The chemistry of high reactive species and their role on the oxidative capacity at polar regions
Over the last two decades, the paradigm of snow as an inert material has been challenged by the discovery of substantial chemical activity within the snowpack and, in particular, its elevated nitrogen oxides content. When sunlight resumes at the end of the polar night, it triggers photochemistry wit...
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ftccsdartic:oai:HAL:tel-03329000v1 2023-05-15T13:35:00+02:00 The chemistry of high reactive species and their role on the oxidative capacity at polar regions Chimie des espèces réactives et leur rôle sur la capacité oxydante en régions polaires Barbero, Albane Institut des Géosciences de l’Environnement (IGE) Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ) Université Grenoble Alpes (UGA) Université Grenoble Alpes 2020-. Joël Savarino Roberto Grilli 2021-06-11 https://tel.archives-ouvertes.fr/tel-03329000 https://tel.archives-ouvertes.fr/tel-03329000/document https://tel.archives-ouvertes.fr/tel-03329000/file/BARBERO_2021_archivage.pdf en eng HAL CCSD NNT: 2021GRALU018 tel-03329000 https://tel.archives-ouvertes.fr/tel-03329000 https://tel.archives-ouvertes.fr/tel-03329000/document https://tel.archives-ouvertes.fr/tel-03329000/file/BARBERO_2021_archivage.pdf info:eu-repo/semantics/OpenAccess https://tel.archives-ouvertes.fr/tel-03329000 Earth Sciences. Université Grenoble Alpes [2020-.], 2021. English. ⟨NNT : 2021GRALU018⟩ Atmosphere Halogenated compounds Oxidants Snow Nitrogen compounds Oxydative capacity Photochemestry Polar regions Régions polaires Photochimie Capacité oxydante Atmosphère Composés halogènes Oxydants Neige Composés azotés [SDU.STU]Sciences of the Universe [physics]/Earth Sciences info:eu-repo/semantics/doctoralThesis Theses 2021 ftccsdartic 2021-10-23T22:56:11Z Over the last two decades, the paradigm of snow as an inert material has been challenged by the discovery of substantial chemical activity within the snowpack and, in particular, its elevated nitrogen oxides content. When sunlight resumes at the end of the polar night, it triggers photochemistry within the porous snowpack. The highly reactive products of this photochemistry can be exchanged between snow and atmosphere, and these exchanges will redistribute the species governing the oxidizing capacity of the atmosphere.Many studies that sought to better understand these polar processes have shown that: i) highly reactive species (such as NO_x, OH, HO_2, RO_2, and XO) play a key role in such a remote environment, controlling the oxidative capacity and the atmospheric chemistry and ii) snow emissions also locally control the oxidative capacity. Indeed, gaseous nitrogen species, especially nitrogen oxides NO_x (NO_x equiv NO + NO_2), emitted from the photolysis of nitrate contained in the snowpack, lead to a strong production of O_3 and OH radicals in the atmosphere. Unfortunately, these mechanisms are still poorly understood due to the lack of information on the behavior of nitrate in snow and the absence of direct measurements of NO_2 at the snow-atmosphere interface.First, we applied a NO_x measurement technique based on incoherent broadband cavity enhanced absorption spectroscopy (IBBCEAS) that is different from those previously used in Antarctica. This technique allows direct measurement of NO_2 and NO_x, and thus it reduces concentration level uncertainties. We developed, tested, and validated two robust instruments, for NO_2 and NO_x detection, respectively, that reached detection limits around 30 times 10^{-12} mol mol^{-1} (3sigma) and we deployed these instruments in the Antarctic field at Dome C.Two hypotheses explain the behavior of nitrate in the snowpack facing the absorption of a photon. The first one, commonly accepted, assumes the existence of two nitrate fractions: one subject to photolysis and the ... Doctoral or Postdoctoral Thesis Antarc* Antarctic Antarctica polar night Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) Antarctic The Antarctic |
institution |
Open Polar |
collection |
Archive ouverte HAL (Hyper Article en Ligne, CCSD - Centre pour la Communication Scientifique Directe) |
op_collection_id |
ftccsdartic |
language |
English |
topic |
Atmosphere Halogenated compounds Oxidants Snow Nitrogen compounds Oxydative capacity Photochemestry Polar regions Régions polaires Photochimie Capacité oxydante Atmosphère Composés halogènes Oxydants Neige Composés azotés [SDU.STU]Sciences of the Universe [physics]/Earth Sciences |
spellingShingle |
