An official website of the United States government
The lifetime of tropospheric O3 is difficult to quantify because we model O3 as a secondary pollutant, without direct emissions. For other reactive greenhouse gases like CH4 and N2O, we readily model lifetimes and timescales that include chemical feedbacks based on direct emissions. Here, we devise a set of artificial experiments with a chemistry-transport model where O3 is directly emitted into the atmosphere at a quantified rate. We create 3 primary emission patterns for O3, mimicking secondary production by surface industrial pollution, that by aviation, and primary injection through stratosphere–troposphere exchange (STE). The perturbation lifetimes for these O3 sources includes chemical feedbacks and varies from 6 to 27 days depending on source location and season. Previous studies derived lifetimes around 24 days estimated from the mean odd-oxygen loss frequency. The timescales for decay of excess O3 varies from 10 to 20 days in northern hemisphere summer to 30 to 40 days in northern hemisphere winter. For each season, we identify a single O3 chemical mode applying to all experiments. Understanding how O3 sources accumulate (the lifetime) and disperse (decay timescale) provides some insight into how changes in pollution emissions, climate, and stratospheric O3 depletion over this century will alter tropospheric O3. This work incidentally found 2 distinct mistakes in how we diagnose tropospheric O3, but not how we model it. First, the chemical pattern of an O3 perturbation or decay mode does not resemble our traditional view of the odd-oxygen family of species that includes NO2. Instead, a positive O3 perturbation is accompanied by a decrease in NO2. Second, heretofore we diagnosed the importance of STE flux to tropospheric O3 with a synthetic “tagged” tracer O3S, which had full stratospheric chemistry and linear tropospheric loss based on odd-oxygen loss rates. These O3S studies predicted that about 40% of tropospheric O3 was of stratospheric origin, but our lifetime and decay experiments show clearly that STE fluxes add about 8% to tropospheric O3, providing further evidence that tagged tracers do not work when the tracer is a major species with chemical feedbacks on its loss rates, as shown previously for CH4.
more »
« less
From the middle stratosphere to the surface, using nitrous oxide to constrain the stratosphere–troposphere exchange of ozone
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.
more »
« less
- Award ID(s):
- 2135749
- PAR ID:
- 10384031
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 22
- Issue:
- 3
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 2079 to 2093
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract This study estimates the stratosphere–troposphere exchange (STE) of air masses and ozone concentrations averaged over 2007 to 2010 using the Modern Era Retrospective‐Analyses for Research and Applications 2 (MERRA2) and ERA5 reanalyses, and observations. The latter includes Microwave Limb Sounder (MLS) for ozone, MLS and Constellation Observing System for Meteorology, Ionosphere, and Climate (COSMIC) for temperatures, and A‐Train measurements for diabatic heating. The extratropical downward ozone fluxes are 538 Tg year−1from the ERA5 reanalysis, 543 Tg year−1from the MERRA2 reanalysis, and 528–539 Tg year−1from the observations, consistent with previous studies. Previous studies, however, did not consider tropical upward ozone flux. Here we show that the tropical upward ozone flux is 183–193 Tg year−1, which compensates about 35% of the extratropical downward ozone fluxes and should not be neglected. After considering the tropical upward ozone flux, the global ozone STE is 346 Tg year−1from the ERA5 reanalysis, 360 Tg year−1from the MERRA2 reanalysis, and 336–346 Tg year−1from the observations. Those estimates (347 ± 12 Tg year−1) can be used as the contribution of ozone STE to the tropospheric ozone budget. We also investigate cloud radiative effects on the STE of air mass and ozone. At 380 K, cloud radiative effects enhance downward fluxes in the extratropics from both reanalyses and observation, but reduce and enhance upward fluxes in the tropics from reanalyses and observation, respectively. The discrepancy in the tropics is related to the tropical tropopause layer thin cirrus that is missing in the reanalyses. We find that cloud radiative effects enhance the global ozone STE by about 21%–29%.more » « less
