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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]

During the StratoClim Geophysica campaign, air with total water mixing ratios up to 200 ppmv and ozone up to 250 ppbv was observed within the Asian summer monsoon anticyclone up to 1.7 km above the local cold-point tropopause (CPT). To investigate the temporal evolution of enhanced water vapor being transported into the stratosphere, we conduct forward trajectory simulations using both a microphysical and an idealized freeze-drying model. The models are initialized at the measurement locations and the evolution of water vapor and ice is compared with satellite observations of MLS and CALIPSO. Our results show that these extremely high water vapor values observed above the CPT are very likely to undergo significant further freeze-drying due to experiencing extremely cold temperatures while circulating in the anticyclonic "dehydration carousel". We also use the Lagrangian dry point (LDP) of the merged back-and-forward trajectories to reconstruct the water vapor fields. The results show that the extremely high water vapor mixed with the stratospheric air has a negligible impact on the overall water vapor budget. The LDP mixing ratios are a better proxy for the large-scale water vapor distributions in the stratosphere during this period. [ABSTRACT FROM AUTHOR]

Carbonyl sulfide (OCS), the most abundant sulfur gas in the Earth's atmosphere, is a greenhouse gas, a precursor to stratospheric sulfate aerosol, and a proxy for terrestrial CO 2 uptake. Estimates of important OCS sources and sinks still have significant uncertainties and the global budget is not considered closed. One particularly uncertain source term, the OCS production during the atmospheric oxidation of dimethyl sulfide (DMS) emitted by the oceans, is addressed by a series of experiments in the atmospheric simulation chamber SAPHIR in conditions comparable to the remote marine atmosphere. DMS oxidation was initiated with OH and/or Cl radicals and DMS, OCS, and several oxidation products and intermediates were measured, including hydroperoxymethyl thioformate (HPMTF), which was recently found to play a key role in DMS oxidation in the marine atmosphere. One important finding is that the onset of HPMTF and OCS formation occurred faster than expected from the current chemical mechanisms. In agreement with other recent studies, OCS yields between 9 % and 12 % were observed in our experiments. Such yields are substantially higher than the 0.7 % yield measured in laboratory experiments in the 1990s, which is generally used to estimate the indirect OCS source from DMS in global budget estimates. However, we do not expect the higher yields found in our experiments to directly translate into a substantially higher OCS source from DMS oxidation in the real atmosphere, where conditions are highly variable, and, as pointed out in recent work, heterogeneous HPMTF loss is expected to effectively limit OCS production via this pathway. Together with other experimental studies, our results will be helpful to further elucidate the DMS oxidation chemical mechanism and in particular the paths leading to OCS formation. [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. 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]

Carbonyl sulfide (OCS), the most abundant sulfur gas in the Earth's atmosphere, is a greenhouse gas, a precursor to stratospheric sulfate aerosol, and a proxy for terrestrial CO2 uptake. Estimates of important OCS sources and sinks still bear significant uncertainties and the global budget is not considered closed. One particularly uncertain source term, the OCS production during the atmospheric oxidation of dimethyl sulfide (DMS) emitted by the oceans, is addressed by a series of experiments in the atmospheric simulation chamber SAPHIR at conditions comparable to the remote marine atmosphere. DMS oxidation was initiated with OH and/or Cl radicals and DMS, OCS and several oxidation products and intermediates were measured, including hydroperoxymethyl thioformate (HPMTF) that was recently found to play a key role in DMS oxidation in the marine atmosphere. One important finding is that the onset of HPMTF and OCS formation occurred faster than expected from the current chemical mechanisms. In agreement with other recent studies, OCS yields between 9 and 12 % were observed in our experiments. Such yields are substantially higher than the 0.7 % yield measured in laboratory experiments in the 1990s that is generally used to estimate the indirect OCS source from DMS in global budget estimates. However, we do not expect the higher yields found in our experiments to directly translate to a substantially higher OCS source from DMS oxidation in the real atmosphere, where conditions are highly variable and, as pointed out in recent work, heterogeneous HPMTF loss is expected to effectively limit OCS production via this pathway. Together with other experimental studies, our results will be helpful to further elucidate the DMS oxidation chemical mechanism and in particular the paths leading to OCS formation. [ABSTRACT FROM AUTHOR]

The Asian Monsoon Anticyclone (AMA) represents the wettest region in the lower stratosphere (LS) and is the key contributor to the global annual maximum in LS water vapour. While the AMA wet pool is linked with persistent convection in the region and horizontal confinement of the anticyclone, there remain ambiguities regarding the role of tropopause-overshooting convection in maintaining the regional LS water vapour maximum. This study tackles this issue using a unique set of observations from onboard the high-altitude M55-Geophysica aircraft deployed in Nepal in Summer 2017 within the EU StratoClim project. We use a combination of airborne measurements (water vapour, ice water, water isotopes, cloud backscatter) together with ensemble trajectory modeling coupled with satellite observations to characterize the processes controlling water vapour and clouds in the confined lower stratosphere (CLS) of AMA. Our analysis puts in evidence the dual role of overshooting convection, which may lead to hydration or dehydration depending on the synoptic-scale tropopause temperatures in AMA. We show that all of the observed CLS water vapour enhancements are traceable to convective events within AMA and furthermore bear an isotopic signature of the overshooting process. A surprising result is that the plumes of moist air with mixing ratios nearly twice the background level can persist for weeks whilst recirculating within the anticyclone, without being subject to irreversible dehydration through ice settling. Our findings highlight the importance of convection and recirculation within AMA for the transport of water into the stratosphere. [ABSTRACT FROM AUTHOR]

