Abstract. Stratosphere–troposphere exchange (STE) is an important source oftropospheric 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 surfaceobservations, allowing us to follow stratospheric signals across thetropopause. The satellite-derived photochemical loss of N2O on annualand quasi-biennial cycles can be matched by the models. The STE flux ofN2O-depleted air in our chemistry transport model drives surfacevariability that closely matches observed fluctuations on both annual andquasi-biennial cycles, confirming the modeled flux. The observed tracercorrelations between N2O and O3 in the lowermost stratosphereprovide a hemispheric scaling of the N2O STE flux to that ofO3. For N2O and CFCl3, we model greater southern hemisphericSTE 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.
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CO2 surface variability: from the stratosphere or not?
Fluctuations in atmospheric CO2 can be measured with great precision and are used to identify human-driven sources as well as natural cycles of ocean and land carbon. One source of variability is the stratosphere, where the influx of aged CO2-depleted air can produce fluctuations at the surface. This process has been speculated to be a potential source of interannual variability (IAV) in CO2 that might obscure the quantification of other sources of IAV. Given the recent success in demonstrating that the stratospheric influx of N2O- and chlorofluorocarbon-depleted air is a dominant source of their surface IAV in the Southern Hemisphere, I apply the same model and measurement analysis here to CO2. Using chemistry-transport modeling or scaling of the observed N2O variability, I find that the stratosphere-driven surface variability in CO2 is at most 10% of the observed IAV and is not an important source. Diagnosing the amplitude of the CO2 annual cycle and its increase from 1985 to 2021 through the annual variance gives rates similar to traditional methods in the Northern Hemisphere (BRW, MLO) but can identify the emergence of small trends (0.08 ppm per decade) in the Southern Hemisphere (SMO, CGO).
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- Award ID(s):
- 2135749
- PAR ID:
- 10378448
- Editor(s):
- Ning Zeng
- Date Published:
- Journal Name:
- Earth system dynamics
- Volume:
- 13
- ISSN:
- 2190-4979
- Page Range / eLocation ID:
- 703-709
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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