Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 7 6 2007 10.5194/acpd-7-17893-2007 http://www.atmos-chem-phys-discuss.net/7/17893/2007/ http://www.atmos-chem-phys-discuss.net/7/17893/2007/acpd-7-17893-2007.html http://www.atmos-chem-phys-discuss.net/7/17893/2007/acpd-7-17893-2007.pdf 17893 17926 2007-12-13 Aerosol distribution over Europe: a model evaluation study with detailed aerosol microphysics B. Langmann baerbel.langmann@zmaw.de S. Varghese E. Marmer E. Vignati J. Wilson P. Stier C. O'Dowd School of Physics and Centre for Climate & Air Pollution Studies, Environmental Change Institute, National University of Ireland, Galway, Ireland Climate Change Unit, Joint Research Centre, Ispra, Italy Atmospheric, Oceanic and Planetary Physics, University of Oxford, Oxford, UK present affiliation: Institute of Geophysics, University Hamburg, Hamburg, Germany This paper summarizes an evaluation of model simulations with a regional scale atmospheric climate-chemistry/aerosol model called REMOTE, which has been extended by a microphysical aerosol module. Model results over Europe are presented and compared with available measurements in surface air focusing on the European distribution and variability of primary and secondary aerosols. Additionally, model results obtained with detailed aerosol microphysics are compared to those based on an aerosol bulk mass approach revealing the impact of dry deposition fluxes on atmospheric burden concentration. An improved determination of elevated ozone and sulfate concentrations could be achieved by considering a diurnal cycle in the anthropogenic emission fluxes. Deviation between modelled and measured organic carbon concentrations can be mainly explained by missing formation of secondary organic aerosols and deficiencies in emission data. Changing residential heating practices in Europe, where the use of wood is no longer restricted to rural areas, need to be considered in emission inventories as well as vegetation fire emissions which present a dominant source of organic carbon. Ackermann, I. J., Hass, H., Memmesheimer, M., Ebel, A., Binkowski, F. S., and Shankar, U.: Modal aerosol dynamics model for Europe: Development and first applications, Atmos. Environ., 32, 2981–2999, 1998. Andersson-Skold, Y. and Simpson, D.: Secondary organic aerosol formation in northern Europe: A model study, J. Geophys. Res., 106, 7357–7374, 2001. Dusek, U., Frank, G. P., Hildebrandt, L., Curtius, J., Schneider, J., Walter, S., Chand, D., Drewnick, F., Hings, S., Jung, D., Borrmann, S., and Andreae, M. O.: Size matters more than chemistry for the cloud-nucleating ability of aerosol particles, Science, 312, 1375–1378, 2006. Feichter, J., Kjellstroem, E., Rohde, H., Dentener, F., Lelieveld, J., and Roelofs, G.-J.: Simulation of the tropospheric sulfure cycle in a global climate model, Atmos. Environ., 30, 1693–1707, 1996. Ganzeveld L., Lelieveld, J., and Roelofs, G.-J.: Dry deposition parameterization of sulfur oxides in a chemistry and general circulation model, J. Geophys. Res., 103, 5679–5694, 1998. Geever, M., O'Dowd, C., van Ekeren, S., Flanagan, R., Nilsson, E. D., de Leeuw, G., and Rannik, Ü.: Sub-micron sea-spray fluxes, Geophys. Res. Lett., 32, doi: 10.1029/2005GL023081, 2005. Gelencser, A., May, B., Simpson, D., Sanchez-Ochoa, A., Kasper-Giebl, A., Puxbaum, H., Caseiro, A., Pio C., and Legrand, M.: Source apportionment of PM2.5 organic aerosol over Europe: primary/secondary, natural/anthropogenic, fossil/biogenic origin, J. Geophys. Res., 112, D23S04, doi:10.1029/2006JD008094, 2007. Gong, S. L., Barrie, L. A., Blanchet, J. P., von Salzen, K., Lohmann, U., Lesins, G., Spacek, L., Zhang, L. M., Girard, E., Lin, H., Leaitch, R., Leighton, H., Chylek, P., and Huang, P.: Canadian Aerosol