首页 » 文章 » 文章详细信息
Atmospheric Chemistry and Physics Volume 20 ,Issue 23 ,2020-12-02
Pollution trace gas distributions and their transport in the Asian monsoon upper troposphere and lowermost stratosphere during the StratoClim campaign 2017
Sören Johansson 1 Michael Höpfner 1 Oliver Kirner 2 Ingo Wohltmann 3 Silvia Bucci 4 Bernard Legras 4 Felix Friedl-Vallon 1 Norbert Glatthor 1 Erik Kretschmer 1 Jörn Ungermann 5 Gerald Wetzel 1
Show affiliations

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.


Copyright: © 2020 Sören Johansson et al.
This work is licensed under the Creative Commons Attribution 4.0 International License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/4.0/


Sören Johansson,Michael Höpfner,Oliver Kirner,Ingo Wohltmann,Silvia Bucci,Bernard Legras,Felix Friedl-Vallon,Norbert Glatthor,Erik Kretschmer,Jörn Ungermann,Gerald Wetzel. Pollution trace gas distributions and their transport in the Asian monsoon upper troposphere and lowermost stratosphere during the StratoClim campaign 2017. Atmospheric Chemistry and Physics ,Vol.20, Issue 23(2020)



[1] Morcrette, J., Boucher, O., Jones, L., Salmond, D., Bechtold, P., Beljaars, A.,Benedetti, A., Bonet, A., Kaiser, J. W., Razinger, M., Schulz, M., Serrar,S., Simmons, A. J., Sofiev, M., Suttie, M., Tompkins, A. M., and Untch, A.:Aerosol analysis and forecast in the European Centre for Medium‐RangeWeather Forecasts Integrated Forecast System: Forward modeling, J. Geophys. Res.-Atmos., 114, D06206, https://doi.org/10.1029/2008JD011235,2009. a
[2] Monks, S. A., Wilson, C., Emmons, L. K., Hannigan, J. W., Helmig, D., Blake,N. J., and Blake, D. R.: Using an Inverse Model to Reconcile Differences inSimulated and Observed Global Ethane Concentrations and Trends Between 2008and 2014, J. Geophys. Res.-Atmos., 123, 11262–11282,https://doi.org/10.1029/2017JD028112,2018. a
[3] Millet, D. B., Baasandorj, M., Farmer, D. K., Thornton, J. A., Baumann, K., Brophy, P., Chaliyakunnel, S., de Gouw, J. A., Graus, M., Hu, L., Koss, A., Lee, B. H., Lopez-Hilfiker, F. D., Neuman, J. A., Paulot, F., Peischl, J., Pollack, I. B., Ryerson, T. B., Warneke, C., Williams, B. J., and Xu, J.: A large and ubiquitous source of atmospheric formic acid, Atmos. Chem. Phys., 15, 6283–6304, https://doi.org/10.5194/acp-15-6283-2015, 2015. a
[4] Inness, A., Blechschmidt, A.-M., Bouarar, I., Chabrillat, S., Crepulja, M., Engelen, R. J., Eskes, H., Flemming, J., Gaudel, A., Hendrick, F., Huijnen, V., Jones, L., Kapsomenakis, J., Katragkou, E., Keppens, A., Langerock, B., de Mazière, M., Melas, D., Parrington, M., Peuch, V. H., Razinger, M., Richter, A., Schultz, M. G., Suttie, M., Thouret, V., Vrekoussis, M., Wagner, A., and Zerefos, C.: Data assimilation of satellite-retrieved ozone, carbon monoxide and nitrogen dioxide with ECMWF's Composition-IFS, Atmos. Chem. Phys., 15, 5275–5303, https://doi.org/10.5194/acp-15-5275-2015, 2015. a
