ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-10-2595-2010 Sources of uncertainties in modelling black carbon at the global scale Vignati E. 1 Karl M. 1 5 Krol M. 2 3 Wilson J. 1 Stier P. 4 Cavalli F. 1 European Commission, Joint Research Centre, Institute for Environment and Sustainability, Ispra, Italy Netherlands Institute for Space Research (SRON), Utrecht, The Netherlands Wageningen University and Research Centre, Wageningen, The Netherlands Atmospheric, Oceanic and Planetary Physics, Department of Physics, University of Oxford, Oxford, UK now at: Norwegian Institute for Air Research, Kjeller, Norway 16 03 2010 10 6 2595 2611 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys.net/10/2595/2010/acp-10-2595-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/10/2595/2010/acp-10-2595-2010.pdf

Our understanding of the global black carbon (BC) cycle is essentially qualitative due to uncertainties in our knowledge of its properties. This work investigates two source of uncertainties in modelling black carbon: those due to the use of different schemes for BC ageing and its removal rate in the global Transport-Chemistry model TM5 and those due to the uncertainties in the definition and quantification of the observations, which propagate through to both the emission inventories, and the measurements used for the model evaluation. <br><br> The schemes for the atmospheric processing of black carbon that have been tested with the model are (i) a simple approach considering BC as bulk aerosol and a simple treatment of the removal with fixed 70% of in-cloud black carbon concentrations scavenged by clouds and removed when rain is present and (ii) a more complete description of microphysical ageing within an aerosol dynamics model, where removal is coupled to the microphysical properties of the aerosol, which results in a global average of 40% in-cloud black carbon that is scavenged in clouds and subsequently removed by rain, thus resulting in a longer atmospheric lifetime. This difference is reflected in comparisons between both sets of modelled results and the measurements. Close to the sources, both anthropogenic and vegetation fire source regions, the model results do not differ significantly, indicating that the emissions are the prevailing mechanism determining the concentrations and the choice of the aerosol scheme does not influence the levels. In more remote areas such as oceanic and polar regions the differences can be orders of magnitude, due to the differences between the two schemes. The more complete description reproduces the seasonal trend of the black carbon observations in those areas, although not always the magnitude of the signal, while the more simplified approach underestimates black carbon concentrations by orders of magnitude. <br><br> The sensitivity to wet scavenging has been tested by varying in-cloud and below-cloud removal. BC lifetime increases by 10% when large scale and convective scale precipitation removal efficiency are reduced by 30%, while the variation is very small when below-cloud scavenging is zero. <br><br> Since the emission inventories are representative of elemental carbon-like substance, the model output should be compared to elemental carbon measurements and if known, the ratio of black carbon to elemental carbon mass should be taken into account when the model is compared with black carbon observations.

