importance of radical-molecule complexes for atmospheric chemistry has been discussed in recent years. In particular, the existence of a ClO·O2 and ClOx water radical complexes like ClO·H2O, OClO·H2O, OClO·(H2O)2, and ClOO·H2O could play a role in enhancing the ClO dimer (Cl2O2) formation and therefore may constitute an important intermediate in polar stratospheric ozone loss cycles. Model simulations performed with the Chemical Lagrangian Model of the Stratosphere (CLaMS) will be presented to study the role of radical complexes on polar stratospheric ozone loss processes. The model simulations are performed for the Arctic winter 2002/2003 at a level of 500 K potential temperature and the results are compared to observed ozone loss rates determined by the Match technique. Moreover, recently reported values for the equilibrium constant of the ClO dimer formation are used to restrict the number of possible model results caused by large uncertainties about radical complex chemistry. Our model simulations show that the potential impact of ClO·O2 on polar ozone loss processes is small (dO3/dt≪0.5 ppb/sunlight h) provided that the ClO·O2 complex is only weakly stable. Assuming that the binding energies of the ClOx water complexes are much higher than theoretically predicted an enhancement of the ozone loss rate by up to ≈0.5 ppb/sunlight h is simulated. Because it is unlikely that the ClOx water complexes are much more stable than predicted we conclude that these complexes have no impact on polar stratospheric ozone loss processes. Although large uncertainties about radical complex chemistry exist, our findings show that the potential impact of ClOx radical molecule complexes on polar stratospheric ozone loss processes is very small considering pure gas-phase chemistry. However the existence of ClOx radical-molecule complexes could possibly explain discrepancies for the equilibrium constant of the ClO dimer formation found between recent laboratory and stratospheric measurements. |
format |
Article in Journal/Newspaper |
author |
Vogel, B. Feng, W. Streibel, M. Müller, R. |
spellingShingle |
Vogel, B. Feng, W. Streibel, M. Müller, R. The potential impact of ClOx radical complexes on polar stratospheric ozone loss processes |
author_facet |
Vogel, B. Feng, W. Streibel, M. Müller, R. |
author_sort |
Vogel, B. |
title |
The potential impact of ClOx radical complexes on polar stratospheric ozone loss processes |
title_short |
The potential impact of ClOx radical complexes on polar stratospheric ozone loss processes |
title_full |
The potential impact of ClOx radical complexes on polar stratospheric ozone loss processes |
title_fullStr |
The potential impact of ClOx radical complexes on polar stratospheric ozone loss processes |
title_full_unstemmed |
The potential impact of ClOx radical complexes on polar stratospheric ozone loss processes |
title_sort |
potential impact of clox radical complexes on polar stratospheric ozone loss processes |
publishDate |
2006 |
url |
https://gfzpublic.gfz-potsdam.de/pubman/item/item_331295 |
geographic |
Arctic |
geographic_facet |
Arctic |
genre |
Arctic |
genre_facet |
Arctic |
op_source |
Atmospheric Chemistry and Physics |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-6-3099-2006 info:eu-repo/semantics/altIdentifier/urn/http://doi.crossref.org/servlet/query?format=unixref&pid=bib@gfz-potsdam.de&id=10.5194/acp-6-3099-2006 https://gfzpublic.gfz-potsdam.de/pubman/item/item_331295 |
op_doi |
https://doi.org/10.5194/acp-6-3099-2006 |
container_title |
Atmospheric Chemistry and Physics |
container_volume |
6 |
container_issue |
10 |
container_start_page |
3099 |
op_container_end_page |
3114 |
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1766345165607272448 |