Investigating stratospheric changes between 2009 and 2018 with halogenated trace gas data from aircraft, AirCores, and a global model focusing on CFC-11
-
Published:2020-08-20
Issue:16
Volume:20
Page:9771-9782
-
ISSN:1680-7324
-
Container-title:Atmospheric Chemistry and Physics
-
language:en
-
Short-container-title:Atmos. Chem. Phys.
Author:
Laube Johannes C., Elvidge Emma C. Leedham, Adcock Karina E.ORCID, Baier Bianca, Brenninkmeijer Carl A. M., Chen HuilinORCID, Droste Elise S.ORCID, Grooß Jens-UweORCID, Heikkinen Pauli, Hind Andrew J., Kivi RigelORCID, Lojko Alexander, Montzka Stephen A.ORCID, Oram David E., Randall Steve, Röckmann ThomasORCID, Sturges William T., Sweeney ColmORCID, Thomas Max, Tuffnell ElinorORCID, Ploeger Felix
Abstract
Abstract. We present new observations of trace gases in the stratosphere
based on a cost-effective sampling technique that can access much higher
altitudes than aircraft. The further development of this method now provides
detection of species with abundances in the parts per trillion (ppt) range
and below. We obtain mixing ratios for six gases (CFC-11, CFC-12, HCFC-22,
H-1211, H-1301, and SF6), all of which are important for understanding
stratospheric ozone depletion and circulation. After demonstrating the
quality of the data through comparisons with ground-based records and
aircraft-based observations, we combine them with the latter to demonstrate
its potential. We first compare the data with results from a global model driven
by three widely used meteorological reanalyses. Secondly, we focus on CFC-11
as recent evidence has indicated renewed atmospheric emissions of that
species relevant on a global scale. Because the stratosphere represents the
main sink region for CFC-11, potential changes in stratospheric circulation
and troposphere–stratosphere exchange fluxes have been identified as the
largest source of uncertainty for the accurate quantification of such
emissions. Our observations span over a decade (up until 2018) and therefore
cover the period of the slowdown of CFC-11 global mixing ratio decreases
measured at the Earth's surface. The spatial and temporal coverage of the
observations is insufficient for a global quantitative analysis, but we do
find some trends that are in contrast with expectations, indicating that the
stratosphere may have contributed to the slower concentration decline in
recent years. Further investigating the reanalysis-driven model data, we find
that the dynamical changes in the stratosphere required to explain the
apparent change in tropospheric CFC-11 emissions after 2013 are possible
but with a very high uncertainty range. This is partly caused by the high
variability of mass flux from the stratosphere to the troposphere,
especially at timescales of a few years, and partly by large differences
between runs driven by different reanalysis products, none of which agree
with our observations well enough for such a quantitative analysis.
Funder
European Commission Helmholtz Association Natural Environment Research Council European Research Council
Publisher
Copernicus GmbH
Subject
Atmospheric Science
Reference41 articles.
1. Bönisch, H., Engel, A., Birner, Th., Hoor, P., Tarasick, D. W., and Ray,
E. A.: On the structural changes in the Brewer–Dobson circulation after
2000, Atmos. Chem. Phys., 11, 3937–3948,
https://doi.org/10.5194/acp-11-3937-2011, 2011. 2. Brenninkmeijer, C. A. M., Crutzen, P., Boumard, F., Dauer, T., Dix, B.,
Ebinghaus, R., Filippi, D., Fischer, H., Franke, H., Frieß, U.,
Heintzenberg, J., Helleis, F., Hermann, M., Kock, H. H., Koeppel, C.,
Lelieveld, J., Leuenberger, M., Martinsson, B. G., Miemczyk, S., Moret, H.
P., Nguyen, H. N., Nyfeler, P., Oram, D., O'Sullivan, D., Penkett, S.,
Platt, U., Pupek, M., Ramonet, M., Randa, B., Reichelt, M., Rhee, T. S.,
Rohwer, J., Rosenfeld, K., Scharffe, D., Schlager, H., Schumann, U., Slemr,
F., Sprung, D., Stock, P., Thaler, R., Valentino, F., van Velthoven,
P.,Waibel, A., Wandel, A., Waschitschek, K., Wiedensohler, A., Xueref-Remy,
I., Zahn, A., Zech, U., and Ziereis, H.: Civil Aircraft for the regular
investigation of the atmosphere based on an instrumented container: The new
CARIBIC system, Atmos. Chem. Phys., 7, 4953–4976,
https://doi.org/10.5194/acp-7-4953-2007, 2007. 3. Dee, D. P., Uppala, S. M., Simmons, A. J., Berrisford, P., Poli, P.,
Kobayashi, S., Andrae, U., Balmaseda, M. A., Balsamo, G.,
Bauer, P., Bechtold, P., Beljaars, A. C. M., van de Berg, L., Bidlot, J.,
Bormann, N., Delsol, C., Dragani, R., Fuentes, M., Geer, A. J., Haimberger,
L., Healy, S. B., Hersbach, H., Hólm, E. V., Isaksen, L., Kållberg,
P., Köhler, M., Matricardi, M., McNally, A. P., Monge-Sanz, B. M.,
Morcrette, J.-J., Park, B.-K., Peubey, C., de Rosnay, P., Tavolato, C.,
Thépaut, J.-N., and Vitart, F.: The ERA-Interim reanalysis:
configuration and performance of the data assimilation system, Q. J. Roy.
Meteor. Soc., 137, 553–597, https://doi.org/10.1002/qj.828, 2011. 4. Douglass, A. R., Stolarski, R. S., Schoeberl, M. R., Jackman, C. H., Gupta,
M. L., Newman, P. A., Nielsen, J. E., and Fleming, E. L.: Relationship of
loss, mean age of air and the distribution of CFCs to stratospheric
circulation and implications for atmospheric lifetimes, J. Geophys. Res.,
113, D14309, https://doi.org/10.1029/2007JD009575, 2008. 5. Engel, A., Mobius, T., Bönisch, H., Schmidt, U., Heinz, R., Levin, I.,
Atlas, E., Aoki, S., Nakazawa, T., Sugawara, S., Moore, F., Hurst, D.,
Elkins, J., Schauffler, S., Andrews, A., and Boering, K.: Age of
stratospheric air unchanged within uncertainties over the past 30 years,
Nat. Geosci., 2, 28–31, https://doi.org/10.1038/Ngeo388, 2009.
Cited by
9 articles.
订阅此论文施引文献
订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献
|
|