 References Alfaro, S. C., Gomes, L., Rajot, J. L., Lafon, S., Gaudichet, A., Chatenet, B., Maille, M., Cautenet, G., Lasserre, F., Cachier, H., and Zhang, X. Y.: Chemical and optical characterization of aerosols measured in spring 2002 at the ACE-Asia supersite, Zhenbeitai, China, J. Geophys. Res.-Atmos., 108(D23), 8641, doi:10.1029/2002JD003214, 2003a. Alfaro, S. C., Gaudichet, A., Rajot, J. L., Gomes, L., Maille, M., and Cachier, H.: Variability of aerosol size-resolved composition at an Indian coastal site during the Indian Ocean Experiment (INDOEX) intensive field phase, J. Geophys. Res.-Atmos., 108(D8), 4235, doi:10.1029/2002JD002645, 2003b. Andreae, M. O., Andreae, T. W., Ferek, R. J., and Raemdonck, H.: Long-range transport of soot carbon in the marine atmosphere, Sci. Total Environ., 36, 73–80, 1984. Andreae, M. O. and Merlet., P.: Emission of trace gases and aerosols from biomass burning, Global Biogeochem. Cy., 15, 955–966, 2001. Andreae, M. O. and Gelencsér, A.: Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols, Atmos. Chem. Phys., 6, 3131–3148, 2006. Bergamaschi, P., Meirink, J. F., Müller, J. F., Körner, S., Heimann, M., Bousquet, P., Dlugokencky, E. J., Kaminski, U., Vecchi, R., Marcazzan, G., Meinhardt, F., Ramonet, M., Sartorius, H., and Zahorowski, W.: Model Inter-comparison on Transport and Chemistry – report on model inter-comparison performed within European Commission FP5 project EVERGREEN Report EUR 22241 EN, 53~pp., 2006. Betts, A. K., Köhler, M., and Zhang, Y.: Comparison of river basin hydrometeorology in ERA-Interim and ERA-40 reanalyses with observations, J. Geophys. Res., 114, D02101, doi:10.1029/2008JD010761, 2009. Bodhaine, B. A.: Aerosol absorption measurements at Barrow, Mauna Loa and the south pole, J. Geophys. Res., 100, 8967-8975, 1995. Bond, T. C., Streets, D. G., Yarber, K. F., Nelson, S. M., Woo, J. H., and Klimont, Z.: A technology-based global inventory of black and organic carbon emissions from combustion, J. Geophys. Res.-Atmos., 109, D14203, doi:10.1029/2003JD003697, 2004. Bond, T. C. and Bergstrom, R. W.: Light absorption by carbonaceous particles: An investigative review, Aerosol Sci. Tech., 40, 1-41, 2006. Chow, J. C., Watson, J.G., Crow, D., Lowenthal, D.H., and Merrifield, T.: Comparison of IMPROVE and NIOSH carbon measurements, Aerosol Sci. Tech., 34, 23–34, 2001. Chung, S. H. and Seinfeld, J. H.: Global distribution and climate forcing of carbonaceous aerosols, J. Geophys. Res., 107(D19), 4407, doi:10.1029/2001JD001397, 2002. Clarke, A. D.: Aerosol light absorption by soot in remote environments, Aerosol Sci. Tech., 10, 161–171, 1989. Cofala, J., Amann, M., Klimont, Z., Kupiainen, K., and Höglund-Isaksson, L.: Scenarios of global anthropogenic emissions of air pollutants and methane until 2030, Atmos. Environ., 41, 8486–8499, 2007 Cooke, W. F. and Wilson, J. J. N.: A global black carbon aerosol model, J. Geophys. Res.-Atmos., 101, 19395–19409, 1996. Croft, B., Lohmann, U., and von Salzen, K.: Black carbon ageing in the Canadian Centre for Climate modelling and analysis atmospheric general circulation model, Atmos. Chem. Phys., 5, 1931–1949, 2005. Currie, L. A., Benner Jr., B. A., Kessler, J. D., Klinedinst, D. B., Klouda, G. A., Marolf, J. V., Slater, J. F., Wise, S. A., Cachier, H., Cary, R., Chow, J. C., Watson, J., Druffel, E. R. M., Masiello, C. A., Eglinton, T. I., Pearson, A., Reddy, C. M., Gustafsson, O., Quinn, J. G., Hartmann, P. C., Hedges, J. I., Prentice, K. M., Kirchstetter, T. W., Novakov, T., Puxbaum, H., and