Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling
International audience The nitrogen ( 15N) and triple oxygen ( 17/18O) isotopic composition of nitrate (NO−3 ) was measured year-round in the atmosphere and snow pits at Dome C (DC, 75.1 S, 123.3 E), and in surface snow on a transect between DC and the coast. Snow pit profiles of 15N ( 18O) in NO−3...
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://hal-insu.archives-ouvertes.fr/insu-00412552 https://hal-insu.archives-ouvertes.fr/insu-00412552/document https://hal-insu.archives-ouvertes.fr/insu-00412552/file/acp-9-8681-2009.pdf https://doi.org/10.5194/acp-9-8681-2009 |
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Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) |
op_collection_id |
ftccsdartic |
language |
English |
topic |
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean Atmosphere |
spellingShingle |
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean Atmosphere Frey, M.M. Savarino, J. Morin, S. Erbland, J. Martins, J.M. F. Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling |
topic_facet |
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean Atmosphere |
description |
International audience The nitrogen ( 15N) and triple oxygen ( 17/18O) isotopic composition of nitrate (NO−3 ) was measured year-round in the atmosphere and snow pits at Dome C (DC, 75.1 S, 123.3 E), and in surface snow on a transect between DC and the coast. Snow pit profiles of 15N ( 18O) in NO−3 5 show significant enrichment (depletion) of >200 (<40) ‰ compared to the isotopic signal in atmospheric NO−3 , whereas post-depositional fractionation in É17O(NO−3 ) is small, allowing reconstruction of past shifts in tropospheric oxidation pathways from ice cores. Assuming a Rayleigh-type process we find in the DC04 (DC07) pit fractionation factors " of −50±10 (−71±12) ‰, 6±3 (9±2) ‰ and 10 1±0.2 (2±0.6) ‰, for 15N, 18O and É17O, respectively. A photolysis model reproduces " for 15N within the range of uncertainty at DC and for lab experiments reported by Blunier et al. (2005), suggesting that the current literature value for photolytic isotopic fractionation in snow is significantly underestimated. Depletion of oxygen stable isotopes is attributed to photolysis followed by isotopic exchange with water and hydroxyl radicals. Conversely, 15N enrichment of the NO−3 15 fraction in the snow implies 15N depletion of emissions. Indeed, 15N in atmospheric NO−3 shows a strong decrease from background levels (4.4±6.8‰) to −35.1‰ in spring followed by recovery during summer, consistent with significant snow pack emissions of reactive nitrogen. Field and lab evidence therefore suggest that photolysis dominates fractionation and associated NO−3 20 loss from snow in the low-accumulation regions of the East Antarctic Ice Sheet (EAIS). The É17O signature confirms previous coastal measurements that the peak of atmospheric NO−3 in spring is of stratospheric origin. After sunrise photolysis drives then redistribution of NO−3 from the snowpack photic zone to the atmosphere and a snow surface skin layer, thereby concentrating NO−3 at the surface. Little NO−3 is 25 exported off the EAIS plateau, still snow emissions from as far ... |
author2 |
British Antarctic Survey (BAS) Natural Environment Research Council (NERC) Laboratoire de glaciologie et géophysique de l'environnement (LGGE) Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-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 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) Laboratoire d'étude des transferts en hydrologie et environnement (LTHE) Institut National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS)-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) European Science Foundation (ESF) under the EUROCORES Programme EuroCLIMATE (contract No. ERAS-CT-2003-980409), ANR-07-VULN-0013,VANISH,Vulnerability of the ANtarctic Ice SHeet and its atmosphere(2007) |
format |
Article in Journal/Newspaper |
author |
Frey, M.M. Savarino, J. Morin, S. Erbland, J. Martins, J.M. F. |
author_facet |
Frey, M.M. Savarino, J. Morin, S. Erbland, J. Martins, J.M. F. |
author_sort |
Frey, M.M. |
title |
Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling |
title_short |
Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling |
title_full |
Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling |
title_fullStr |
Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling |
title_full_unstemmed |
Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling |
title_sort |
photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of east antarctica and implications for reactive nitrogen cycling |
publisher |
HAL CCSD |
publishDate |
2009 |
url |
https://hal-insu.archives-ouvertes.fr/insu-00412552 https://hal-insu.archives-ouvertes.fr/insu-00412552/document https://hal-insu.archives-ouvertes.fr/insu-00412552/file/acp-9-8681-2009.pdf https://doi.org/10.5194/acp-9-8681-2009 |
geographic |
Antarctic East Antarctic Ice Sheet East Antarctica |
geographic_facet |
Antarctic East Antarctic Ice Sheet East Antarctica |
genre |
Antarc* Antarctic Antarctica East Antarctica Ice Sheet |
genre_facet |
