Constraining N 2 O emissions since 1940 using firn air isotope measurements in both hemispheres
International audience N2O is currently the third most important anthropogenic greenhouse gas in terms of radiative forcing and its atmospheric mole fraction is rising steadily. To quantify the growth rate and its causes over the past decades, we performed a multi-site reconstruction of the atmosphe...
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
2017
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Online Access: | https://hal.univ-grenoble-alpes.fr/hal-01598604 https://hal.univ-grenoble-alpes.fr/hal-01598604/document https://hal.univ-grenoble-alpes.fr/hal-01598604/file/acp-17-4539-2017.pdf https://doi.org/10.5194/acp-17-4539-2017 |
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Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) |
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English |
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[SPI.AUTO]Engineering Sciences [physics]/Automatic |
spellingShingle |
[SPI.AUTO]Engineering Sciences [physics]/Automatic Prokopiou, Markella Martinerie, Patricia Sapart, Célia J. Witrant, Emmanuel Monteil, Guillaume Ishijima, Kentaro Bernard, Sophie Kaiser, Jan Levin, Ingeborg Blunier, Thomas Etheridge, David Dlugokencky, Ed van de Wal, Roderik S. W. Röckmann, Thomas Constraining N 2 O emissions since 1940 using firn air isotope measurements in both hemispheres |
topic_facet |
[SPI.AUTO]Engineering Sciences [physics]/Automatic |
description |
International audience N2O is currently the third most important anthropogenic greenhouse gas in terms of radiative forcing and its atmospheric mole fraction is rising steadily. To quantify the growth rate and its causes over the past decades, we performed a multi-site reconstruction of the atmospheric N2O mole fraction and isotopic composition using new and previously published firn air data collected from Greenland and Antarctica in combination with a firn diffusion and densification model. The multi-site reconstruction showed that while the global mean N2O mole fraction increased from (290 ± 1) nmol mol−1 in 1940 to (322 ± 1) nmol mol−1 in 2008, the isotopic composition of atmospheric N2O decreased by (−2.2 ± 0.2) ‰ for δ15Nav, (−1.0 ± 0.3) ‰ for δ18O, (−1.3 ± 0.6) ‰ for δ15Nα, and (−2.8 ± 0.6) ‰ for δ15Nβ over the same period. The detailed temporal evolution of the mole fraction and isotopic composition derived from the firn air model was then used in a two-box atmospheric model (comprising a stratospheric box and a tropospheric box) to infer changes in the isotopic source signature over time. The precise value of the source strength depends on the choice of the N2O lifetime, which we choose to fix at 123 years. The average isotopic composition over the investigated period is δ15Nav = (−7.6 ± 0.8) ‰ (vs. air-N2), δ18O = (32.2 ± 0.2) ‰ (vs. Vienna Standard Mean Ocean Water – VSMOW) for δ18O, δ15Nα = (−3.0 ± 1.9) ‰ and δ15Nβ = (−11.7 ± 2.3) ‰. δ15Nav, and δ15Nβ show some temporal variability, while for the other signatures the error bars of the reconstruction are too large to retrieve reliable temporal changes. Possible processes that may explain trends in 15N are discussed. The 15N site preference ( = δ15Nα − δ15Nβ) provides evidence of a shift in emissions from denitrification to nitrification, although the uncertainty envelopes are large. |
author2 |
Institute for Marine and Atmospheric Research Utrecht (IMAU) Utrecht University Utrecht Institut des Géosciences de l’Environnement (IGE) Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Recherche pour le Développement (IRD)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 ) Laboratoire de Glaciologie Université libre de Bruxelles (ULB) GIPSA - Systèmes linéaires et robustesse (GIPSA-SLR) Département Automatique (GIPSA-DA) Grenoble Images Parole Signal Automatique (GIPSA-lab ) Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut Polytechnique de Grenoble - Grenoble Institute of Technology-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut Polytechnique de Grenoble - Grenoble Institute of Technology-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Grenoble Images Parole Signal Automatique (GIPSA-lab ) Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut Polytechnique de Grenoble - Grenoble Institute of Technology-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut Polytechnique de Grenoble - Grenoble Institute of