Changes to the chemical state of the Northern Hemisphere atmosphere during the second half of the twentieth century
International audience The NOx (NO and NO2) and HOx (OH and HO2) budgets of the atmosphere exert a major influence on atmospheric composition, controlling removal of primary pollutants and formation of a wide range of secondary products, including ozone, that can influence human health and climate....
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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2017
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Online Access: | https://hal.univ-grenoble-alpes.fr/hal-01598584 https://hal.univ-grenoble-alpes.fr/hal-01598584/document https://hal.univ-grenoble-alpes.fr/hal-01598584/file/acp-17-8269-2017.pdf https://doi.org/10.5194/acp-17-8269-2017 |
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Institut national des sciences de l'Univers: HAL-INSU |
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English |
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[SPI.AUTO]Engineering Sciences [physics]/Automatic |
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[SPI.AUTO]Engineering Sciences [physics]/Automatic Newland, Mike Martinerie, Patricia Witrant, Emmanuel Helmig, Detlev Worton, David R. Hogan, Chris Sturges, William T. Reeves, Claire E. Changes to the chemical state of the Northern Hemisphere atmosphere during the second half of the twentieth century |
topic_facet |
[SPI.AUTO]Engineering Sciences [physics]/Automatic |
description |
International audience The NOx (NO and NO2) and HOx (OH and HO2) budgets of the atmosphere exert a major influence on atmospheric composition, controlling removal of primary pollutants and formation of a wide range of secondary products, including ozone, that can influence human health and climate. However, there remain large uncertainties in the changes to these budgets over recent decades. Due to their short atmospheric lifetimes, NOx and HOx are highly variable in space and time, and so the measurements of these species are of limited value for examining long-term, large-scale changes to their budgets. Here, we take an alternative approach by examining long-term atmospheric trends of alkyl nitrates, the production efficiency of which is dependent on the atmospheric [NO] ∕ [HO2] ratio. We derive long-term trends in the alkyl nitrates from measurements in firn air from the NEEM site, Greenland. Their mixing ratios increased by a factor of 3–5 between the 1970s and 1990s. This was followed by a steep decline to the sampling date of 2008. Moreover, we examine how the trends in the alkyl nitrates compare to similarly derived trends in their parent alkanes (i.e. the alkanes which, when oxidised in the presence of NOx, lead to the formation of the alkyl nitrates). The ratios of the alkyl nitrates to their parent alkanes increased from around 1970 to the late 1990s. This is consistent with large changes to the [NO] ∕ [HO2] ratio in the Northern Hemisphere atmosphere during this period. Alternatively, they could represent changes to concentrations of the hydroxyl radical, OH, or to the transport time of the air masses from source regions to the Arctic. |
author2 |
Centre for Ocean and Atmospheric, school of Environmental Sciences University of East Anglia Norwich (UEA) Institut des Géosciences de l’Environnement (IGE) Institut de Recherche pour le Développement (IRD)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 ) 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 National Polytechnique de Grenoble (INPG)-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 National Polytechnique de Grenoble (INPG)-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 National Polytechnique de Grenoble (INPG)-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 National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 ) Institute of Arctic Alpine Research University of Colorado Boulder (INSTAAR) University of Colorado Boulder National Physical Laboratory Teddington (NPL) |
format |
Article in Journal/Newspaper |
author |
Newland, Mike Martinerie, Patricia Witrant, Emmanuel Helmig, Detlev Worton, David R. Hogan, Chris Sturges, William T. Reeves, Claire E. |
author_facet |
Newland, Mike Martinerie, Patricia Witrant, Emmanuel Helmig, Detlev Worton, David R. Hogan, Chris Sturges, William T. Reeves, Claire E. |
author_sort |
Newland, Mike |
title |
Changes to the chemical state of the Northern Hemisphere atmosphere during the second half of the twentieth century |
title_short |
Changes to the chemical state of the Northern Hemisphere atmosphere during the second half of the twentieth century |
title_full |
Changes to the chemical state of the Northern Hemisphere atmosphere during the second half of the twentieth century |
title_fullStr |
Changes to the chemical state of the Northern Hemisphere atmosphere during the second half of the twentieth century |
title_full_unstemmed |
Changes to the chemical state of the Northern Hemisphere atmosphere during the second half of the twentieth century |
title_sort |
changes to the chemical state of the northern hemisphere atmosphere during the second half of the twentieth century |
publisher |
HAL CCSD |
publishDate |
2017 |