-
Abstract This study investigates changes in stratosphere‐troposphere exchange (STE) of air masses and ozone concentrations from 1960 to 2099 using multiple model simulations from Chemistry Climate Model Initiative (CCMI) under climate change scenario RCP6.0. We employ a lowermost stratosphere mass budget approach with dynamic isentropic surfaces fitted to the tropical tropopause as the upper boundary of lowermost stratosphere. The multi‐model mean (MMM) trends of air mass STEs are all small over all regions, which are within 0.3 (0.1) % decade−1for 1960–2000 (2000–2099). The MMM trends of ozone STE for 1960–2000 are 0.3%, −2.7%, 3.4%, −0.9%, and −2.7% decade−1over the Northern hemisphere (NH) extratropics, Southern hemisphere (SH) extratropics, tropics, extratropics, and globe, respectively. The corresponding ozone STE trends for 2000–2099 are 3.0%, 4.3%, 0.8%, 3.5%, and 4.7% decade−1. Changes in ozone STEs are dominated by ozone concentration changes, driven by climate‐induced changes and ozone‐depleting substance (ODS) changes. For 1960–2000, small changes in ozone STEs in the NH extratropics are due to a cancellation between effects of climate‐induced changes and ODS increases, while the ODS effect dominates in the SH extratropics, leading to a large ozone STE magnitude decrease. Increased ozone transport from tropical troposphere to stratosphere for 1960–2000 is due to increased tropospheric ozone. A decreased global ozone STE magnitude for 1960–2000 was largely caused by ODS‐induced ozone loss that is partly compensated by climate‐induced ozone changes. For 2000–2099, about two‐thirds of global ozone STE magnitude increases are caused by ozone increases in the extratropical lower stratosphere due to climate‐induced changes. The remaining one‐third is caused by ozone recovery due to the phaseout of ODS.more » « less
-
Ning Zeng (Ed.)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).more » « less
-
Abstract Stratosphere‐Troposphere exchange (STE) of air mass and ozone in ERA5 and Modern Era Retrospective analysis for Research and Application, version 2 (MERRA2) reanalyses from 1980 to 2022 are investigated on their seasonal cycle, annual‐mean climatology, and monthly anomalies smoothed using a 1‐year Lanczos low‐pass filter. We employ a lowermost stratosphere mass budget approach with dynamic isentropic surfaces fitted to tropical tropopause as the upper boundary of lowermost stratosphere. The annual‐mean ozone STEs over the NH extratropics, SH extratropics, tropics, extratropics, and globe in ERA5 are −342, −239, 201, −581, and −380 Tg year−1, respectively, versus −305, −224, 168, −529, −361 Tg year−1from MERRA2. The annual‐mean global ozone STE difference between ERA5 and MERRA2 is dominated by the diabatic heating difference, partly compensated by the ozone concentration difference. There are about 40% (−40%) differences between ERA5 and MERRA2 in global ozone STEs in boreal summer (autumn), mainly due to the difference in seasonal breathing of the lowermost stratosphere ozone mass between reanalyses. The correlation coefficient between ERA5 and MERRA2 global ozone mass STE monthly anomalies is 0.57 and thus ERA5 and MERRA2 can only explain each other's variance by 33%. Multiple linear regression analysis shows that El Niño–Southern Oscillation, quasi‐biennial oscillation, and Brewer‐Dobson circulation explain the variance in the ERA5 (MERRA2) global ozone STE monthly anomalies by 17.3 (5.0), 5.4 (7.2), and 1.0 (3.1)%, respectively. The volcanic aerosol impacts on ozone STEs from ERA5 and MERRA2 have opposite signs and thus are inconclusive. Cautions are therefore needed when using ERA5 and MERRA2 to investigate the STE seasonal cycle and interannual variability.more » « less
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.5194/acp-22-2079-2022
