Pollution trace gas distributions and their transport in the Asian monsoon upper troposphere and lowermost stratosphere during the StratoClim campaign 2017
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Published:2020-12-02
Issue:23
Volume:20
Page:14695-14715
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Johansson SörenORCID, Höpfner MichaelORCID, Kirner OliverORCID, Wohltmann IngoORCID, Bucci SilviaORCID, Legras BernardORCID, Friedl-Vallon FelixORCID, Glatthor Norbert, Kretschmer ErikORCID, Ungermann JörnORCID, Wetzel Gerald
Abstract
Abstract. We present the first high-resolution measurements of pollutant trace gases in the Asian summer monsoon upper troposphere and lowermost stratosphere (UTLS) from the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) during the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) campaign based in Kathmandu, Nepal, 2017. Measurements of peroxyacetyl nitrate (PAN), acetylene (C2H2), and formic acid (HCOOH) show strong local enhancements up to altitudes of 16 km. More than 500 pptv of PAN, more than 200 pptv of C2H2, and more than 200 pptv of HCOOH are observed. Air masses with increased volume mixing ratios of PAN and C2H2 at altitudes up to 18 km, reaching to the lowermost stratosphere, were present at these altitudes for more than 10 d, as indicated by trajectory analysis. A local minimum of HCOOH is correlated with a previously reported maximum of ammonia (NH3), which suggests different washout efficiencies of these species in the same air masses.
A backward trajectory analysis based on the models Alfred Wegener InsTitute LAgrangian Chemistry/Transport System (ATLAS) and TRACZILLA, using advanced techniques for detection of convective events, and starting at geolocations of GLORIA measurements with enhanced pollution trace gas concentrations, has been performed. The analysis shows that convective events along trajectories leading to GLORIA measurements with enhanced pollutants are located close to regions where satellite measurements by the Ozone Monitoring Instrument (OMI) indicate enhanced tropospheric columns of nitrogen dioxide (NO2) in the days prior to the observation.
A comparison to the global atmospheric models Copernicus Atmosphere Monitoring Service (CAMS) and ECHAM/MESSy Atmospheric Chemistry (EMAC) has been performed. It is shown that these models are able to reproduce large-scale structures of the pollution trace gas distributions for one part of the flight, while the other part of the flight reveals large discrepancies between models and measurement. These discrepancies possibly result from convective events that are not resolved or parameterized in the models, uncertainties in the emissions of source gases, and uncertainties in the rate constants of chemical reactions.
Funder
European Commission
Publisher
Copernicus GmbH
Subject
Atmospheric Science
Reference105 articles.
1. Bian, J., Pan, L. L., Paulik, L., Vömel, H., Chen, H., and Lu, D.: In situ
water vapor and ozone measurements in Lhasa and Kunming during the Asian
summer monsoon, Geophys. Res. Lett., 39, L19808, https://doi.org/10.1029/2012GL052996,
2012. a 2. Bourtsoukidis, E., Helleis, F., Tomsche, L., Fischer, H., Hofmann, R., Lelieveld, J., and Williams, J.: An aircraft gas chromatograph–mass spectrometer System for Organic Fast Identification Analysis (SOFIA): design, performance and a case study of Asian monsoon pollution outflow, Atmos. Meas. Tech., 10, 5089–5105, https://doi.org/10.5194/amt-10-5089-2017, 2017. a 3. Bozem, H., Butler, T. M., Lawrence, M. G., Harder, H., Martinez, M., Kubistin, D., Lelieveld, J., and Fischer, H.: Chemical processes related to net ozone tendencies in the free troposphere, Atmos. Chem. Phys., 17, 10565–10582, https://doi.org/10.5194/acp-17-10565-2017, 2017. a, b 4. Brasseur, G. and Solomon, S.: Aeronomy of the middle atmosphere: Chemistry and
physics of the stratosphere and mesosphere, Vol. 32 of Atmospheric and
oceanographic sciences library,
3rd rev., Springer, Dordrecht and Great Britain, 2005. a, b, c 5. Braun, M., Grooß, J.-U., Woiwode, W., Johansson, S., Höpfner, M., Friedl-Vallon, F., Oelhaf, H., Preusse, P., Ungermann, J., Sinnhuber, B.-M., Ziereis, H., and Braesicke, P.: Nitrification of the lowermost stratosphere during the exceptionally cold Arctic winter 2015–2016, Atmos. Chem. Phys., 19, 13681–13699, https://doi.org/10.5194/acp-19-13681-2019, 2019. a
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