Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn
The budgets of seven halogenated gases (CFC-11, CFC-12, CFC-113, CFC-114, CFC-115, CCl4 and SF6) are studied by comparing measurements in polar firn air from two Arctic and three Antarctic sites, and simulation results of two numerical models: a 2-D atmospheric chemistry model and a 1-D firn diffusi...
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2009
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ftnonlinearchiv:oai:noa.gwlb.de:cop_mods_00047769 2023-05-15T13:55:41+02:00 Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn Martinerie, P. Nourtier-Mazauric, E. Barnola, J.-M. Sturges, W. T. Worton, D. R. Atlas, E. Gohar, L. K. Shine, K. P. Brasseur, G. P. 2009-06 electronic https://doi.org/10.5194/acp-9-3911-2009 https://noa.gwlb.de/receive/cop_mods_00047769 https://noa.gwlb.de/servlets/MCRFileNodeServlet/cop_derivate_00047389/acp-9-3911-2009.pdf https://acp.copernicus.org/articles/9/3911/2009/acp-9-3911-2009.pdf eng eng Copernicus Publications Atmospheric Chemistry and Physics -- http://www.atmos-chem-phys.net/volumes_and_issues.html -- http://www.bibliothek.uni-regensburg.de/ezeit/?2069847 -- 1680-7324 https://doi.org/10.5194/acp-9-3911-2009 https://noa.gwlb.de/receive/cop_mods_00047769 https://noa.gwlb.de/servlets/MCRFileNodeServlet/cop_derivate_00047389/acp-9-3911-2009.pdf https://acp.copernicus.org/articles/9/3911/2009/acp-9-3911-2009.pdf uneingeschränkt info:eu-repo/semantics/openAccess article Verlagsveröffentlichung article Text doc-type:article 2009 ftnonlinearchiv https://doi.org/10.5194/acp-9-3911-2009 2022-02-08T22:38:18Z The budgets of seven halogenated gases (CFC-11, CFC-12, CFC-113, CFC-114, CFC-115, CCl4 and SF6) are studied by comparing measurements in polar firn air from two Arctic and three Antarctic sites, and simulation results of two numerical models: a 2-D atmospheric chemistry model and a 1-D firn diffusion model. The first one is used to calculate atmospheric concentrations from emission trends based on industrial inventories; the calculated concentration trends are used by the second one to produce depth concentration profiles in the firn. The 2-D atmospheric model is validated in the boundary layer by comparison with atmospheric station measurements, and vertically for CFC-12 by comparison with balloon and FTIR measurements. Firn air measurements provide constraints on historical atmospheric concentrations over the last century. Age distributions in the firn are discussed using a Green function approach. Finally, our results are used as input to a radiative model in order to evaluate the radiative forcing of our target gases. Multi-species and multi-site firn air studies allow to better constrain atmospheric trends. The low concentrations of all studied gases at the bottom of the firn, and their consistency with our model results confirm that their natural sources are small. Our results indicate that the emissions, sinks and trends of CFC-11, CFC-12, CFC-113, CFC-115 and SF6 are well constrained, whereas it is not the case for CFC-114 and CCl4. Significant emission-dependent changes in the lifetimes of halocarbons destroyed in the stratosphere were obtained. Those result from the time needed for their transport from the surface where they are emitted to the stratosphere where they are destroyed. Efforts should be made to update and reduce the large uncertainties on CFC lifetimes. Article in Journal/Newspaper Antarc* Antarctic Arctic Niedersächsisches Online-Archiv NOA Antarctic Arctic Atmospheric Chemistry and Physics 9 12 3911 3934 |
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article Verlagsveröffentlichung |
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article Verlagsveröffentlichung Martinerie, P. Nourtier-Mazauric, E. Barnola, J.-M. Sturges, W. T. Worton, D. R. Atlas, E. Gohar, L. K. Shine, K. P. Brasseur, G. P. Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn |
topic_facet |
article Verlagsveröffentlichung |
description |
The budgets of seven halogenated gases (CFC-11, CFC-12, CFC-113, CFC-114, CFC-115, CCl4 and SF6) are studied by comparing measurements in polar firn air from two Arctic and three Antarctic sites, and simulation results of two numerical models: a 2-D atmospheric chemistry model and a 1-D firn diffusion model. The first one is used to calculate atmospheric concentrations from emission trends based on industrial inventories; the calculated concentration trends are used by the second one to produce depth concentration profiles in the firn. The 2-D atmospheric model is validated in the boundary layer by comparison with atmospheric station measurements, and vertically for CFC-12 by comparison with balloon and FTIR measurements. Firn air measurements provide constraints on historical atmospheric concentrations over the last century. Age distributions in the firn are discussed using a Green function approach. Finally, our results are used as input to a radiative model in order to evaluate the radiative forcing of our target gases. Multi-species and multi-site firn air studies allow to better constrain atmospheric trends. The low concentrations of all studied gases at the bottom of the firn, and their consistency with our model results confirm that their natural sources are small. Our results indicate that the emissions, sinks and trends of CFC-11, CFC-12, CFC-113, CFC-115 and SF6 are well constrained, whereas it is not the case for CFC-114 and CCl4. Significant emission-dependent changes in the lifetimes of halocarbons destroyed in the stratosphere were obtained. Those result from the time needed for their transport from the surface where they are emitted to the stratosphere where they are destroyed. Efforts should be made to update and reduce the large uncertainties on CFC lifetimes. |
format |
Article in Journal/Newspaper |
author |
Martinerie, P. Nourtier-Mazauric, E. Barnola, J.-M. Sturges, W. T. Worton, D. R. Atlas, E. Gohar, L. K. Shine, K. P. Brasseur, G. P. |
author_facet |
Martinerie, P. Nourtier-Mazauric, E. Barnola, J.-M. Sturges, W. T. Worton, D. R. Atlas, E. Gohar, L. K. Shine, K. P. Brasseur, G. P. |
author_sort |
Martinerie, P. |
title |
Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn |
title_short |
Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn |
title_full |
Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn |
title_fullStr |
Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn |
title_full_unstemmed |
Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn |
title_sort |
long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn |
publisher |
Copernicus Publications |
publishDate |
2009 |
url |
https://doi.org/10.5194/acp-9-3911-2009 https://noa.gwlb.de/receive/cop_mods_00047769 https://noa.gwlb.de/servlets/MCRFileNodeServlet/cop_derivate_00047389/acp-9-3911-2009.pdf https://acp.copernicus.org/articles/9/3911/2009/acp-9-3911-2009.pdf |
geographic |
Antarctic Arctic |
geographic_facet |
Antarctic Arctic |
genre |
Antarc* Antarctic Arctic |
genre_facet |
Antarc* Antarctic Arctic |
op_relation |
Atmospheric Chemistry and Physics -- http://www.atmos-chem-phys.net/volumes_and_issues.html -- http://www.bibliothek.uni-regensburg.de/ezeit/?2069847 -- 1680-7324 https://doi.org/10.5194/acp-9-3911-2009 https://noa.gwlb.de/receive/cop_mods_00047769 https://noa.gwlb.de/servlets/MCRFileNodeServlet/cop_derivate_00047389/acp-9-3911-2009.pdf https://acp.copernicus.org/articles/9/3911/2009/acp-9-3911-2009.pdf |
op_rights |
uneingeschränkt info:eu-repo/semantics/openAccess |
op_doi |
https://doi.org/10.5194/acp-9-3911-2009 |
container_title |
Atmospheric Chemistry and Physics |
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9 |
container_issue |
12 |
container_start_page |
3911 |
op_container_end_page |
3934 |
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1766262490716438528 |