Module: A size-segregated simulation of atmospheric aerosol processes for climate and air quality models: 1. Model development, J. Geophys. Res., 108, D4007, doi:10.1029/2001JD002002, 2003. Grell, G. A., Peckham, S. E., Schmitz, R., McKeen, S. A., Frost, G., Skamarock, W. C., and Eder, B.: Fully coupled "online chemistry" within the WRF model, Atmos. Environ., 39, 6957–6975, 2005. Haywood, J. and Boucher, O.: Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: A review, Rev. of Geoph., 38, 513–543, 2000. Heald, C. L., Jacob, D. J., Park, R. J., Russell, L. M., Hubert, B. J., Seinfeld, J. H., Liao, H., and Weber, R. J.: A large organic aerosol source in the free troposphere missing from current models, Geophys. Res. Lett., 32, L18809, doi:10.1029/2005GL023831, 2005. Hodzic, A., Madronich, S., Bohn, B., Massie, S., Menut, L., and Wiedinmeyer, C.: Wildfire particulate matter in Europe during summer 2003: meso-scale modeling of smoke emissions, transport and radiative effects, Atmos. Chem. Phys., 7, 4043–4064, 2007. Jacobson, M. Z.: Global direct radiative forcing due to multicomponent anthropogenic and natural aerosols, J. Geophys. Res., 106, 1551–1568, 2001. Kasper-Giebl, A., Koch, A., Hitzenberger, R., and Puxbaum, H.: Scavenging efficiency of aerosol carbon and sulfate in super-cooled clouds at Mt. Sonnblick (3106 m a.s.l, Austria), J. Atmos. Chem., 35, 33–46, 2000. Koch, D., Schmidt, G. A., and Field, C. V.: Sulfur, sea salt and radionuclide aerosols in GISS Model, J. Geophys. Res., 111, DO6206, doi:10.1029JD005550, 2006. Langmann, B.: Numerical modelling of regional scale transport and photochemistry directly together with meteorological processes, Atmos. Environ., 34, 3585–3598, 2000. Langmann, B.: A model study of the smoke-haze influence on clouds and warm precipitation formation in Indonesia 1997/1998, Atmos. Environ., 41, 6838–6852, doi:10.1016/j.atmosenv.2007.04.050, 2007. Lauer, A., Hendricks, J., Ackermann, I. J., Schell, B., Hass, H., and Metzger, S.: Simulating aerosol microphysics with the ECHAM/MADE GCM – Part I: Model description and comparison with observations, Atmos. Chem. Phys., 5, 3251–3276, 2005. Majewski, D.: The Europa Modell of the Deutscher Wetterdienst, Seminar Proceedings ECMWF, Vol. 2, 147–191, 1991. Marmer E. and Langmann, B.: Aerosol modelling over Europe Part I: Inter-annual variability of aerosol distribution, J. Geophys. Res., 112, D23S15, doi:10.1029/2006JD008113, 2007. Memmesheimer, M., Tippke, J., Ebel, A., Hass, H., Jacobs, H. J., and Laube, M.: On the use of EMEP emission inventories for European scale air pollution modelling with the EURAD model, EMEP Workshop on photooxidant modelling for long-range transport in relation to abatment strategies, Berlin, Germany, 16–19 April 1991, 307–324, 1991. Novakov, T., Cachier, H., Clark, J. S., Gaudichet, A., Macko, S., and Masclet, P.: Characterization of particulate products of biomass combustion, in Sediment Records of Biomass Burning and Global Change, edited by: Clak, J. S., Cachier, H., Goldammer, J. G., and Stocks, B., NATO ASI Series, Springer Verlag, Berlin, Germany, 1997. O'Dowd, C., Facchini, M. C., Cavalli, F., Ceburnis, D., Mircea, M., Decesari, S., Fuzzi, S., Yoon, Y. J., and Putaud, J. P.: Biogenically-driven organic contribution to marine aerosol, Nature, 432, 7009, doi:10.1038/nature02959, 2004. O'Dowd, C., Langmann, B., Varghese, S., Scannell, C., Ceburnis, D., and Facchini, M. C.: A combined organic-inorganic sea-spray source function, Geophys. Res. Lett., doi:10.1029/2007GL030331, in press, 2007. Roeckner, E., Arpe, K., Bengtsson, L., Christoph, M., Claussen, M., Dümenil, L., Esch, M., Giorgetta, M., Schlese, U., and Schulzweida, U.: The atmospheric general circulation model ECHAM-4: Model description and simulation of present-day climate, MPI-Report No. 218, Max Planck Institute for Meteorology, Hamburg, Germany, 1996. Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: from air pollution to climate change, Wiley-Interscience, 1998. Simpson, D., Winiwarter, W., Boerjesson, G., Cinderby, S., Ferreiro, A. Guenther, A., Hewitt, C. N., Janson, R., Khalil, M. A. K., Owen, S., Pierce, T. E., Puxbaum, H., Shearer, M., Skiba, U., Steinbrecher, R., Tarrason L., and Oequist, M. G.: Inventorying emissions from nature in Europe, J. Geophys. Res., 104, 8113–8152, 1999. Solmon, F., Giorgi F., and Liousse, C.: Aerosol modelling for regional climate studies: application to anthropogenic particles and evaluation over a European / African domain, Tellus, 58B, 51–72, 2006. Stier, P., Feichter, J., Kinne, S., Kloster, S., Vignati, E., Wilson, J., Ganzeveld, L., Tegen, I., Werner, M., Balkanski, Y., Schulz, M., Boucher, O., Minikin, A., and Petzold, A.: The aerosol-climate model ECHAM5-HAM, Atmos. Chem. Phys., 5, 1125–1156, 2005. Stoddart, J., Jeffries, D., Lkewolle, A., Clair, T., Dillon, P., Driscoll, C., Fortius, M., Johannsessen, M., Kahl, J., Kellogg, J., Kemp., A., Mannio, J., Montheith, D., Murdoch, P., Patrick, S., Rebsdorf, A., and Skjelkv, B.: Regional trends in aquatic recovery from acidification in North America and Europe, Nature, 401, 575–578, 1999. Szidat, S., Prevot, A. S. H., Sandradewi, J., Alfarra, M. R., Synal, H.-A., Wacker, L., and Baltenschlager, U.: Dominant impact of residential wood burning on particulate matter in Alpine valleys during winter, Geophys. Res. Lett., 34, L05820, doi:10.1029/2006GL028325, 2007. Tsyro, S., Simpson, D., Tarrason, L., Klimont, Z., Kupiainen, K., Pio C., and Yttri, K. E.: Modelling of elemental carbon over Europe, J. Geophys. Res., 112, D23S19, doi:10.1029/2006JD008164, 2007. Van der Werf, G. R., Randerson, J. T., Giglio, L., Collatz, G. J., Kasibhatla, P. S., and Arellano, A. F. Jr.: Interannual variability in global biomass burning emissions from 1997 to 2004, Atmos. Chem. Phys., 6, 3423–3441, 2006. Vignati, E., Wilson, J., and Stier, P.: M7: An efficient size-resolved aerosol microphysics module for large-scale aerosol transport models, J. Geophys. Res., 109, D22202, doi:10.1029/2003JD004485, 2004. WHO, World Health Report 2002, Tech. Rep., World Health Organisation, Genova 2002. Walcek, C. J. and Taylor, G. R.: A theoretical method for computing vertical distributions of acidity and sulfate production within cumulus clouds, J. Atmos. Sci., 43, 339–355, 1986. Walcek, C. J., Brost, R. A., Chang, J. S., and Wesley, M. L.: SO₂, Sulfate and HNO₃ deposition velocities computed using regional landuse and meteorological data, Atmos. Environ., 20, 946–964, 1986. Wesley, M. L.: Parameterization of surface resistances to gaseous dry deposition in regional-sclae numerical models, Atmos. Environ., 23, 1293–1304, 1989. Yoon, Y. J., Ceburnis, D., Cavalli, F., Jourdan, O., Putaud, J. P., Facchini, M. C., Decesari, S., Fuzzi, S., Jennings, S. G., and O'Dowd, C.: Seasonal characteristics of the physico-chemical properties of North Atlantc marine aerosols, J. Geophys. Res., 112, D04206, doi:10.1029/2005JD007044, 2007. Yttri, K. E., Aas, W., Bjerke, A., Ceburnis, D., Dye, C., Emblico, L., Facchini, M. C., Forster, C., Hanssen, J. E., Hannsson, H. C., Jennings, S. G., Maenhaut, W., Putaud, J. P., and Torseth, K.: Elemental and organic carbon in PM10: A one year measurement campaign within the European Monitoring and Evaluations Programme EMEP, Atmos. Chem. Phys., 7, 5711–5725, 2007. Zhang, Y., Seigneur, C., Seinfeld, J. H., Jacobson, M. Z., and Binkowsky, F. S.: Simulation of aerosol dynamics: A comparative review of algorithms used in air quality models, Aerosol Sci. Technol., 31, 487–514, 1999.