Stratospheric Fluorine as a Tracer of Circulation Changes: Comparison Between Infrared Remote-Sensing Observations and Simulations With Five Modern Reanalyses

M. Prignon*, S. Chabrillat, M. Friedrich, D. Smale, S. E. Strahan, P. F. Bernath, M. P. Chipperfield, S. S. Dhomse, W. Feng, D. Minganti, C. Servais, E. Mahieu

*Corresponding author for this work

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Abstract

Using multidecadal time series of ground-based and satellite Fourier transform infrared measurements of inorganic fluorine (i.e., total fluorine resident in stratospheric fluorine reservoirs), we investigate stratospheric circulation changes over the past 20 years. The representation of these changes in five modern reanalyses is further analyzed through chemical-transport model (CTM) simulations. From the observations but also from all reanalyses, we show that the inorganic fluorine is accumulating less rapidly in the Southern Hemisphere than in the Northern Hemisphere during the 21st century. Comparisons with a study evaluating the age-of-air of these reanalyses using the same CTM allow us to link this hemispheric asymmetry to changes in the Brewer-Dobson circulation (BDC), with the age-of-air of the Southern Hemisphere getting younger relative to that of the Northern Hemisphere. Large differences in simulated total columns and absolute trend values are, nevertheless, depicted between our simulations driven by the five reanalyses. Superimposed on this multidecadal change, we, furthermore, confirm a 5–7-year variability of the BDC that was first described in a recent study analyzing long-term time series of hydrogen chloride (HCl) and nitric acid (HNO3). It is important to stress that our results, based on observations and meteorological reanalyses, are in contrast with the projections of chemistry-climate models in response to the coupled increase of greenhouse gases and decrease of ozone-depleting substances, calling for further investigations and the continuation of long-term observations.

Original languageEnglish
Article numbere2021JD034995
Pages (from-to)1-24
Number of pages24
JournalJournal of Geophysical Research: Atmospheres
Volume126
Issue number19
Early online date14 Sept 2021
DOIs
Publication statusPublished - 16 Oct 2021

Bibliographical note

Funding Information:
The authors are grateful to the International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG, Bern) for supporting the facilities needed to perform the FTIR observations at Jungfraujoch. Measurements at Lauder are core-funded by NIWA (program CAAC_2101) through New Zealand's Ministry of Business, Innovation, and Employment Strategic Science Investment Fund. The Atmospheric Chemistry Experiment mission is funded by the Canadian Space Agency. The authors thank the reanalysis centers (ECMWF, NASA GSFC, and JMA) for providing their support and data products. The TOMCAT modeling work was supported by the NERC SISLAC project (NE/R001782/1) and used the national Archer and Leeds ARC HPC facilities. S. E. Strahan thanks the NASA ACMA program for support. M. Prignon and D. Minganti were financially supported by the F.R.S.?FNRS (Brussels) through the ACCROSS research project (Grant no. PDR.T.0040.16). The University of Li?ge contribution was further supported by the GAW-CH program of MeteoSwiss and the F?d?ration Wallonie-Bruxelles. E. Mahieu is a senior research associate with the F.R.S.?FNRS. The authors thank Olivier Flock for their vital contribution to the maintenance of our infrastructures and to the FTIR observations. The authors further thank Yves Christophe and Quentin Errera (BIRA-IASB, Brussels, Belgium) for their contributions to the development of BASCOE.

