Constraining the propagation of the 17O-excess of ozone in the troposphere : Towards a quantitative interpretation of the oxygen isotopic composition of atmospheric nitrate
The unique and distinctive 17O-excess (Δ17O) of ozone (O3) serves as a valuable tracer for oxidative processes in both modern and ancient atmospheres. This isotopic signature is propagated throughout the atmospheric reactive nitrogen (NOx = NO + NO2) cycle and preserved in nitrate (NO3-) aerosols an...
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Other Authors: | , , , , |
Format: | Doctoral or Postdoctoral Thesis |
Language: | French |
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HAL CCSD
2013
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Online Access: | https://tel.archives-ouvertes.fr/tel-00856960 https://tel.archives-ouvertes.fr/tel-00856960v2/document https://tel.archives-ouvertes.fr/tel-00856960v2/file/pdf2star-1397485622-34090_VICARS_2013_archivage.pdf |
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ftccsdartic:oai:HAL:tel-00856960v2 |
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record_format |
openpolar |
institution |
Open Polar |
collection |
Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) |
op_collection_id |
ftccsdartic |
language |
French |
topic |
Atmospheric nitrate Ozone Nitrogen Oxygen Polar regions Atmospheric chemistry Climate Isotope anomalies Nitrate atmosphérique Anomalies isotopiques Climat Chimie atmosphérique Régions polaires Oxygène Azote [PHYS.COND.CM-GEN]Physics [physics]/Condensed Matter [cond-mat]/Other [cond-mat.other] |
spellingShingle |
Atmospheric nitrate Ozone Nitrogen Oxygen Polar regions Atmospheric chemistry Climate Isotope anomalies Nitrate atmosphérique Anomalies isotopiques Climat Chimie atmosphérique Régions polaires Oxygène Azote [PHYS.COND.CM-GEN]Physics [physics]/Condensed Matter [cond-mat]/Other [cond-mat.other] Vicars, William Constraining the propagation of the 17O-excess of ozone in the troposphere : Towards a quantitative interpretation of the oxygen isotopic composition of atmospheric nitrate |
topic_facet |
Atmospheric nitrate Ozone Nitrogen Oxygen Polar regions Atmospheric chemistry Climate Isotope anomalies Nitrate atmosphérique Anomalies isotopiques Climat Chimie atmosphérique Régions polaires Oxygène Azote [PHYS.COND.CM-GEN]Physics [physics]/Condensed Matter [cond-mat]/Other [cond-mat.other] |
description |
The unique and distinctive 17O-excess (Δ17O) of ozone (O3) serves as a valuable tracer for oxidative processes in both modern and ancient atmospheres. This isotopic signature is propagated throughout the atmospheric reactive nitrogen (NOx = NO + NO2) cycle and preserved in nitrate (NO3-) aerosols and mineral deposits, providing a conservative tracer for the relative importance of ozone and other key oxidants involved in NOx cycling. However, despite the intense research effort dedicated to the interpretation of Δ17O(NO3-) measurements, the atmospheric processes responsible for the transfer of Δ17O to nitrate and their overall influence on nitrate isotopic composition on different spatial and temporal scales are not well understood. Furthermore, due to the inherent complexity of extracting ozone from ambient air, the absolute magnitude and spatiotemporal variability of Δ17O(O3) remains poorly constrained, a problem that has confounded the interpretation of Δ17O measurements for over a decade. The research questions that have been pursued in this thesis were formulated to address these knowledge gaps. The primary analytical tool used was the bacterial denitrifier method followed by continuous-flow isotope ratio mass spectrometry (CF-IRMS), which allows for the comprehensive isotopic analysis of nitrate (i.e., δ15N, δ18O, Δ17O). This method was applied to the isotopic analysis of nitrate samples in two case studies: (i) an investigation of the diurnal and spatial features of atmospheric nitrate isotopic composition in coastal California; and (ii) a study of the seasonality and air-snow transfer of nitrate stable isotopes on the Antarctic plateau. Furthermore, the method was adapted to the isotopic characterization of ozone via chemical conversion of its terminal oxygen atoms to nitrate. During the course of this thesis, a large dataset of tropospheric Δ17O(O3) measurements has been obtained, including a full annual record from Grenoble, France (45 °N) and a ship-based latitudinal profile from 50 °S to 50 °N in the ... |
author2 |
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) Université de Grenoble Joël Savarino |
format |
Doctoral or Postdoctoral Thesis |
author |
Vicars, William |
author_facet |
Vicars, William |
author_sort |
Vicars, William |
title |
Constraining the propagation of the 17O-excess of ozone in the troposphere : Towards a quantitative interpretation of the oxygen isotopic composition of atmospheric nitrate |
title_short |
Constraining the propagation of the 17O-excess of ozone in the troposphere : Towards a quantitative interpretation of the oxygen isotopic composition of atmospheric nitrate |
title_full |
Constraining the propagation of the 17O-excess of ozone in the troposphere : Towards a quantitative interpretation of the oxygen isotopic composition of atmospheric nitrate |