[5] Wolff, M. A., Kerzenmacher, T., Strong, K., Walker, K. A., Toohey, M., Dupuy, E., Bernath, P. F., Boone, C. D., Brohede, S., Catoire, V., von Clarmann, T., Coffey, M., Daffer, W. H., De Mazière, M., Duchatelet, P., Glatthor, N., Griffith, D. W. T., Hannigan, J., Hase, F., Höpfner, M., Huret, N., Jones, N., Jucks, K., Kagawa, A., Kasai, Y., Kramer, I., Küllmann, H., Kuttippurath, J., Mahieu, E., Manney, G., McElroy, C. T., McLinden, C., Mébarki, Y., Mikuteit, S., Murtagh, D., Piccolo, C., Raspollini, P., Ridolfi, M., Ruhnke, R., Santee, M., Senten, C., Smale, D., Tétard, C., Urban, J., and Wood, S.: Validation of HNO3, ClONO2, and N2O5 from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), Atmos. Chem. Phys., 8, 3529–3562, https://doi.org/10.5194/acp-8-3529-2008, 2008. a
[6] Inness, A., Ades, M., Agustí-Panareda, A., Barré, J., Benedictow, A., Blechschmidt, A.-M., Dominguez, J. J., Engelen, R., Eskes, H., Flemming, J., Huijnen, V., Jones, L., Kipling, Z., Massart, S., Parrington, M., Peuch, V.-H., Razinger, M., Remy, S., Schulz, M., and Suttie, M.: The CAMS reanalysis of atmospheric composition, Atmos. Chem. Phys., 19, 3515–3556, https://doi.org/10.5194/acp-19-3515-2019, 2019. a
[7] Xiao, Y., Jacob, D. J., and Turquety, S.: Atmospheric acetylene and itsrelationship with CO as an indicator of air mass age, J. Geophys.Res.-Atmos., 112, D12305, https://doi.org/10.1029/2006JD008268,2007. a, b
[8] Wohltmann, I., Lehmann, R., Gottwald, G. A., Peters, K., Protat, A., Louf, V., Williams, C., Feng, W., and Rex, M.: A Lagrangian convective transport scheme including a simulation of the time air parcels spend in updrafts (LaConTra v1.0), Geosci. Model Dev., 12, 4387–4407, https://doi.org/10.5194/gmd-12-4387-2019, 2019. a
[9] James, R., Bonazzola, M., Legras, B., Surbled, K., and Fueglistaler, S.: Watervapor transport and dehydration above convective outflow during Asianmonsoon, Geophys. Res. Lett., 35, L20810, https://doi.org/10.1029/2008GL035441,2008. a
[10] Woiwode, W., Oelhaf, H., Gulde, T., Piesch, C., Maucher, G., Ebersoldt, A., Keim, C., Höpfner, M., Khaykin, S., Ravegnani, F., Ulanovsky, A. E., Volk, C. M., Hösen, E., Dörnbrack, A., Ungermann, J., Kalicinsky, C., and Orphal, J.: MIPAS-STR measurements in the Arctic UTLS in winter/spring 2010: instrument characterization, retrieval and validation, Atmos. Meas. Tech., 5, 1205–1228, https://doi.org/10.5194/amt-5-1205-2012, 2012. a
[11] Burkholder, J. B., Sander, S. P., Abbatt, J., Barker, J. R., Huie, R. E., Kolb,C. E., Kurylo, M. J., Orkin, V. L., Wilmouth, D. M., and Wine, P. H.:Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies,Evaluation No. 18, JPL Publication, 15-10, available at:http://jpldataeval.jpl.nasa.gov (last access: 30 November 2020), 2015. a
[12] Livesey, N. J., Filipiak, M. J., Froidevaux, L., Read, W. G., Lambert, A.,Santee, M. L., Jiang, J. H., Pumphrey, H. C., Waters, J. W., Cofield, R. E.,Cuddy, D. T., Daffer, W. H., Drouin, B. J., Fuller, R. A., Jarnot, R. F.,Jiang, Y. B., Knosp, B. W., Li, Q. B., Perun, V. S., Schwartz, M. J., Snyder,W. V., Stek, P. C., Thurstans, R. P., Wagner, P. A., Avery, M., Browell,E. V., Cammas, J., Christensen, L. E., Diskin, G. S., Gao, R., Jost, H.,Loewenstein, M., Lopez, J. D., Nedelec, P., Osterman, G. B., Sachse, G. W.,and Webster, C. R.: Validation of Aura Microwave Limb Sounder O3 and COobservations in the upper troposphere and lower stratosphere, J. Geophys. Res.-Atmos., 113, D15S02, https://doi.org/10.1029/2007JD008805,2008. a