Technology-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 ) Lund University Lund National Institute of Polar Research Tokyo (NiPR) School of Environmental Sciences Norwich University of East Anglia Norwich (UEA) Institut für Umweltphysik Heidelberg Universität Heidelberg Heidelberg Centre for Ice and Climate Copenhagen Niels Bohr Institute Copenhagen (NBI) Faculty of Science Copenhagen University of Copenhagen = Københavns Universitet (KU)-University of Copenhagen = Københavns Universitet (KU)-Faculty of Science Copenhagen University of Copenhagen = Københavns Universitet (KU)-University of Copenhagen = Københavns Universitet (KU) CSIRO Marine and Atmospheric Research (CSIRO-MAR) Commonwealth Scientific and Industrial Research Organisation Canberra (CSIRO) NOAA Earth System Research Laboratory (ESRL) National Oceanic and Atmospheric Administration (NOAA) |
format |
Article in Journal/Newspaper |
author |
Prokopiou, Markella Martinerie, Patricia Sapart, Célia J. Witrant, Emmanuel Monteil, Guillaume Ishijima, Kentaro Bernard, Sophie Kaiser, Jan Levin, Ingeborg Blunier, Thomas Etheridge, David Dlugokencky, Ed van de Wal, Roderik S. W. Röckmann, Thomas |
author_facet |
Prokopiou, Markella Martinerie, Patricia Sapart, Célia J. Witrant, Emmanuel Monteil, Guillaume Ishijima, Kentaro Bernard, Sophie Kaiser, Jan Levin, Ingeborg Blunier, Thomas Etheridge, David Dlugokencky, Ed van de Wal, Roderik S. W. Röckmann, Thomas |
author_sort |
Prokopiou, Markella |
title |
Constraining N 2 O emissions since 1940 using firn air isotope measurements in both hemispheres |
title_short |
Constraining N 2 O emissions since 1940 using firn air isotope measurements in both hemispheres |
title_full |
Constraining N 2 O emissions since 1940 using firn air isotope measurements in both hemispheres |
title_fullStr |
Constraining N 2 O emissions since 1940 using firn air isotope measurements in both hemispheres |
title_full_unstemmed |
Constraining N 2 O emissions since 1940 using firn air isotope measurements in both hemispheres |
title_sort |
constraining n 2 o emissions since 1940 using firn air isotope measurements in both hemispheres |
publisher |
HAL CCSD |
publishDate |
2017 |
url |
https://hal.univ-grenoble-alpes.fr/hal-01598604 https://hal.univ-grenoble-alpes.fr/hal-01598604/document https://hal.univ-grenoble-alpes.fr/hal-01598604/file/acp-17-4539-2017.pdf https://doi.org/10.5194/acp-17-4539-2017 |
geographic |
Greenland |
geographic_facet |
Greenland |
genre |
Antarc* Antarctica Greenland |
genre_facet |
Antarc* Antarctica Greenland |
op_source |
ISSN: 1680-7316 EISSN: 1680-7324 Atmospheric Chemistry and Physics https://hal.univ-grenoble-alpes.fr/hal-01598604 Atmospheric Chemistry and Physics, European Geosciences Union, 2017, 17 (7), pp.4539 - 4564. ⟨10.5194/acp-17-4539-2017⟩ |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-17-4539-2017 hal-01598604 https://hal.univ-grenoble-alpes.fr/hal-01598604 https://hal.univ-grenoble-alpes.fr/hal-01598604/document https://hal.univ-grenoble-alpes.fr/hal-01598604/file/acp-17-4539-2017.pdf doi:10.5194/acp-17-4539-2017 |
op_rights |
http://creativecommons.org/licenses/by-nc/ info:eu-repo/semantics/OpenAccess |
op_rightsnorm |
CC-BY-NC |
op_doi |
https://doi.org/10.5194/acp-17-4539-2017 |
container_title |
Atmospheric Chemistry and Physics |
container_volume |
17 |
container_issue |
7 |
container_start_page |
4539 |
op_container_end_page |
4564 |
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1766264165390876672 |
spelling |
ftccsdartic:oai:HAL:hal-01598604v1 2023-05-15T13:56:38+02:00 Constraining N 2 O emissions since 1940 using firn air isotope measurements in both hemispheres Prokopiou, Markella Martinerie, Patricia Sapart, Célia J. Witrant, Emmanuel Monteil, Guillaume Ishijima, Kentaro Bernard, Sophie Kaiser, Jan Levin, Ingeborg Blunier, Thomas Etheridge, David Dlugokencky, Ed van de Wal, Roderik S. W. Röckmann, Thomas Institute for Marine and Atmospheric Research Utrecht (IMAU) Utrecht University Utrecht Institut des Géosciences de l’Environnement (IGE) Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut de Recherche pour le Développement (IRD)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 ) Laboratoire de Glaciologie Université libre de Bruxelles (ULB) GIPSA - Systèmes linéaires et robustesse (GIPSA-SLR) Département Automatique (GIPSA-DA) Grenoble Images Parole Signal Automatique (GIPSA-lab ) Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut Polytechnique de Grenoble - Grenoble Institute of