url |
https://hal.univ-grenoble-alpes.fr/hal-01598584 https://hal.univ-grenoble-alpes.fr/hal-01598584/document https://hal.univ-grenoble-alpes.fr/hal-01598584/file/acp-17-8269-2017.pdf https://doi.org/10.5194/acp-17-8269-2017 |
genre |
Arctic Greenland Human health |
genre_facet |
Arctic Greenland Human health |
op_source |
ISSN: 1680-7316 EISSN: 1680-7324 Atmospheric Chemistry and Physics https://hal.univ-grenoble-alpes.fr/hal-01598584 Atmospheric Chemistry and Physics, 2017, 17 (13), pp.8269-8283. ⟨10.5194/acp-17-8269-2017⟩ |
op_relation |
info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-17-8269-2017 hal-01598584 https://hal.univ-grenoble-alpes.fr/hal-01598584 https://hal.univ-grenoble-alpes.fr/hal-01598584/document https://hal.univ-grenoble-alpes.fr/hal-01598584/file/acp-17-8269-2017.pdf doi:10.5194/acp-17-8269-2017 |
op_rights |
http://creativecommons.org/licenses/by-nc/ info:eu-repo/semantics/OpenAccess |
op_doi |
https://doi.org/10.5194/acp-17-8269-2017 |
container_title |
Atmospheric Chemistry and Physics |
container_volume |
17 |
container_issue |
13 |
container_start_page |
8269 |
op_container_end_page |
8283 |
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spelling |
ftinsu:oai:HAL:hal-01598584v1 2024-04-28T08:11:36+00:00 Changes to the chemical state of the Northern Hemisphere atmosphere during the second half of the twentieth century Newland, Mike Martinerie, Patricia Witrant, Emmanuel Helmig, Detlev Worton, David R. Hogan, Chris Sturges, William T. Reeves, Claire E. Centre for Ocean and Atmospheric, school of Environmental Sciences University of East Anglia Norwich (UEA) Institut des Géosciences de l’Environnement (IGE) Institut de Recherche pour le Développement (IRD)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 ) 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 National Polytechnique de Grenoble (INPG)-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 National Polytechnique de Grenoble (INPG)-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 National Polytechnique de Grenoble (INPG)-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 National Polytechnique de Grenoble (INPG)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes 2016-2019 (UGA 2016-2019 ) Institute of Arctic Alpine Research University of Colorado Boulder (INSTAAR) University of Colorado Boulder National Physical Laboratory Teddington (NPL) 2017 https://hal.univ-grenoble-alpes.fr/hal-01598584 https://hal.univ-grenoble-alpes.fr/hal-01598584/document https://hal.univ-grenoble-alpes.fr/hal-01598584/file/acp-17-8269-2017.pdf https://doi.org/10.5194/acp-17-8269-2017 en eng HAL CCSD European Geosciences Union info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-17-8269-2017 hal-01598584 https://hal.univ-grenoble-alpes.fr/hal-01598584 https://hal.univ-grenoble-alpes.fr/hal-01598584/document https://hal.univ-grenoble-alpes.fr/hal-01598584/file/acp-17-8269-2017.pdf doi:10.5194/acp-17-8269-2017 http://creativecommons.org/licenses/by-nc/ info:eu-repo/semantics/OpenAccess ISSN: 1680-7316 EISSN: 1680-7324 Atmospheric Chemistry and Physics https://hal.univ-grenoble-alpes.fr/hal-01598584 Atmospheric Chemistry and Physics, 2017, 17 (13), pp.8269-8283. ⟨10.5194/acp-17-8269-2017⟩ [SPI.AUTO]Engineering Sciences [physics]/Automatic info:eu-repo/semantics/article Journal articles 2017 ftinsu https://doi.org/10.5194/acp-17-8269-2017 2024-04-05T00:38:39Z International audience The NOx (NO and NO2) and HOx (OH and HO2) budgets of the atmosphere exert a major influence on atmospheric composition, controlling removal of primary pollutants and formation of a wide range of secondary products, including ozone, that can influence human health and climate. However, there remain large uncertainties in the changes to these budgets over recent decades. Due to their short atmospheric lifetimes, NOx and HOx are highly variable in space and time, and so the measurements of these species are of limited value for examining long-term, large-scale changes to their budgets. Here, we take an alternative approach by examining long-term atmospheric trends of alkyl nitrates, the production efficiency of which is dependent on the atmospheric [NO] ∕ [HO2] ratio. We derive long-term trends in the alkyl nitrates from measurements in firn air from the NEEM site, Greenland. Their mixing ratios increased by a factor of 3–5 between the 1970s and 1990s. This was followed by a steep decline to the sampling date of 2008. Moreover, we examine how the trends in the alkyl nitrates compare to similarly derived trends in their parent alkanes (i.e. the alkanes which, when oxidised in the presence of NOx, lead to the formation of the alkyl nitrates). The ratios of the alkyl nitrates to their parent alkanes increased from around 1970 to the late 1990s. This is consistent with large changes to the [NO] ∕ [HO2] ratio in the Northern Hemisphere atmosphere during this period. Alternatively, they could represent changes to concentrations of the hydroxyl radical, OH, or to the transport time of the air masses from source regions to the Arctic. Article in Journal/Newspaper Arctic Greenland Human health Institut national des sciences de l'Univers: HAL-INSU Atmospheric Chemistry and Physics 17 13 8269 8283 |