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Abstract We divide the atmosphere into distinct spheres based on their physical, chemical, and dynamical traits. In deriving chemical budgets and climate trends, which differ across spheres, we need clearly defined boundaries. Our primary spheres are the troposphere and stratosphere (∼99.9% by mass), and the boundary between them is the tropopause. Every global climate‐weather model has one or more methods to calculate the lapse rate tropopause, but these involve subjective choices and are known to fail near the sub‐tropical jets and polar regions. Age‐of‐air tracers clock the effective time‐distance from the tropopause, allowing unambiguous separation of stratosphere from troposphere in the chaotic jet regions. We apply a global model with synthetic tracer e90 (90‐day e‐folding), focusing on ozone and temperature structures about the tropopause using ozone sonde and satellite observations. We calibrate an observation‐consistent tropopause for e90 using tropics‐plus‐midlatitudes and then apply it globally to calculate total tropospheric air‐mass and tropopause ozone values. The tropopause mixing barrier for the current UCI CTM is identified by a transition in the vertical transport gradient to stratospheric values of 15 days km−1, corresponding to an e90 tropopause at 81 ± 2 ppb with a global tropospheric air mass of 82.2 ± 0.3%. The best e90 tropopause based on sonde pressures is 70–80 ppb; but that for ozone is 80–90 ppb, implying that the CTM tropopause ozone values are too large. This approach of calibrating an age‐of‐air tropopause can be readily applied to other models and possibly used with observed age‐of‐air tracers like sulfur hexafluoride.
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Age of air from ACE-FTS measurements of sulfur hexafluoride
Abstract. Climate models predict that the Brewer–Dobson circulation (BDC) will accelerate due to tropospheric warming, leading to a redistribution of trace gases and, consequently, to a change of the radiative properties of the atmosphere. Changes in the BDC are diagnosed by the so-called “age of air”, that is, the time since air in the stratosphere exited the troposphere. These changes can be derived from a long-term observation-based record of long-lived trace gases with increasing concentration in the troposphere, such as sulfur hexafluoride (SF6). The Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) provides the longest available continuous time series of vertically resolved SF6 measurements, spanning 2004 to the present. In this study, a new age-of-air product is derived from the ACE-FTS SF6 dataset. The ACE-FTS product is in good agreement with other observation-based age-of-air datasets and shows the expected global distribution of age-of-air values. Age of air from a chemistry–climate model is evaluated, and the linear trend of the observation-based age of air is calculated in 12 regions within the lower stratospheric midlatitudes (14–20 km, 40–70°) in each hemisphere. In 8 of 12 regions, there was not a statistically significant trend. The trends in the other regions, specifically 50–60 and 60–70° S at 17–20 km and 40–50° N at 14–17 and 17–20 km, are negative and significant to 2 standard deviations. This is therefore the first observation-based age-of-air trend study to suggest an acceleration of the shallow branch of the BDC, which transports air poleward in the lower stratosphere, in regions within both hemispheres.
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- Award ID(s):
- 2239242
- PAR ID:
- 10585192
- Publisher / Repository:
- Atmospheric Chemistry and Physics
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 25
- Issue:
- 7
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 4185 to 4209
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.5194/acp-25-4185-2025