Technology-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut Polytechnique de Grenoble - Grenoble Institute of Technology-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Grenoble Images Parole Signal Automatique (GIPSA-lab ) Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut Polytechnique de Grenoble - Grenoble Institute of Technology-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 )-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut Polytechnique de Grenoble - Grenoble Institute of Technology-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 ) Lund University Lund National Institute of Polar Research Tokyo (NiPR) School of Environmental Sciences Norwich University of East Anglia Norwich (UEA) Institut für Umweltphysik Heidelberg Universität Heidelberg Heidelberg Centre for Ice and Climate Copenhagen Niels Bohr Institute Copenhagen (NBI) Faculty of Science Copenhagen University of Copenhagen = Københavns Universitet (KU)-University of Copenhagen = Københavns Universitet (KU)-Faculty of Science Copenhagen University of Copenhagen = Københavns Universitet (KU)-University of Copenhagen = Københavns Universitet (KU) CSIRO Marine and Atmospheric Research (CSIRO-MAR) Commonwealth Scientific and Industrial Research Organisation Canberra (CSIRO) NOAA Earth System Research Laboratory (ESRL) National Oceanic and Atmospheric Administration (NOAA) 2017 https://hal.univ-grenoble-alpes.fr/hal-01598604 https://hal.univ-grenoble-alpes.fr/hal-01598604/document https://hal.univ-grenoble-alpes.fr/hal-01598604/file/acp-17-4539-2017.pdf https://doi.org/10.5194/acp-17-4539-2017 en eng HAL CCSD European Geosciences Union info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-17-4539-2017 hal-01598604 https://hal.univ-grenoble-alpes.fr/hal-01598604 https://hal.univ-grenoble-alpes.fr/hal-01598604/document https://hal.univ-grenoble-alpes.fr/hal-01598604/file/acp-17-4539-2017.pdf doi:10.5194/acp-17-4539-2017 http://creativecommons.org/licenses/by-nc/ info:eu-repo/semantics/OpenAccess CC-BY-NC ISSN: 1680-7316 EISSN: 1680-7324 Atmospheric Chemistry and Physics https://hal.univ-grenoble-alpes.fr/hal-01598604 Atmospheric Chemistry and Physics, European Geosciences Union, 2017, 17 (7), pp.4539 - 4564. ⟨10.5194/acp-17-4539-2017⟩ [SPI.AUTO]Engineering Sciences [physics]/Automatic info:eu-repo/semantics/article Journal articles 2017 ftccsdartic https://doi.org/10.5194/acp-17-4539-2017 2021-11-07T00:22:26Z International audience N2O is currently the third most important anthropogenic greenhouse gas in terms of radiative forcing and its atmospheric mole fraction is rising steadily. To quantify the growth rate and its causes over the past decades, we performed a multi-site reconstruction of the atmospheric N2O mole fraction and isotopic composition using new and previously published firn air data collected from Greenland and Antarctica in combination with a firn diffusion and densification model. The multi-site reconstruction showed that while the global mean N2O mole fraction increased from (290 ± 1) nmol mol−1 in 1940 to (322 ± 1) nmol mol−1 in 2008, the isotopic composition of atmospheric N2O decreased by (−2.2 ± 0.2) ‰ for δ15Nav, (−1.0 ± 0.3) ‰ for δ18O, (−1.3 ± 0.6) ‰ for δ15Nα, and (−2.8 ± 0.6) ‰ for δ15Nβ over the same period. The detailed temporal evolution of the mole fraction and isotopic composition derived from the firn air model was then used in a two-box atmospheric model (comprising a stratospheric box and a tropospheric box) to infer changes in the isotopic source signature over time. The precise value of the source strength depends on the choice of the N2O lifetime, which we choose to fix at 123 years. The average isotopic composition over the investigated period is δ15Nav = (−7.6 ± 0.8) ‰ (vs. air-N2), δ18O = (32.2 ± 0.2) ‰ (vs. Vienna Standard Mean Ocean Water – VSMOW) for δ18O, δ15Nα = (−3.0 ± 1.9) ‰ and δ15Nβ = (−11.7 ± 2.3) ‰. δ15Nav, and δ15Nβ show some temporal variability, while for the other signatures the error bars of the reconstruction are too large to retrieve reliable temporal changes. Possible processes that may explain trends in 15N are discussed. The 15N site preference ( = δ15Nα − δ15Nβ) provides evidence of a shift in emissions from denitrification to nitrification, although the uncertainty envelopes are large. Article in Journal/Newspaper Antarc* Antarctica Greenland Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) Greenland Atmospheric Chemistry and Physics 17 7 4539 4564 |