From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone
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Published:2022-02-15
Issue:3
Volume:22
Page:2079-2093
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Ruiz Daniel J.ORCID, Prather Michael J.ORCID
Abstract
Abstract. 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 (O3). In this work, we use modeled tracers (N2O and CFCl3), 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 N2O on annual
and quasi-biennial cycles can be matched by the models. The STE flux of
N2O-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 N2O and O3 in the lowermost stratosphere
provide a hemispheric scaling of the N2O STE flux to that of
O3. For N2O and CFCl3, 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 O3, however, is predominantly northern hemispheric, but evidence shows that this is caused by the Antarctic ozone hole reducing southern hemispheric O3 STE by 14 %. Our best estimate of the current STE O3 flux based on a range of constraints is 400 Tg(O3) yr−1, with a 1σ 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 O3 flux in future assessments.
Funder
Directorate for Geosciences National Aeronautics and Space Administration
Publisher
Copernicus GmbH
Subject
Atmospheric Science
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