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Observational monitoring of the stratospheric transport circulation, the Brewer–Dobson circulation (BDC), is crucial to estimate any decadal to long-term changes therein, a prerequisite to interpret trends in stratospheric composition and to constrain the consequential impacts on climate. The transport time along the BDC (i.e. the mean stratospheric age of air, AoA) can best be deduced from trace gas measurements of tracers which increase linearly with time and are chemically passive. The gas sulfur hexafluoride (SF 6) is often used to deduce AoA because it has been increasing monotonically since the ∼ 1950s, and previously its chemical sinks in the mesosphere have been assumed to be negligible for AoA estimates. However, recent studies have shown that the chemical sinks of SF 6 are stronger than assumed and become increasingly relevant with rising SF 6 concentrations. To adjust biases in AoA that result from the chemical SF 6 sinks, we here propose a simple correction scheme for SF 6 -based AoA estimates accounting for the time-dependent effects of chemical sinks. The correction scheme is based on theoretical considerations with idealized assumptions, resulting in a relation between ideal AoA and apparent AoA which is a function of the tropospheric reference time series of SF 6 and of the AoA-dependent effective lifetime of SF 6. The correction method is thoroughly tested within a self-consistent data set from a climate model that includes explicit calculation of chemical SF 6 sinks. It is shown within the model that the correction successfully reduces biases in SF 6 -based AoA to less than 5 % for mean ages below 5 years. Tests using only subsampled data for deriving the fit coefficients show that applying the correction scheme even with imperfect knowledge of the sink is far superior to not applying a sink correction. Furthermore, we show that based on currently available measurements, we are not able to constrain the fit parameters of the correction scheme based on observational data alone. However, the model-based correction curve lies within the observational uncertainty, and we thus recommend using the model-derived fit coefficients until more high-quality measurements are able to further constrain the correction scheme. The application of the correction scheme to AoA from satellites and in situ data suggests that it is highly beneficial to reconcile different observational estimates of mean AoA. [ABSTRACT FROM AUTHOR]

Chemistry Climate Models (CCMs) are essential tools for characterizing and predicting the role of atmospheric composition and chemistry in Earth's climate system. This study demonstrates the use of airborne in situ observations to diagnose the representation of chemical composition and transport by CCMs. Process‐based diagnostics using dynamical and chemical coordinates are presented which minimize the spatial and temporal sampling differences between airborne in situ measurements and CCM grid points. The chosen process is the chemical impact of the Asian summer monsoon (ASM), where deep convection serves as a rapid transport pathway for surface emissions to reach the upper troposphere and lower stratosphere (UTLS). We examine two CCM configurations for their representation of the ASM UTLS using a set of airborne observations from south Asia. The diagnostics reveal good model performance at representing tropospheric tracer distribution throughout the troposphere and lower stratosphere, and excellent representation of chemical aging in the lower stratosphere when chemical loss is dominated by photolysis. Identified model limitations include the use of zonally averaged mole fraction boundary conditions for species with sufficiently short tropospheric lifetimes, which may obscure enhanced regional emissions sources. Overall, the diagnostics underscore the skill of current‐generation models at representing pollution transport from the boundary layer to the stratosphere via the ASM mechanism, and demonstrate the strength of airborne in situ observations toward characterizing this representation. Plain Language Summary: The chemical composition of Earth's atmosphere is important to understand for future climate prediction. This study establishes an approach for evaluating the representation of chemical composition in global climate models, and demonstrates the capabilities of the approach using a set of observations collected by research aircraft. We specifically target an evaluation of the Asian summer monsoon, a process with a well‐documented transport pathway for chemical species near the surface to reach the upper atmosphere. In doing so, we identify specific areas where focused model improvement is needed. Key Points: Process‐based diagnostics for model evaluation using airborne in situ observations are presentedThe Asian summer monsoon is explored for its role in impacting global composition and climateThe diagnostics use dynamical and chemical coordinates to identify model strengths and limitations [ABSTRACT FROM AUTHOR]