title_fullStr |
Constraining the propagation of the 17O-excess of ozone in the troposphere : Towards a quantitative interpretation of the oxygen isotopic composition of atmospheric nitrate |
title_full_unstemmed |
Constraining the propagation of the 17O-excess of ozone in the troposphere : Towards a quantitative interpretation of the oxygen isotopic composition of atmospheric nitrate |
title_sort |
constraining the propagation of the 17o-excess of ozone in the troposphere : towards a quantitative interpretation of the oxygen isotopic composition of atmospheric nitrate |
publisher |
HAL CCSD |
publishDate |
2013 |
url |
https://tel.archives-ouvertes.fr/tel-00856960 https://tel.archives-ouvertes.fr/tel-00856960v2/document https://tel.archives-ouvertes.fr/tel-00856960v2/file/pdf2star-1397485622-34090_VICARS_2013_archivage.pdf |
geographic |
Antarctic The Antarctic |
geographic_facet |
Antarctic The Antarctic |
genre |
Antarc* Antarctic |
genre_facet |
Antarc* Antarctic |
op_source |
https://tel.archives-ouvertes.fr/tel-00856960 Autre [cond-mat.other]. Université de Grenoble, 2013. Français. ⟨NNT : 2013GRENU037⟩ |
op_relation |
NNT: 2013GRENU037 tel-00856960 https://tel.archives-ouvertes.fr/tel-00856960 https://tel.archives-ouvertes.fr/tel-00856960v2/document https://tel.archives-ouvertes.fr/tel-00856960v2/file/pdf2star-1397485622-34090_VICARS_2013_archivage.pdf |
op_rights |
info:eu-repo/semantics/OpenAccess |
_version_ |
1766263358452924416 |
spelling |
ftccsdartic:oai:HAL:tel-00856960v2 2023-05-15T13:56:06+02:00 Constraining the propagation of the 17O-excess of ozone in the troposphere : Towards a quantitative interpretation of the oxygen isotopic composition of atmospheric nitrate Transfert de l'anomalie isotopique portée par l'ozone dans la troposphère : vers une interprétation quantitative de la composition isotopique en oxygène du nitrate atmosphérique Vicars, William 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) Université de Grenoble Joël Savarino 2013-04-19 https://tel.archives-ouvertes.fr/tel-00856960 https://tel.archives-ouvertes.fr/tel-00856960v2/document https://tel.archives-ouvertes.fr/tel-00856960v2/file/pdf2star-1397485622-34090_VICARS_2013_archivage.pdf fr fre HAL CCSD NNT: 2013GRENU037 tel-00856960 https://tel.archives-ouvertes.fr/tel-00856960 https://tel.archives-ouvertes.fr/tel-00856960v2/document https://tel.archives-ouvertes.fr/tel-00856960v2/file/pdf2star-1397485622-34090_VICARS_2013_archivage.pdf info:eu-repo/semantics/OpenAccess https://tel.archives-ouvertes.fr/tel-00856960 Autre [cond-mat.other]. Université de Grenoble, 2013. Français. ⟨NNT : 2013GRENU037⟩ Atmospheric nitrate Ozone Nitrogen Oxygen Polar regions Atmospheric chemistry Climate Isotope anomalies Nitrate atmosphérique Anomalies isotopiques Climat Chimie atmosphérique Régions polaires Oxygène Azote [PHYS.COND.CM-GEN]Physics [physics]/Condensed Matter [cond-mat]/Other [cond-mat.other] info:eu-repo/semantics/doctoralThesis Theses 2013 ftccsdartic 2021-10-24T13:02:15Z The unique and distinctive 17O-excess (Δ17O) of ozone (O3) serves as a valuable tracer for oxidative processes in both modern and ancient atmospheres. This isotopic signature is propagated throughout the atmospheric reactive nitrogen (NOx = NO + NO2) cycle and preserved in nitrate (NO3-) aerosols and mineral deposits, providing a conservative tracer for the relative importance of ozone and other key oxidants involved in NOx cycling. However, despite the intense research effort dedicated to the interpretation of Δ17O(NO3-) measurements, the atmospheric processes responsible for the transfer of Δ17O to nitrate and their overall influence on nitrate isotopic composition on different spatial and temporal scales are not well understood. Furthermore, due to the inherent complexity of extracting ozone from ambient air, the absolute magnitude and spatiotemporal variability of Δ17O(O3) remains poorly constrained, a problem that has confounded the interpretation of Δ17O measurements for over a decade. The research questions that have been pursued in this thesis were formulated to address these knowledge gaps. The primary analytical tool used was the bacterial denitrifier method followed by continuous-flow isotope ratio mass spectrometry (CF-IRMS), which allows for the comprehensive isotopic analysis of nitrate (i.e., δ15N, δ18O, Δ17O). This method was applied to the isotopic analysis of nitrate samples in two case studies: (i) an investigation of the diurnal and spatial features of atmospheric nitrate isotopic composition in coastal California; and (ii) a study of the seasonality and air-snow transfer of nitrate stable isotopes on the Antarctic plateau. Furthermore, the method was adapted to the isotopic characterization of ozone via chemical conversion of its terminal oxygen atoms to nitrate. During the course of this thesis, a large dataset of tropospheric Δ17O(O3) measurements has been obtained, including a full annual record from Grenoble, France (45 °N) and a ship-based latitudinal profile from 50 °S to 50 °N in the ... Doctoral or Postdoctoral Thesis Antarc* Antarctic Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) Antarctic The Antarctic |