Antarc* Antarctic Antarctica East Antarctica Ice Sheet |
op_source |
ISSN: 1680-7316 EISSN: 1680-7324 Atmospheric Chemistry and Physics https://hal-insu.archives-ouvertes.fr/insu-00412552 Atmospheric Chemistry and Physics, European Geosciences Union, 2009, 9 (22), pp.8681-8696. ⟨10.5194/acp-9-8681-2009⟩ |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-9-8681-2009 insu-00412552 https://hal-insu.archives-ouvertes.fr/insu-00412552 https://hal-insu.archives-ouvertes.fr/insu-00412552/document https://hal-insu.archives-ouvertes.fr/insu-00412552/file/acp-9-8681-2009.pdf doi:10.5194/acp-9-8681-2009 |
op_rights |
info:eu-repo/semantics/OpenAccess |
op_doi |
https://doi.org/10.5194/acp-9-8681-2009 |
container_title |
Atmospheric Chemistry and Physics |
container_volume |
9 |
container_issue |
22 |
container_start_page |
8681 |
op_container_end_page |
8696 |
_version_ |
1766257602887417856 |
spelling |
ftccsdartic:oai:HAL:insu-00412552v1 2023-05-15T13:52:51+02:00 Photolysis imprint in the nitrate stable isotope signal in snow and atmosphere of East Antarctica and implications for reactive nitrogen cycling Frey, M.M. Savarino, J. Morin, S. Erbland, J. Martins, J.M. F. British Antarctic Survey (BAS) Natural Environment Research Council (NERC) Laboratoire de glaciologie et géophysique de l'environnement (LGGE) Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-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 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) Laboratoire d'étude des transferts en hydrologie et environnement (LTHE) Institut National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS)-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) European Science Foundation (ESF) under the EUROCORES Programme EuroCLIMATE (contract No. ERAS-CT-2003-980409), ANR-07-VULN-0013,VANISH,Vulnerability of the ANtarctic Ice SHeet and its atmosphere(2007) 2009 https://hal-insu.archives-ouvertes.fr/insu-00412552 https://hal-insu.archives-ouvertes.fr/insu-00412552/document https://hal-insu.archives-ouvertes.fr/insu-00412552/file/acp-9-8681-2009.pdf https://doi.org/10.5194/acp-9-8681-2009 en eng HAL CCSD European Geosciences Union info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-9-8681-2009 insu-00412552 https://hal-insu.archives-ouvertes.fr/insu-00412552 https://hal-insu.archives-ouvertes.fr/insu-00412552/document https://hal-insu.archives-ouvertes.fr/insu-00412552/file/acp-9-8681-2009.pdf doi:10.5194/acp-9-8681-2009 info:eu-repo/semantics/OpenAccess ISSN: 1680-7316 EISSN: 1680-7324 Atmospheric Chemistry and Physics https://hal-insu.archives-ouvertes.fr/insu-00412552 Atmospheric Chemistry and Physics, European Geosciences Union, 2009, 9 (22), pp.8681-8696. ⟨10.5194/acp-9-8681-2009⟩ [SDU.OCEAN]Sciences of the Universe [physics]/Ocean Atmosphere info:eu-repo/semantics/article Journal articles 2009 ftccsdartic https://doi.org/10.5194/acp-9-8681-2009 2021-10-24T19:39:44Z International audience The nitrogen ( 15N) and triple oxygen ( 17/18O) isotopic composition of nitrate (NO−3 ) was measured year-round in the atmosphere and snow pits at Dome C (DC, 75.1 S, 123.3 E), and in surface snow on a transect between DC and the coast. Snow pit profiles of 15N ( 18O) in NO−3 5 show significant enrichment (depletion) of >200 (<40) ‰ compared to the isotopic signal in atmospheric NO−3 , whereas post-depositional fractionation in É17O(NO−3 ) is small, allowing reconstruction of past shifts in tropospheric oxidation pathways from ice cores. Assuming a Rayleigh-type process we find in the DC04 (DC07) pit fractionation factors " of −50±10 (−71±12) ‰, 6±3 (9±2) ‰ and 10 1±0.2 (2±0.6) ‰, for 15N, 18O and É17O, respectively. A photolysis model reproduces " for 15N within the range of uncertainty at DC and for lab experiments reported by Blunier et al. (2005), suggesting that the current literature value for photolytic isotopic fractionation in snow is significantly underestimated. Depletion of oxygen stable isotopes is attributed to photolysis followed by isotopic exchange with water and hydroxyl radicals. Conversely, 15N enrichment of the NO−3 15 fraction in the snow implies 15N depletion of emissions. Indeed, 15N in atmospheric NO−3 shows a strong decrease from background levels (4.4±6.8‰) to −35.1‰ in spring followed by recovery during summer, consistent with significant snow pack emissions of reactive nitrogen. Field and lab evidence therefore suggest that photolysis dominates fractionation and associated NO−3 20 loss from snow in the low-accumulation regions of the East Antarctic Ice Sheet (EAIS). The É17O signature confirms previous coastal measurements that the peak of atmospheric NO−3 in spring is of stratospheric origin. After sunrise photolysis drives then redistribution of NO−3 from the snowpack photic zone to the atmosphere and a snow surface skin layer, thereby concentrating NO−3 at the surface. Little NO−3 is 25 exported off the EAIS plateau, still snow emissions from as far ... Article in Journal/Newspaper Antarc* Antarctic Antarctica East Antarctica Ice Sheet Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) Antarctic East Antarctic Ice Sheet East Antarctica Atmospheric Chemistry and Physics 9 22 8681 8696 |