From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone
Stratosphere–troposphere exchange (STE) is an important source of tropospheric ozone, affecting all of atmospheric chemistry, climate, and air quality. The study of impacts needs STE fluxes to be resolved by latitude and month, and for this, we rely on global chemistry models, whose results diverge...
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ftdoajarticles:oai:doaj.org/article:3c1b51f12d914a3f84ad93b56d73f174 2023-05-15T13:56:11+02:00 From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone D. J. Ruiz M. J. Prather 2022-02-01T00:00:00Z https://doi.org/10.5194/acp-22-2079-2022 https://doaj.org/article/3c1b51f12d914a3f84ad93b56d73f174 EN eng Copernicus Publications https://acp.copernicus.org/articles/22/2079/2022/acp-22-2079-2022.pdf https://doaj.org/toc/1680-7316 https://doaj.org/toc/1680-7324 doi:10.5194/acp-22-2079-2022 1680-7316 1680-7324 https://doaj.org/article/3c1b51f12d914a3f84ad93b56d73f174 Atmospheric Chemistry and Physics, Vol 22, Pp 2079-2093 (2022) Physics QC1-999 Chemistry QD1-999 article 2022 ftdoajarticles https://doi.org/10.5194/acp-22-2079-2022 2022-12-31T15:09:02Z Stratosphere–troposphere exchange (STE) is an important source of tropospheric ozone, affecting all of atmospheric chemistry, climate, and air quality. The study of impacts needs STE fluxes to be resolved by latitude and month, and for this, we rely on global chemistry models, whose results diverge greatly. Overall, we lack guidance from model–measurement metrics that inform us about processes and patterns related to the STE flux of ozone (O 3 ). In this work, we use modeled tracers (N 2 O and CFCl 3 ), whose distributions and budgets can be constrained by satellite and surface observations, allowing us to follow stratospheric signals across the tropopause. The satellite-derived photochemical loss of N 2 O on annual and quasi-biennial cycles can be matched by the models. The STE flux of N 2 O-depleted air in our chemistry transport model drives surface variability that closely matches observed fluctuations on both annual and quasi-biennial cycles, confirming the modeled flux. The observed tracer correlations between N 2 O and O 3 in the lowermost stratosphere provide a hemispheric scaling of the N 2 O STE flux to that of O 3 . For N 2 O and CFCl 3 , we model greater southern hemispheric STE fluxes, a result supported by some metrics, but counter to the prevailing theory of wave-driven stratospheric circulation. The STE flux of O 3 , however, is predominantly northern hemispheric, but evidence shows that this is caused by the Antarctic ozone hole reducing southern hemispheric O 3 STE by 14 %. Our best estimate of the current STE O 3 flux based on a range of constraints is 400 Tg(O 3 ) yr −1 , with a 1 σ uncertainty of ± 15 % and with a NH : SH ratio ranging from 50:50 to 60:40 . We identify a range of observational metrics that can better constrain the modeled STE O 3 flux in future assessments. Article in Journal/Newspaper Antarc* Antarctic Directory of Open Access Journals: DOAJ Articles Antarctic The Antarctic Atmospheric Chemistry and Physics 22 3 2079 2093 |
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Open Polar |
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Directory of Open Access Journals: DOAJ Articles |
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ftdoajarticles |
language |
English |
topic |
Physics QC1-999 Chemistry QD1-999 |
spellingShingle |
Physics QC1-999 Chemistry QD1-999 D. J. Ruiz M. J. Prather From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone |
topic_facet |
Physics QC1-999 Chemistry QD1-999 |
description |
Stratosphere–troposphere exchange (STE) is an important source of tropospheric ozone, affecting all of atmospheric chemistry, climate, and air quality. The study of impacts needs STE fluxes to be resolved by latitude and month, and for this, we rely on global chemistry models, whose results diverge greatly. Overall, we lack guidance from model–measurement metrics that inform us about processes and patterns related to the STE flux of ozone (O 3 ). In this work, we use modeled tracers (N 2 O and CFCl 3 ), whose distributions and budgets can be constrained by satellite and surface observations, allowing us to follow stratospheric signals across the tropopause. The satellite-derived photochemical loss of N 2 O on annual and quasi-biennial cycles can be matched by the models. The STE flux of N 2 O-depleted air in our chemistry transport model drives surface variability that closely matches observed fluctuations on both annual and quasi-biennial cycles, confirming the modeled flux. The observed tracer correlations between N 2 O and O 3 in the lowermost stratosphere provide a hemispheric scaling of the N 2 O STE flux to that of O 3 . For N 2 O and CFCl 3 , we model greater southern hemispheric STE fluxes, a result supported by some metrics, but counter to the prevailing theory of wave-driven stratospheric circulation. The STE flux of O 3 , however, is predominantly northern hemispheric, but evidence shows that this is caused by the Antarctic ozone hole reducing southern hemispheric O 3 STE by 14 %. Our best estimate of the current STE O 3 flux based on a range of constraints is 400 Tg(O 3 ) yr −1 , with a 1 σ uncertainty of ± 15 % and with a NH : SH ratio ranging from 50:50 to 60:40 . We identify a range of observational metrics that can better constrain the modeled STE O 3 flux in future assessments. |
format |
Article in Journal/Newspaper |
author |
D. J. Ruiz M. J. Prather |
author_facet |
D. J. Ruiz M. J. Prather |
author_sort |
D. J. Ruiz |
title |
From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone |
title_short |
From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone |
title_full |
From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone |
title_fullStr |
From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone |
title_full_unstemmed |
From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone |
title_sort |
from the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone |
publisher |
Copernicus Publications |
publishDate |
2022 |
url |
https://doi.org/10.5194/acp-22-2079-2022 https://doaj.org/article/3c1b51f12d914a3f84ad93b56d73f174 |
geographic |
Antarctic The Antarctic |
geographic_facet |
Antarctic The Antarctic |
genre |
Antarc* Antarctic |
genre_facet |
Antarc* Antarctic |
op_source |
Atmospheric Chemistry and Physics, Vol 22, Pp 2079-2093 (2022) |
op_relation |
https://acp.copernicus.org/articles/22/2079/2022/acp-22-2079-2022.pdf https://doaj.org/toc/1680-7316 https://doaj.org/toc/1680-7324 doi:10.5194/acp-22-2079-2022 1680-7316 1680-7324 https://doaj.org/article/3c1b51f12d914a3f84ad93b56d73f174 |
op_doi |
https://doi.org/10.5194/acp-22-2079-2022 |
container_title |
Atmospheric Chemistry and Physics |
container_volume |
22 |
container_issue |
3 |
container_start_page |
2079 |
op_container_end_page |
2093 |
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1766263560520859648 |