Funding Information:
The authors are grateful to the International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG, Bern) for supporting the facilities needed to perform the FTIR observations at Jungfraujoch. Measurements at Lauder are core‐funded by NIWA (program CAAC_2101) through New Zealand's Ministry of Business, Innovation, and Employment Strategic Science Investment Fund. The Atmospheric Chemistry Experiment mission is funded by the Canadian Space Agency. The authors thank the reanalysis centers (ECMWF, NASA GSFC, and JMA) for providing their support and data products. The TOMCAT modeling work was supported by the NERC SISLAC project (NE/R001782/1) and used the national Archer and Leeds ARC HPC facilities. S. E. Strahan thanks the NASA ACMA program for support. M. Prignon and D. Minganti were financially supported by the F.R.S.—FNRS (Brussels) through the ACCROSS research project (Grant no. PDR.T.0040.16). The University of Liège contribution was further supported by the GAW‐CH program of MeteoSwiss and the Fédération Wallonie‐Bruxelles. E. Mahieu is a senior research associate with the F.R.S.—FNRS. The authors thank Olivier Flock for their vital contribution to the maintenance of our infrastructures and to the FTIR observations. The authors further thank Yves Christophe and Quentin Errera (BIRA‐IASB, Brussels, Belgium) for their contributions to the development of BASCOE.

Publisher Copyright:
© 2021. American Geophysical Union. All Rights Reserved.

Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.

Funding

The authors are grateful to the International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG, Bern) for supporting the facilities needed to perform the FTIR observations at Jungfraujoch. Measurements at Lauder are core-funded by NIWA (program CAAC_2101) through New Zealand's Ministry of Business, Innovation, and Employment Strategic Science Investment Fund. The Atmospheric Chemistry Experiment mission is funded by the Canadian Space Agency. The authors thank the reanalysis centers (ECMWF, NASA GSFC, and JMA) for providing their support and data products. The TOMCAT modeling work was supported by the NERC SISLAC project (NE/R001782/1) and used the national Archer and Leeds ARC HPC facilities. S. E. Strahan thanks the NASA ACMA program for support. M. Prignon and D. Minganti were financially supported by the F.R.S.?FNRS (Brussels) through the ACCROSS research project (Grant no. PDR.T.0040.16). The University of Li?ge contribution was further supported by the GAW-CH program of MeteoSwiss and the F?d?ration Wallonie-Bruxelles. E. Mahieu is a senior research associate with the F.R.S.?FNRS. The authors thank Olivier Flock for their vital contribution to the maintenance of our infrastructures and to the FTIR observations. The authors further thank Yves Christophe and Quentin Errera (BIRA-IASB, Brussels, Belgium) for their contributions to the development of BASCOE. The authors are grateful to the International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG, Bern) for supporting the facilities needed to perform the FTIR observations at Jungfraujoch. Measurements at Lauder are core‐funded by NIWA (program CAAC_2101) through New Zealand's Ministry of Business, Innovation, and Employment Strategic Science Investment Fund. The Atmospheric Chemistry Experiment mission is funded by the Canadian Space Agency. The authors thank the reanalysis centers (ECMWF, NASA GSFC, and JMA) for providing their support and data products. The TOMCAT modeling work was supported by the NERC SISLAC project (NE/R001782/1) and used the national Archer and Leeds ARC HPC facilities. S. E. Strahan thanks the NASA ACMA program for support. M. Prignon and D. Minganti were financially supported by the F.R.S.—FNRS (Brussels) through the ACCROSS research project (Grant no. PDR.T.0040.16). The University of Liège contribution was further supported by the GAW‐CH program of MeteoSwiss and the Fédération Wallonie‐Bruxelles. E. Mahieu is a senior research associate with the F.R.S.—FNRS. The authors thank Olivier Flock for their vital contribution to the maintenance of our infrastructures and to the FTIR observations. The authors further thank Yves Christophe and Quentin Errera (BIRA‐IASB, Brussels, Belgium) for their contributions to the development of BASCOE.

FundersFunder number
ECMWF
GAW‐CH program of MeteoSwiss
HFSJG
International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat
MeteoSwiss
Ministry of Business
NASA GSFC
National Aeronautics and Space Administration
National Institute of Water and Atmospheric ResearchCAAC_2101
Canadian Space Agency
Natural Environment Research CouncilNE/R001782/1
Fonds De La Recherche Scientifique - FNRSPDR.T.0040.16
Fédération Wallonie-Bruxelles

    Keywords

    • Brewer-Dobson circulation
    • circulation changes
    • stratospheric transport
    • trends

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