Schmid, H.: A critical evaluation of interlaboratory data on total, elemental, and isotopic carbon in the carbonaceous particle reference material, NIST SRM 1649a, J. Res. Natl. Inst. Stan., 107, 279–298, 2002. Dana, M. T. and Hales, J. M.: Statistical aspects of the washout of polydisperse aerosols, Atmos. Environ., 10, 45–50, 1976. de Meij, A., Krol, M., Dentener, F., Vignati, E., Cuvelier, C., and Thunis, P.: The sensitivity of aerosol in Europe to two different emission inventories and temporal distribution of emissions, Atmos. Chem. Phys., 6, 4287-4309, 2006. Decesari, S., Fuzzi, S., Facchini, M. C., Mircea, M., Emblico, L., Cavalli, F., Maenhaut, W., Chi, X., Schkolnik, G., Falkovich, A., Rudich, Y., Claeys, M., Pashynska, V., Vas, G., Kourtchev, I., Vermeylen, R., Hoffer, A., Andreae, M. O., Tagliavini, E., Moretti, F., and Artaxo, P.: Characterization of the organic composition of aerosols from Rondônia, Brazil, during the LBA-SMOCC 2002 experiment and its representation through model compounds, Atmos. Chem. Phys., 6, 375–402, 2006. Dentener, F., Stevenson, D., Cofala, J., Mechler, R., Amann, M., Bergamaschi, P., Raes, F., and Derwent, R.: The impact of air pollutant and methane emission controls on tropospheric ozone and radiative forcing: CTM calculations for the period 1990–2030, Atmos. Chem. Phys., 5, 1731–1755, 2005. Dentener, F., Kinne, S., Bond, T., Boucher, O., Cofala, J., Generoso, S., Ginoux, P., Gong, S., Hoelzemann, J. J., Ito, A., Marelli, L., Penner, J. E., Putaud, J.-P., Textor, C., Schulz, M., van der Werf, G. R., and Wilson, J.: Emissions of primary aerosol and precursor gases in the years 2000 and 1750 prescribed data-sets for AeroCom, Atmos. Chem. Phys., 6, 4321–4344, 2006. Dzubay, T. G., Stevens, R. K., and Haagenson, P. L.: Composition and origins of aerosol at a forested mountain in Soviet Georgia, Environ. Sci. Technol., 18, 873–883, 1984. Echalar, F., Artaxo, P., Martins, J. V., Yamasoe, M., Gerab, F., Maenhaut, W., and Holben, B.: Long-term monitoring of atmospheric aerosols in the amazon basin: Source identification and apportionment, J. Geophys. Res.-Atmos., 103, 31849–31864, 1998. Eleftheriadis, K., Vratolis, S., and Nyeki, S.: Aerosol black carbon in the European Arctic: Measurements at Zeppelin station, Ny-Ã…lesund, Svalbard from 1998–2007, Geophys. Res. Lett., 36, L02809, doi:10.1029/2008GL035741, 2009. Fassi-Fihri, A., Suhre, K., and Rosset, R.: Internal and external mixing in atmospheric aerosols by coagulation: Impact on the optical and hygroscopic properties of the sulphate-soot system, Atmos. Environ., 31, 1393–1402, 1997. Ganzeveld, L. and Lelieveld, J.: Dry deposition parameterization in a chemistry general circulation model and its influence on the distribution of reactive trace gases, J. Geophys. Res., 100, 20999–921012, 1995. Gery, M. W., Whitten, G. Z., and Killus, J. P: Development and testing of the CBM-IV for urban and regional modelling, US EPA, Research Triangle Park EPA-600/3-88-012, 1989a. Gery, M. W., Whitten, G. Z., Killus, J. P., and Dodge, M. C.: A photochemical kinetics mechanism for urban and regional scale computer modeling, J. Geophys. Res., 94, 12925–912956, 1989b. Gong, S. L.: A parameterization of sea-salt aerosol source function for sub- and super-micron particles, Global Biogeochem. Cy., 17(4), 1097, doi:10.1029/2003GB002079, 2003. 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. Module development, J. Geophys. Res.