This study presents airborne in-situ and satellite remote sensing climatologies of cirrus clouds and humidity. The climatologies serve as a guide to the properties of cirrus clouds, with the new in-situ data base providing detailed insights into boreal mid-latitudes and the tropics, while the satellite-borne data set offers a global overview. To this end, an extensive, quality checked data archive, the Cirrus Guide II in-situ data base, is created from airborne in-situ measurements during 150 flights in 24 campaigns. The archive contains meteorological parameters, IWC, Nice, Rice, RHice and H2O for each of the flights (IWC: ice water content, Nice: number concentration of ice crystals, Rice: ice crystal mean mass radius, RHice: relative humidity with respect to ice, H2O: water vapor mixing ratio). Depending on the specific parameter, the data base has extended by about a factor of 5-10 compared to the previous studies of Schiller et al. (2008), JGR, and Krämer et al. (2009), ACP. One result of our investigations is, that across all latitudes, the thicker liquid origin cirrus predominate at lower altitudes, while at higher altitudes the thinner in-situ cirrus prevail. Further, exemplary investigations of the radiative characteristics of in-situ and liquid origin cirrus show that the in-situ origin cirrus only slightly warm the atmosphere, while liquid origin cirrus have a strong cooling effect. An important step in completing the Cirrus Guide II is the provision of the global cirrus Nice climatology, derived by means of the retrieval algorithm DARDAR-Nice from ten years of cirrus remote sensing observations from satellite. The in-situ data base has been used to evaluate and adjust the satellite observations. We found that the global median Nice from satellite observations is almost two times higher than the in-situ median and increases slightly with decreasing temperature. Nice medians of the most frequentl occuring cirrus sorted by geographical regions are highest in the tropics, followed by austral/boreal mid-latitudes, Antarctica and the Arctic. Since the satellite climatologies enclose the entire spatial and temporal Nice occurrence, we could deduce that half of the cirrus are located in the lowest, warmest cirrus layer and contain a significant amount of liquid origin cirrus. A specific highlight of the study is the in-situ observations of tropical tropopause layer (TTL) cirrus and humidity in the Asian monsoon anticyclone and the comparison to the surrounding tropics. In the convectively very active Asian monsoon, peak values of Nice and IWC of 30 ppmv and 1000 ppmv are detected around the cold point tropopause (CPT). Above the CPT, ice particles that are convectively injected can locally add a significant amount of water available for exchange with the stratosphere. We found IWCs of up to 8 ppmv in the Asian monsoon in comparison to only 2 ppmv in the surrounding tropics. Also, the highest RHice inside of the clouds as well as in clear sky (120-150 %) are observed around and above the CPT. We attribute this to the high amount of H2O (3-5 ppmv) in comparison to 1.5-3 ppmv in other tropical regions. The supersaturations above the CPT suggest that the water exchange with the stratosphere is 10-20 % higher than expected in regions of weak convective activity and up to about 50 % in the Asian monsoon. [ABSTRACT FROM AUTHOR]

The StratoClim stratospheric aircraft campaign took place in summer 2017 in Nepal (the 27th of July-10th of August) and provided a wide dataset of observations of air composition inside the Asian Monsoon Anticyclone. In the framework of this project, with the purpose of modelling the injection of pollutants and natural compounds into the stratosphere, we performed a series of diffusive back-trajectories runs along the flights' tracks. The availability of in-situ measurements of trace gases has been exploited to evaluate the capability of the trajectory system to reproduce the transport in the Upper Troposphere-Lower Stratosphere (UTLS) region. The diagnostics of the convective sources and mixing in the air parcel samples have been derived by integrating the trajectories output with high-resolution observations of cloud tops from the Meteosat Second Generation (MSG1) and Himawari geostationary satellites. Back-trajectories have been calculated using meteorological fields from European Centre for Medium-Range Weather Forecasts (ECMWF) Reanalysis (ERA-Interim and ERA-5) at 3 h and 1 h resolution, using both kinematic and diabatic vertical motion. The comparison among the different trajectory runs shows, in general, a higher consistency with observed data, as well as a better agreement between the diabatic and kinematic version, when using ERA-5 based runs with respect to ERA-Interim. Overall, a better capacity in reproducing the pollution features is finally found in the diabatic version of the ERA-5 runs. Adopting this setting for the analysis, a large variety of transport conditions have been individuated during the 8 flights of the campaign. The larger influence by convective injections is found from the continental sources of China and India. Only a small contribution appears to be originated from maritime regions, in particular the South Pacific and the Bay of Bengal that, unexpectedly, was not particularly active during the period of the campaign. Thin filamentary structures of polluted air, characterized by peaks in CO, are observed, mostly associated with young convective air (age less than a few days) and a predominant South-China origin. Observed air from continental India, on the contrary, is often linked to a lower concentration of the trace gas and to air masses that recirculated within the anticyclone for 10 to 20 days. Vertical stratification in the age of air is observed: up to 15 km, the age is less than 3 days and these fresh air masses constitute almost the totality of the air composition. A transition layer is then individuated between 15 km and 17 km, where the convective contribution is still dominant and the ages vary between one and two weeks. Above this level, the mean age of the air sampled by the aircraft is estimated to be 20 days. There, the convective contribution rapidly decreases with height, and finally became negligible around 20 km. [ABSTRACT FROM AUTHOR]