During the Asian monsoon season, greenhouse gases and pollution emitted near the ground are rapidly uplifted by convection up to an altitude of ∼ 13 km, with slower ascent and mixing with the stratospheric background above. Here, we address the robustness of the representation of these transport processes in different reanalysis data sets using ERA5, ERA-Interim and ERA5 1∘×1∘. This transport assessment includes the mean age of air from global three-dimensional simulations by the Lagrangian transport model CLaMS (Chemical Lagrangian Model of the Stratosphere), as well as different trajectory-based transport times and associated ascent rates compared with observation-based age of air and ascent rates of long-lived trace gases from airborne measurements during the Asian summer monsoon 2017 in Nepal. Our findings confirm that the ERA5 reanalysis yields a better representation of convection than ERA-Interim, resulting in different transport times and air mass origins at the Earth's surface. In the Asian monsoon region above 430 K, the mean age of air driven by ERA-Interim is too young, whereas the mean age of air from ERA5 1∘×1∘ is too old but somewhat closer to the observations. The mean effective ascent rates derived from ERA5 and ERA5 1∘×1∘ back trajectories are in good agreement with the observation-based mean ascent rates, unlike ERA-Interim, which is much faster above 430 K. Although a reliable CO2 reconstruction is a challenge for model simulations, we show that, up to 410 K, the CO2 reconstruction using ERA5 agrees best with high-resolution in situ aircraft CO2 measurements, indicating a better representation of Asian monsoon transport in the newest ECMWF reanalysis product, ERA5. [ABSTRACT FROM AUTHOR]

Observational monitoring of the stratospheric transport circulation, the Brewer-Dobson-Circulation (BDC), is crucial to estimate any decadal to long-term changes therein, a prerequisite to interpret trends in stratospheric composition and to constrain the consequential impacts on climate. The transport time along the BDC (i.e., the mean age of stratospheric air, AoA) can best be deduced from trace gas measurements of tracers which increase linearly in time and are chemically passive. The gas SF 6 is often used to deduce AoA, because it has been increasing monotonically since the ~1950s, and previously its chemical sinks in the mesosphere have been assumed to be negligible for AoA estimates. However, recent studies have shown that the chemical sinks of SF 6 are stronger than assumed, and become increasingly relevant with rising SF 6 concentrations. To adjust biases in AoA that result from the chemical SF 6 sinks, we here propose a simple correction scheme for SF 6-based AoA estimates accounting for the time-dependent effects of chemical sinks. The correction scheme is based on theoretical considerations with idealized assumptions, resulting in a relation between ideal AoA and apparent AoA which is a function of the tropospheric reference time-series of SF 6 and of the AoA-dependent effective lifetime of SF 6. The correction method is thoroughly tested within a self-consistent data set from a climate model that includes explicit calculation of chemical SF 6 sinks. It is shown within the model that the correction successfully reduces biases in SF 6-based AoA to less than 5 % for mean ages below 5 years. Tests with using only sub-sampled data for deriving the fit coefficients show that applying the correction scheme even with imperfect knowledge of the sink is far superior to not applying a sink correction. Further, we show that based on currently available measurements, we are not able to constrain the fit parameters of the correction scheme based on observational data alone. However, the model-based correction curve lies within the observational uncertainty, and we thus recommend to use the model-derived fit coefficients until more high-quality measurements will be able to further constrain the correction scheme. The application of the correction scheme to AoA from satellites and in-situ data suggests that it is highly beneficial to reconcile different observational estimates of mean AoA. [ABSTRACT FROM AUTHOR]