-Atmos., 108, 4007, doi:10.1029/2001JD002002, 2003. Guelle, W., Balkanski, Y. J., Schulz, M., Dulac, F., and Monfray, P.: Wet deposition in a global size-dependent aerosol transport model. 1. Comparison of a 1 year 210Pb simulation with ground measurements, J. Geophys. Res.-Atmos., 103, 11429-11445, 1998. Guillaume, B., Liousse, C., Rosset, R., Cachier, H., Van Velthoven, P., Bessagnet, B., and Poisson, N.: ORISAM-TM4: A new global sectional multi-component aerosol model including SOA formation - Focus on carbonaceous BC and OC aerosols, Tellus~B, 59, 283–302, 2007. Hagemann, S., Arpe, K., and Bengtsson, L.: Validation of the hydrological cycle of ERA-40, ERA-40 Project Report Series, ECMWF, Reading, England, 2005. Haywood, J. M. and Shine, K. P.: The effect of anthropogenic sulfate and soot aerosol on the clear sky planetary radiation budget, Geophys. Res. Lett., 22, 603–606, 1995. Heintzenberg, J. and Bigg, E. K.: Tropospheric transport of trace substances in the Southern Hemisphere, Tellus~B, 42, 355–363, 1990. Hertel, O., Berkowicz, R., Christensen, J., and Hov, O.: Test of two numerical schemes for use in atmospheric transport-chemistry models, Atmos. Environ. A-Gen, 27, 2591–2611, 1993. Hitzenberger, R., Berner, A., Giebl, H., Kromp, R., Larson, S. M., Rouc, A., Koch, A., Marischka, S., and Puxbaum, H.: Contribution of carbonaceous material to cloud condensation nuclei concentrations in European background (Mt Sonnblick) and urban (Vienna) aerosols, Atmos. Environ., 33, 2647–2659, 1999. Hitzenberger, R., Petzold, A., Bauer, H., Ctyroky, P., Pouresmaeil, P., Laskus, L., and Puxbaum, H.: Intercomparison of thermal and optical measurement methods for elemental carbon and black carbon at an urban location, Environ. Sci. Technol., 40, 6377–6383, 2006. Houweling, S., Dentener, F., and Lelieveld, J.: The impact of nonmethane hydrocarbon compounds on tropospheric photochemistry, J. Geophys. Res., 103, 10673–10696, 1998. IPCC: The Physical Science Basis, in: Contribution of Working Group I ot the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, ISBN~978~0521~88009-1 Hardback; 978~0521~70596-7 Paperback, 2007. Jacobson, M. Z.: Global direct radiative forcing due to multicomponent anthropogenic and natural aerosols, J. Geophys. Res.-Atmos., 106, 1551–1568, 2001. Jacobson, M. Z.: Control of fossil-fuel particulate black carbon and organic matter, possibly the most effective method of slowing global warming, J. Geophys. Res.-Atmos., 107(D19), 4410, doi:10.1029/2001JD001376, 2002. Jeong, C.-H., Hopke, P. K., Kim, E., and Lee, D.-W.: The comparison between thermal-optical transmittance elemental carbon and Aethalometer black carbon measured at multiple monitoring sites, Atmos. Environ., 38, 5193–5204, 2004. Jeuken, A., Veefkind, J. P., Dentener, F., Metzger, S., and Robles Gonzalez, C.: Simulation of the aerosol optical depth over Europe for August 1997 and a comparison with observations, J. Geophys. Res.-Atmos., 106, 28295–28311, 2001. Junker, C., Sheahan, J. N., Jennings, S. G., O'Brien, P., Hinds, B. D., Martinez-Twary, E., Hansen, A. D. A., White, C., Garvey, D. M., and Pinnick, R. G.: Measurement and analysis of aerosol and black carbon in the southwestern United States and Panama and their dependence on air mass origin, J. Geophys. Res.