Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn
International audience 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 mode...
Published in: | Atmospheric Chemistry and Physics |
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Main Authors: | , , , , , , , , |
Other Authors: | , , , , , , , , , , , , , , , |
Format: | Article in Journal/Newspaper |
Language: | English |
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HAL CCSD
2009
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Online Access: | https://insu.hal.science/insu-00421106 https://insu.hal.science/insu-00421106/document https://insu.hal.science/insu-00421106/file/acp-9-3911-2009.pdf https://doi.org/10.5194/acp-9-3911-2009 |
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Open Polar |
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Institut national des sciences de l'Univers: HAL-INSU |
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ftinsu |
language |
English |
topic |
[SDU.STU.GL]Sciences of the Universe [physics]/Earth Sciences/Glaciology |
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[SDU.STU.GL]Sciences of the Universe [physics]/Earth Sciences/Glaciology Martinerie, Patricia Nourtier-Mazauric, E. Barnola, Jean-Marc Sturges, W. R. Worton, D. Atlas, E. Gohar, L. Shine, K. P. Brasseur, G. Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn |
topic_facet |
[SDU.STU.GL]Sciences of the Universe [physics]/Earth Sciences/Glaciology |
description |
International audience 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 |
author2 |
Laboratoire de glaciologie et géophysique de l'environnement (LGGE) Observatoire des Sciences de l'Univers de Grenoble (OSUG) Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB Université de Savoie Université de Chambéry )-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB Université de Savoie Université de Chambéry )-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS) School of Environmental Sciences Norwich University of East Anglia Norwich (UEA) University of Miami University of Miami Coral Gables Department of Environmental Science, Policy, and Management Berkeley (ESPM) University of California Berkeley (UC Berkeley) University of California (UC)-University of California (UC) Department of Meteorology Reading University of Reading (UOR) Met Office Hadley Centre (MOHC) United Kingdom Met Office Exeter National Center for Atmospheric Research Boulder (NCAR) CEC programmes: EUK2-CT2001-00116 (CRYOSTAT) and ENV4-CT97-0406 (FIRETRACC). |
format |
Article in Journal/Newspaper |
author |
Martinerie, Patricia Nourtier-Mazauric, E. Barnola, Jean-Marc Sturges, W. R. Worton, D. Atlas, E. Gohar, L. Shine, K. P. Brasseur, G. |
author_facet |
Martinerie, Patricia Nourtier-Mazauric, E. Barnola, Jean-Marc Sturges, W. R. Worton, D. Atlas, E. Gohar, L. Shine, K. P. Brasseur, G. |
author_sort |
Martinerie, Patricia |
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 |
HAL CCSD |
publishDate |
2009 |
url |
https://insu.hal.science/insu-00421106 https://insu.hal.science/insu-00421106/document https://insu.hal.science/insu-00421106/file/acp-9-3911-2009.pdf https://doi.org/10.5194/acp-9-3911-2009 |
genre |
Antarc* Antarctic Arctic |
genre_facet |
Antarc* Antarctic Arctic |
op_source |
ISSN: 1680-7316 EISSN: 1680-7324 Atmospheric Chemistry and Physics https://insu.hal.science/insu-00421106 Atmospheric Chemistry and Physics, 2009, 9 (12), pp.3911-3934. ⟨10.5194/acp-9-3911-2009⟩ |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-9-3911-2009 insu-00421106 https://insu.hal.science/insu-00421106 https://insu.hal.science/insu-00421106/document https://insu.hal.science/insu-00421106/file/acp-9-3911-2009.pdf doi:10.5194/acp-9-3911-2009 |
op_rights |
info:eu-repo/semantics/OpenAccess |
op_doi |
https://doi.org/10.5194/acp-9-3911-2009 |
container_title |
Atmospheric Chemistry and Physics |
container_volume |
9 |
container_issue |
12 |
container_start_page |
3911 |
op_container_end_page |
3934 |
_version_ |
1797573736473296896 |
spelling |
ftinsu:oai:HAL:insu-00421106v1 2024-04-28T08:02:21+00:00 Long-lived halocarbon trends and budgets from atmospheric chemistry modelling constrained with measurements in polar firn Martinerie, Patricia Nourtier-Mazauric, E. Barnola, Jean-Marc Sturges, W. R. Worton, D. Atlas, E. Gohar, L. Shine, K. P. Brasseur, G. Laboratoire de glaciologie et géophysique de l'environnement (LGGE) Observatoire des Sciences de l'Univers de Grenoble (OSUG) Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB Université de Savoie Université de Chambéry )-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB Université de Savoie Université de Chambéry )-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS) School of Environmental Sciences Norwich University of East Anglia Norwich (UEA) University of Miami University of Miami Coral Gables Department of Environmental Science, Policy, and Management Berkeley (ESPM) University of California Berkeley (UC Berkeley) University of California (UC)-University of California (UC) Department of Meteorology Reading University of Reading (UOR) Met Office Hadley Centre (MOHC) United Kingdom Met Office Exeter National Center for Atmospheric Research Boulder (NCAR) CEC programmes: EUK2-CT2001-00116 (CRYOSTAT) and ENV4-CT97-0406 (FIRETRACC). 2009-06-17 https://insu.hal.science/insu-00421106 https://insu.hal.science/insu-00421106/document https://insu.hal.science/insu-00421106/file/acp-9-3911-2009.pdf https://doi.org/10.5194/acp-9-3911-2009 en eng HAL CCSD European Geosciences Union info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-9-3911-2009 insu-00421106 https://insu.hal.science/insu-00421106 https://insu.hal.science/insu-00421106/document https://insu.hal.science/insu-00421106/file/acp-9-3911-2009.pdf doi:10.5194/acp-9-3911-2009 info:eu-repo/semantics/OpenAccess ISSN: 1680-7316 EISSN: 1680-7324 Atmospheric Chemistry and Physics https://insu.hal.science/insu-00421106 Atmospheric Chemistry and Physics, 2009, 9 (12), pp.3911-3934. ⟨10.5194/acp-9-3911-2009⟩ [SDU.STU.GL]Sciences of the Universe [physics]/Earth Sciences/Glaciology info:eu-repo/semantics/article Journal articles 2009 ftinsu https://doi.org/10.5194/acp-9-3911-2009 2024-04-05T00:28:17Z International audience 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 Institut national des sciences de l'Univers: HAL-INSU Atmospheric Chemistry and Physics 9 12 3911 3934 |