Atmosphere Halogenated compounds Oxidants Snow Nitrogen compounds Oxydative capacity Photochemestry Polar regions Régions polaires Photochimie Capacité oxydante Atmosphère Composés halogènes Oxydants Neige Composés azotés [SDU.STU]Sciences of the Universe [physics]/Earth Sciences Barbero, Albane The chemistry of high reactive species and their role on the oxidative capacity at polar regions |
topic_facet |
Atmosphere Halogenated compounds Oxidants Snow Nitrogen compounds Oxydative capacity Photochemestry Polar regions Régions polaires Photochimie Capacité oxydante Atmosphère Composés halogènes Oxydants Neige Composés azotés [SDU.STU]Sciences of the Universe [physics]/Earth Sciences |
description |
Over the last two decades, the paradigm of snow as an inert material has been challenged by the discovery of substantial chemical activity within the snowpack and, in particular, its elevated nitrogen oxides content. When sunlight resumes at the end of the polar night, it triggers photochemistry within the porous snowpack. The highly reactive products of this photochemistry can be exchanged between snow and atmosphere, and these exchanges will redistribute the species governing the oxidizing capacity of the atmosphere.Many studies that sought to better understand these polar processes have shown that: i) highly reactive species (such as NO_x, OH, HO_2, RO_2, and XO) play a key role in such a remote environment, controlling the oxidative capacity and the atmospheric chemistry and ii) snow emissions also locally control the oxidative capacity. Indeed, gaseous nitrogen species, especially nitrogen oxides NO_x (NO_x equiv NO + NO_2), emitted from the photolysis of nitrate contained in the snowpack, lead to a strong production of O_3 and OH radicals in the atmosphere. Unfortunately, these mechanisms are still poorly understood due to the lack of information on the behavior of nitrate in snow and the absence of direct measurements of NO_2 at the snow-atmosphere interface.First, we applied a NO_x measurement technique based on incoherent broadband cavity enhanced absorption spectroscopy (IBBCEAS) that is different from those previously used in Antarctica. This technique allows direct measurement of NO_2 and NO_x, and thus it reduces concentration level uncertainties. We developed, tested, and validated two robust instruments, for NO_2 and NO_x detection, respectively, that reached detection limits around 30 times 10^{-12} mol mol^{-1} (3sigma) and we deployed these instruments in the Antarctic field at Dome C.Two hypotheses explain the behavior of nitrate in the snowpack facing the absorption of a photon. The first one, commonly accepted, assumes the existence of two nitrate fractions: one subject to photolysis and the ... |
author2 |
Institut des Géosciences de l’Environnement (IGE) Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP ) Université Grenoble Alpes (UGA) Université Grenoble Alpes 2020-. Joël Savarino Roberto Grilli |
format |
Doctoral or Postdoctoral Thesis |
author |
Barbero, Albane |
author_facet |
Barbero, Albane |
author_sort |
Barbero, Albane |
title |
The chemistry of high reactive species and their role on the oxidative capacity at polar regions |
title_short |
The chemistry of high reactive species and their role on the oxidative capacity at polar regions |
title_full |
The chemistry of high reactive species and their role on the oxidative capacity at polar regions |
title_fullStr |
The chemistry of high reactive species and their role on the oxidative capacity at polar regions |
title_full_unstemmed |
The chemistry of high reactive species and their role on the oxidative capacity at polar regions |
title_sort |
chemistry of high reactive species and their role on the oxidative capacity at polar regions |
publisher |
HAL CCSD |
publishDate |
2021 |
url |
https://tel.archives-ouvertes.fr/tel-03329000 https://tel.archives-ouvertes.fr/tel-03329000/document https://tel.archives-ouvertes.fr/tel-03329000/file/BARBERO_2021_archivage.pdf |
geographic |
Antarctic The Antarctic |
geographic_facet |
Antarctic The Antarctic |
genre |
Antarc* Antarctic Antarctica polar night |
genre_facet |
Antarc* Antarctic Antarctica polar night |
op_source |
https://tel.archives-ouvertes.fr/tel-03329000 Earth Sciences. Université Grenoble Alpes [2020-.], 2021. English. ⟨NNT : 2021GRALU018⟩ |
op_relation |
NNT: 2021GRALU018 tel-03329000 https://tel.archives-ouvertes.fr/tel-03329000 https://tel.archives-ouvertes.fr/tel-03329000/document https://tel.archives-ouvertes.fr/tel-03329000/file/BARBERO_2021_archivage.pdf |
op_rights |
info:eu-repo/semantics/OpenAccess |
_version_ |
1766060037109710848 |