-Atmos., 109, D13201, doi:10.1029/2003JD004066, 2004. Junker, C. and Liousse, C.: A global emission inventory of carbonaceous aerosol from historic records of fossil fuel and biofuel consumption for the period 1860-1997, Atmos. Chem. Phys., 8, 1195–1207, 2008. Kasper-Giebl, A., Koch, A., Hitzenberger, R., and Puxbaum, H.: Scavenging efficiency of "Aerosol carbon" and sulfate in supercooled clouds at Mt Sonnblick (3106 m a.s.l., Austria), J. Atmos. Chem., 35, 33–46, 2000. Kettle, A. J., Andreae, M. O., Amouroux, D., Andreae, T. W., Bates, T. S., Berresheim, H., Bingemer, H., et al.: A global database of sea surface dimethylsulfide (DMS) measurements and a procedure to predict sea surface DMS as a function of latitude, longitude, and month, Global Biogeochem. Cy., 13(2), 399–444, 1999. Kleefeld, S., Hoffer, A., Krivácsy, Z., and Jennings, S. G.: Importance of organic and black carbon in atmospheric aerosols at Mace Head, on the West Coast of Ireland (53&deg;19&deg; N, 9&deg;54&deg; W), Atmos. Environ., 36, 4479–4490, 2002. Koch, D. and Hansen, J.: Distant origins of Arctic black carbon: A Goddard Institute for Space Studies ModelE experiment, J. Geophys. Res.-Atmos., 110, D04204, doi:10.1029/2004JD005296, 2005. Koch, D., Bond, T. C., Streets, D., Unger, N., and van der Werf, G. R.: Global impacts of aerosols from particular source regions and sectors, J. Geophys. Res.-Atmos., 112, D02205, doi:10.1029/2005JD007024, 2007. Koch, D., Schulz, M., Kinne, S., McNaughton, C., Spackman, J. R., Balkanski, Y., Bauer, S., Berntsen, T., Bond, T. C., Boucher, O., Chin, M., Clarke, A., De Luca, N., Dentener, F., Diehl, T., Dubovik, O., Easter, R., Fahey, D. W., Feichter, J., Fillmore, D., Freitag, S., Ghan, S., Ginoux, P., Gong, S., Horowitz, L., Iversen, T., Kirkev&aring;g, A., Klimont, Z., Kondo, Y., Krol, M., Liu, X., Miller, R., Montanaro, V., Moteki, N., Myhre, G., Penner, J. E., Perlwitz, J., Pitari, G., Reddy, S., Sahu, L., Sakamoto, H., Schuster, G., Schwarz, J. P., Seland, Ø., Stier, P., Takegawa, N., Takemura, T., Textor, C., van Aardenne, J. A., and Zhao, Y.: Evaluation of black carbon estimations in global aerosol models, Atmos. Chem. Phys., 9, 9001–9026, 2009. Kouvarakis, G., Doukelis, Y., Mihalopoulos, N., Rapsomanikis, S., Sciare, J., and Blumthaler, M.: Chemical, physical, and optical characterization of aerosols during PAUR II experiment, J. Geophys. Res.-Atmos., 107(D18), 8141, doi:10.1029/2000JD000291, 2002. Krol, M., Houweling, S., Bregman, B., van den Broek, M., Segers, A., van Velthoven, P., Peters, W., Dentener, F., and Bergamaschi, P.: The two-way nested global chemistry-transport zoom model TM5: algorithm and applications, Atmos. Chem. Phys., 5, 417–432, 2005. Lee, J. H., Kim, Y. P., Moon, K. C., Kim, H. K., and Lee, C. B.: Fine particle measurements at two background sites in Korea between 1996 and 1997, Atmos. Environ., 35, 635–643, 2001. Liousse, C., Penner, J. E., Chuang, C., Walton, J. J., Eddleman, H., and Cachier, H.: A global three-dimensional model study of carbonaceous aerosols, J. Geophys. Res.-Atmos., 101, 19411–19432, 1996. Liss, P. and Merlivat, L.: The role of sea-air exchange in geochemical cycling, edited by: Menard, P., Reidel, Dordrecht, 113-127, 1986. Ma, L., Zhang, T., Frauenfeld, O. W., Ye, B., Yang, D., and Qin, D.: Evaluation of precipitation from the ERA-40, NCEP-1, and NCEP-2 Reanalyses and CMAP-1, CMAP-2, and GPCP-2 with ground-based measurements in China, J. Geophys. Res., 114, D09105, doi:10.1029/2008JD011178, 2009. Maenhaut, W., Salma, I., Cafmeyer, J., Annegarn, H. J., and Andreae, M. O.: Regional atmospheric aerosol composition and sources in the eastern Transvaal, South Africa, and impact of biomass burning, J. Geophys. Res.