[13] Li, D., Vogel, B., Müller, R., Bian, J., Günther, G., Li, Q., Zhang, J., Bai, Z., Vömel, H., and Riese, M.: High tropospheric ozone in Lhasa within the Asian summer monsoon anticyclone in 2013: influence of convective transport and stratospheric intrusions, Atmos. Chem. Phys., 18, 17979–17994, https://doi.org/10.5194/acp-18-17979-2018, 2018. a
[14] Bucci, S., Legras, B., Sellitto, P., D'Amato, F., Viciani, S., Montori, A., Chiarugi, A., Ravegnani, F., Ulanovsky, A., Cairo, F., and Stroh, F.: Deep-convective influence on the upper troposphere–lower stratosphere composition in the Asian monsoon anticyclone region: 2017 StratoClim campaign results, Atmos. Chem. Phys., 20, 12193–12210, https://doi.org/10.5194/acp-20-12193-2020, 2020. a, b, c, d
[15] WMO: Scientific Assessment of Ozone Depletion: 2018, Vol. 58 ofReport/World Meteorological Organization, Global Ozone Research andMonitoring Project, WMO, Geneva, Switzerland, available at:https://csl.noaa.gov/assessments/ozone/2018/ (last access: 30 November 2020),2019. a, b
[16] Guenther, A. B., Jiang, X., Heald, C. L., Sakulyanontvittaya, T., Duhl, T., Emmons, L. K., and Wang, X.: The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions, Geosci. Model Dev., 5, 1471–1492, https://doi.org/10.5194/gmd-5-1471-2012, 2012. a
[17] Wohltmann, I. and Rex, M.: The Lagrangian chemistry and transport model ATLAS: validation of advective transport and mixing, Geosci. Model Dev., 2, 153–173, https://doi.org/10.5194/gmd-2-153-2009, 2009. a, b
[18] Meinshausen, M., Smith, S. J., Calvin, K., Daniel, J. S., Kainuma, M. L. T.,Lamarque, J.-F., Matsumoto, K., Montzka, S. A., Raper, S. C. B., Riahi, K.,Thomson, A., Velders, G. J. M., and van Vuuren, D. P.: The RCP greenhousegas concentrations and their extensions from 1765 to 2300, Climatic Change,109, 213–241, https://doi.org/10.1007/s10584-011-0156-z, 2011. a
[19] Hoyle, C. R., Marécal, V., Russo, M. R., Allen, G., Arteta, J., Chemel, C., Chipperfield, M. P., D'Amato, F., Dessens, O., Feng, W., Hamilton, J. F., Harris, N. R. P., Hosking, J. S., Lewis, A. C., Morgenstern, O., Peter, T., Pyle, J. A., Reddmann, T., Richards, N. A. D., Telford, P. J., Tian, W., Viciani, S., Volz-Thomas, A., Wild, O., Yang, X., and Zeng, G.: Representation of tropical deep convection in atmospheric models – Part 2: Tracer transport, Atmos. Chem. Phys., 11, 8103–8131, https://doi.org/10.5194/acp-11-8103-2011, 2011. a
[20] Coheur, P.-F., Herbin, H., Clerbaux, C., Hurtmans, D., Wespes, C., Carleer, M., Turquety, S., Rinsland, C. P., Remedios, J., Hauglustaine, D., Boone, C. D., and Bernath, P. F.: ACE-FTS observation of a young biomass burning plume: first reported measurements of C2H4, C3H6O, H