Atmospheric concentrations of many greenhouse gases especially CO2 are increasing globally. In particular the rapid increase of anthropogenic CO2 emissions in Asia contributes strongly to the acceleration of the CO2 growth rate in the atmosphere. During the Asian monsoon season, greenhouse gases as well as pollution emitted near the ground rapidly propagate up to an altitude of 13 km (~360 K potential temperature) with slower ascent and mixing with the stratospheric background above. However, CO2 sources in South Asia are poorly quantified. Here, differences in transport of air in the regions of the Asian summer monsoon 2017 were inferred using the Chemical Lagrangian Model of the Stratosphere (CLaMS) driven by three data sets, namely two ECMWF reanalyses in different resolutions (ERA-Interim, ERA5 and ERA5 1° x 1°). These model results are assessed using unique airborne measurements up to altitudes of ~20 km (~475 K) during the Asian summer monsoon 2017 conducted with the Geophysica aircraft during the StratoClim campaign in Nepal. Trajectory-based transport times, air mass source regions at the Earth's surface, mean effective ascent rates and age spectra as well as mean age of air from 3-dimensional CLaMS simulations are compared using the three data sets and evaluated by observation-based ascent rates. Our findings confirm that because of a better spatial and temporal resolution, ERA5 reanalysis yields a better representation of convection than ERA-Interim. Further, our findings show that transport times from the surface to the Asian monsoon anticyclone as well as the origin of air at the Earth's surface are both very sensitive to the used reanalysis. Above 430 K, the mean effective ascent rates derived from ERA5 back-trajectories and ERA5 1° x 1° (~0.2–0.3 K/day) are in good agreement with the observation-based mean ascent rates inferred from long-lived trace gases such as C2F6 and HFC-125 derived from air samples collected by the whole air sampler aboard Geophysica. Mean effective ascent rates derived from ERA-Interim back-trajectories are much faster ~0.5 K/day at these altitudes. In the Asian monsoon region at 470 K, mean age of air is larger than 3 years for ERA5 1° x 1° and about 2 years for ERA-Interim, whereas an observation-based age of air is up to 2.5 years. A reliable reconstruction (simulation) of vertical CO2 profiles during the Asian monsoon is a challenge for model simulations because the seasonal variability of CO2 at the ground, mixing with aged stratospheric air and the vertical velocities (including convection as well as vertical ascent caused by diabatic heating in the UTLS) have to be represented accurately in the simulations. Up to 410 K, the presented CO2 reconstruction agrees best with high-resolution in situ aircraft CO2 measurements using ERA5 compared to ERA5 1° x 1° and ERA-Interim, indicating a better representation of Asian monsoon transport for the newer ECMWF reanalysis product ERA5. Above 410 K the uncertainties of the CO2 reconstruction are increasing because of mixing with aged air. [ABSTRACT FROM AUTHOR]

The stratospheric meridional overturning circulation, also referred to as the Brewer-Dobson circulation (BDC), controls the composition of the stratosphere, which, in turn, affects radiation and climate. As the BDC cannot be directly measured, one has to infer its strength and trends indirectly. For instance, trace gas measurements allow the calculation of average transit times. Satellite measurements provide information on the distributions of trace gases for the entire stratosphere, with measurements of particularly long and dense coverage available for stratospheric water vapour (H2O). Although chemical processes and boundary conditions confound interpretation, the influence of CH4 oxidation on H2O is relatively straightforward, and thus H2O is an appealing tracer for transport analysis despite these caveats. In this work, we explore how mean age of air trends can be estimated from the combination of stratospheric H2O and CH4 data. We carry out different sensitivity studies with the Chemical Lagrangian Model of the Stratosphere (CLaMS) and focus on the analysis of the periods of 1990-2006 and 1990-2017. In particular, we assess the methodological uncertainties related to the two commonly-used approximations of (i) instantaneous stratospheric entry mixing ratio propagation, and (ii) constant correlation between mean age and the fractional release factor of methane. Our results show that the estimated mean age of air trends from the combination of observed stratospheric H2O and CH4 changes may be significantly affected by the assumed approximations. Depending on the investigated stratospheric region and the considered period, the error in estimated mean age of air decadal trends can be large - the discrepancies are up to 10 % per decade or even more at the lower stratosphere. For particular periods, the errors from the two approximations can lead to opposite effects, which may even cancel out. Finally, we propose an improvement to the approximation method by using an idealised age spectrum to propagate stratospheric entry mixing ratios. The findings of this work can be used for improving and assessing the uncertainties in stratospheric BDC trend estimation from global satellite measurements. [ABSTRACT FROM AUTHOR]

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 it 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 required 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 time scales 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. [ABSTRACT FROM AUTHOR]