Formulation of the cosmic ray–driven electron-induced reaction mechanism for quantitative understanding of global ozone depletion

This paper formulates the cosmic ray–driven electron-induced reaction as a universal mechanism to provide a quantitative understanding of global ozone depletion. Based on a proposed electrostatic bonding mechanism for charge-induced adsorption of molecules on surfaces and on the measured dissociativ...

Full description

Bibliographic Details
Published in:Proceedings of the National Academy of Sciences
Main Author: Lu, Qing-Bin
Format: Text
Language:English
Published: National Academy of Sciences 2023
Subjects:
Online Access:http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10319005/
http://www.ncbi.nlm.nih.gov/pubmed/37364123
https://doi.org/10.1073/pnas.2303048120
id ftpubmed:oai:pubmedcentral.nih.gov:10319005
record_format openpolar
spelling ftpubmed:oai:pubmedcentral.nih.gov:10319005 2024-01-28T10:01:02+01:00 Formulation of the cosmic ray–driven electron-induced reaction mechanism for quantitative understanding of global ozone depletion Lu, Qing-Bin 2023-06-26 http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10319005/ http://www.ncbi.nlm.nih.gov/pubmed/37364123 https://doi.org/10.1073/pnas.2303048120 en eng National Academy of Sciences http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10319005/ http://www.ncbi.nlm.nih.gov/pubmed/37364123 http://dx.doi.org/10.1073/pnas.2303048120 Copyright © 2023 the Author(s). Published by PNAS. https://creativecommons.org/licenses/by-nc-nd/4.0/This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND) (https://creativecommons.org/licenses/by-nc-nd/4.0/) . Proc Natl Acad Sci U S A Physical Sciences Text 2023 ftpubmed https://doi.org/10.1073/pnas.2303048120 2023-12-31T01:41:22Z This paper formulates the cosmic ray–driven electron-induced reaction as a universal mechanism to provide a quantitative understanding of global ozone depletion. Based on a proposed electrostatic bonding mechanism for charge-induced adsorption of molecules on surfaces and on the measured dissociative electron transfer (DET) cross sections of ozone-depleting substances (ODSs) adsorbed on ice, an analytical equation is derived to give atmospheric chlorine atom concentration: [Formula: see text] where Φ(e) is the prehydrated electron (e(pre)(−)) flux produced by cosmic ray ionization on atmospheric particle surfaces, [Formula: see text] is the surface coverage of an ODS, and k(i) is the ODS’s effective DET coefficient that is the product of the DET cross section, the lifetimes of surface-trapped e(pre)(−) and Cl(−), and the particle surface area density. With concentrations of ODSs as the sole variable, our calculated results of time-series ozone depletion rates in global regions in the 1960s, 1980s, and 2000s show generally good agreement with observations, particularly with ground-based ozonesonde data and satellite-measured data over Antarctica and with satellite data in a narrow altitude band at 13 to 20 km of the tropics. Good agreements with satellite data in the Arctic and midlatitudes are also found. A previously unreported effect of denitrification on ozone loss is found and expressed quantitatively. But this equation overestimates tropospheric ozone loss at northern midlatitudes and the Arctic, likely due to increased ozone production by the halogen chemistry in polluted regions. The results render confidence in applying the equation to achieve a quantitative understanding of global ozone depletion. Text Antarc* Antarctica Arctic PubMed Central (PMC) Arctic Proceedings of the National Academy of Sciences 120 27
institution Open Polar
collection PubMed Central (PMC)
op_collection_id ftpubmed
language English
topic Physical Sciences
spellingShingle Physical Sciences
Lu, Qing-Bin
Formulation of the cosmic ray–driven electron-induced reaction mechanism for quantitative understanding of global ozone depletion
topic_facet Physical Sciences
description This paper formulates the cosmic ray–driven electron-induced reaction as a universal mechanism to provide a quantitative understanding of global ozone depletion. Based on a proposed electrostatic bonding mechanism for charge-induced adsorption of molecules on surfaces and on the measured dissociative electron transfer (DET) cross sections of ozone-depleting substances (ODSs) adsorbed on ice, an analytical equation is derived to give atmospheric chlorine atom concentration: [Formula: see text] where Φ(e) is the prehydrated electron (e(pre)(−)) flux produced by cosmic ray ionization on atmospheric particle surfaces, [Formula: see text] is the surface coverage of an ODS, and k(i) is the ODS’s effective DET coefficient that is the product of the DET cross section, the lifetimes of surface-trapped e(pre)(−) and Cl(−), and the particle surface area density. With concentrations of ODSs as the sole variable, our calculated results of time-series ozone depletion rates in global regions in the 1960s, 1980s, and 2000s show generally good agreement with observations, particularly with ground-based ozonesonde data and satellite-measured data over Antarctica and with satellite data in a narrow altitude band at 13 to 20 km of the tropics. Good agreements with satellite data in the Arctic and midlatitudes are also found. A previously unreported effect of denitrification on ozone loss is found and expressed quantitatively. But this equation overestimates tropospheric ozone loss at northern midlatitudes and the Arctic, likely due to increased ozone production by the halogen chemistry in polluted regions. The results render confidence in applying the equation to achieve a quantitative understanding of global ozone depletion.
format Text
author Lu, Qing-Bin
author_facet Lu, Qing-Bin
author_sort Lu, Qing-Bin
title Formulation of the cosmic ray–driven electron-induced reaction mechanism for quantitative understanding of global ozone depletion
title_short Formulation of the cosmic ray–driven electron-induced reaction mechanism for quantitative understanding of global ozone depletion
title_full Formulation of the cosmic ray–driven electron-induced reaction mechanism for quantitative understanding of global ozone depletion
title_fullStr Formulation of the cosmic ray–driven electron-induced reaction mechanism for quantitative understanding of global ozone depletion
title_full_unstemmed Formulation of the cosmic ray–driven electron-induced reaction mechanism for quantitative understanding of global ozone depletion
title_sort formulation of the cosmic ray–driven electron-induced reaction mechanism for quantitative understanding of global ozone depletion
publisher National Academy of Sciences
publishDate 2023
url http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10319005/
http://www.ncbi.nlm.nih.gov/pubmed/37364123
https://doi.org/10.1073/pnas.2303048120
geographic Arctic
geographic_facet Arctic
genre Antarc*
Antarctica
Arctic
genre_facet Antarc*
Antarctica
Arctic
op_source Proc Natl Acad Sci U S A
op_relation http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10319005/
http://www.ncbi.nlm.nih.gov/pubmed/37364123
http://dx.doi.org/10.1073/pnas.2303048120
op_rights Copyright © 2023 the Author(s). Published by PNAS.
https://creativecommons.org/licenses/by-nc-nd/4.0/This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND) (https://creativecommons.org/licenses/by-nc-nd/4.0/) .
op_doi https://doi.org/10.1073/pnas.2303048120
container_title Proceedings of the National Academy of Sciences
container_volume 120
container_issue 27
_version_ 1789325731633823744