-Atmos., 101, 23631–23650, 1996. Matsumoto, K., Uematsu, M., Hayano, T., Yoshioka, K., Tanimoto, H., and Iida, T.: Simultaneous measurements of particulate elemental carbon on the ground observation network over the western North Pacific during the ACE-Asia campaign, J. Geophys. Res.-Atmos., 108(D23), 8635, doi:10.1029/2002JD002744, 2003. Nyeki, S., Bauer, H., Puxbaum, H., Dye, C., Teinila, K., Hillamo, R., Ström, J., and Eleftheriadis, K.: Comparison of Black Carbon concentrations derived by filter-based light transmission and thermo-optical techniques for Arctic aerosol, in: Proceedings of the European Aerosol Conference, Ghent, Belgium, 28 August–2 September 2005, 122~pp., 2005. Penner, J. E., Eddleman, H., and Novakov, T.: Towards the development of a global inventory for black carbon emissions, Atmos. Environ. A-Gen, 27, 1277–1295, 1993. Pereira, E. B., Evangelista, H., Pereira, K. C. D., Cavalcanti, I. F. A., and Setzer, A. W.: Apportionment of black carbon in the South Shetland Islands, Antartic Peninsula, J. Geophys. Res.-Atmos., 111, D03303, doi:10.1029/2005JD006086, 2006. Peters, W., Krol, M. C., Dlugokencky, E. J., Dentener, F. J., Bergamaschi, P., Dutton, G., Velthoven, P. V., Miller, J. B., Bruhwiler, L., and Tans, P. P.: Toward regional-scale modeling using the two-way nested global model TM5: Characterization of transport using SF6, J. Geophys. Res.-Atmos., 109, D19314, doi:10.1029/2004JD005020, 2004. Petersen, A. C., Spee, E. J., Dop, H. V., and Hundsdorfer, W.: An evaluation and intercomparison of four new advection schemes for use in global chemistry models, J. Geophys. Res., 103, 19253–19269, 1998 Pöschl, U., Letzel, T., Schauer, C., and Niessner, R.: Interaction of ozone and water vapor with spark discharge soot aerosol particles coated with benzo[a]pyrene: O<sub>3</sub> and H<sub>2</sub>O adsorption, benzo[a]pyrene degradation, and atmospheric implications, J. Phys. Chem A, 105, 4029–4041, 2001. Reddy, M. S. and Boucher, O.: Climate impact of black carbon emitted from energy consumption in the world's regions, Geophys. Res. Lett., 34, L11802, doi:10.1029/2006GL028904, 2007. Reisinger, P., Wonaschütz, A., Hitzenberger, R., Petzold, A., Bauer, H., Jankowski, N., Puxbaum, H., Chi, X., and Maenhaut, W.: Intercomparison of measurement techniques for black or elemental carbon under urban background conditions in wintertime: Influence of biomass combustion, Environ. Sci. Technol., 42, 884–889, 2008. Russell, G. L. and Lerner, J. A.: A new finite-differencing scheme for the tracer transport equation. J. Appl. Meteorol., 20, 1483–1498, 1981. Schaap, M., Denier Van Der Gon, H. A. C., Dentener, F. J., Visschedijk, A. J. H., Van Loon, M., ten Brink, H. M., Putaud, J. P., Guillaume, B., Liousse, C., and Builtjes, P. J. H.: Anthropogenic black carbon and fine aerosol distribution over Europe, J. Geophys. Res.-Atmos., 109, D18207, doi:10.1029/2003JD004330, 2004. Schmid, H., Laskus, L., Jürgen Abraham, H., Baltensperger, U., Lavanchy, V., Bizjak, M., Burba, P., Cachier, H., Crow, D., Chow, J., Gnauk, T., Even, A., Ten Brink, H. M., Giesen, K. P., Hitzenberger, R., Hueglin, C., Maenhaut, W., Pio, C., Carvalho, A., Putaud, J. P., Toom-Sauntry, D., and Puxbaum, H.: Results of the "carbon conference" international aerosol carbon round robin test stage I, Atmos. Environ., 35, 2111–2121, 2001. Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: from air pollution to climate change, J Wiley, New York, Chichester, xxvii, 1326~pp., 1998. Sharma, S., Lavoue, D., Chachier, H., Barrie, L. A., and Gong, S. L.: Long-term trends of the black carbon concentrations in the Canadian Arctic, J. Geophys. Res.-Atmos., 109, D15203 15201–15210, 2004. Sharma, S., Andrews, E., Barrie, L. A., Ogren, J. A., and Lavoue, D.: Variations and sources of the equivalent black carbon in the high Arctic revealed by long-term observations at Alert and Barrow: 1989–2003, J. Geophys. Res.-Atmos., 111, D14208, doi:10.1029/2005JD006581, 2006. Schwarz, J. P., Gao, R. S., Fahey, D. W., et al.: Single-particle measurements of midlatitude black carbon and lightscattering aerosols from the boundary layer to the lower stratosphere, J. Geophys. Res., 111, D16207, doi:10.1029/2006JD007076, 2006. Slowik, J. G., Cross, E. S., Han, J.-H., et al.: An intercomparison of instruments measuring black carbon content of soot particles, Aerosol Sci. Tech., 41, p 295, 2007. Spracklen, D. V., Pringle, K. J., Carslaw, K. S., Mann, G. W., Manktelow, P., and Heintzenberg, J.: Evaluation of a global aerosol microphysics model against size-resolved particle statistics in the marine atmosphere, Atmos. Chem. Phys., 7, 2073–2090, 2007. 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. Stier, P., Feichter, J., Kloster, S., Vignati, E., and Wilson, J.: Emission-induced nonlinearities in the global aerosol system: Results from the ECHAM5-HAM aerosol-climate model, J. Climate, 19, 3845–3862, 2006. Stier, P., Seinfeld, J. H., Kinne, S., and Boucher, O.: Aerosol absorption and radiative forcing, Atmos. Chem. Phys., 7, 5237–5261, 2007. Ström, J., Okada, K., and Heintzenberg, J.: On the state of mixing of particles due to Brownian coagulation, J. Aerosol Sci., 23, 467–480, 1992. Tegen, I., Hollrig, P., Chin, M., Fung, I., Jacob, D., and Penner, J.: Contribution of different aerosol species to the global aerosol extinction optical thickness: Estimates from model results, J. Geophys. Res.-Atmos., 102, 23895–23915, 1997. ten Brink, H., Maenhaut, W., Hitzenberger, R., Gnauk, T., Spindler, G., Even, A., Chi, X., Bauer, H., Puxbaum, H., Putaud, J. P., Tursic, J., and Berner, A.: INTERCOMP2000: The comparability of methods in use in Europe for measuring the carbon content of aerosol, Atmos. Environ., 38, 6507–6519, 2004. Textor, C., Schulz, M., Guibert, S., Kinne, S., Balkanski, Y., Bauer, S., Berntsen, T., Berglen, T., Boucher, O., Chin, M., Dentener, F., Diehl, T., Easter, R., Feichter, H., Fillmore, D., Ghan, S., Ginoux, P., Gong, S., Grini, A., Hendricks, J., Horowitz, L., Huang, P., Isaksen, I., Iversen, I., Kloster, S., Koch, D., Kirkev&aring;g, A., Kristjansson, J. E., Krol, M., Lauer, A., Lamarque, J. F., Liu, X., Montanaro, V., Myhre, G., Penner, J., Pitari, G., Reddy, S., Seland, Ø., Stier, P., Takemura, T., and Tie, X.: Analysis and quantification of the diversities of aerosol life cycles within AeroCom, Atmos. Chem. Phys., 6, 1777–1813, 2006. Textor, C., Schulz, M., Guibert, S., Kinne, S., Balkanski, Y., Bauer, S., Berntsen, T., Berglen, T., Boucher, O., Chin, M., Dentener, F., Diehl, T., Feichter, J., Fillmore, D., Ginoux, P., Gong, S., Grini, A., Hendricks, J., Horowitz, L., Huang, P., Isaksen, I. S. A., Iversen, T., Kloster, S., Koch, D., Kirkev&aring;g, A., Kristjansson, J. E., Krol, M., Lauer, A., Lamarque, J. F., Liu, X., Montanaro, V., Myhre, G., Penner, J. E., Pitari, G., Reddy, M. S., Seland, Ø., Stier, P., Takemura, T., and Tie, X.: The effect of harmonized emissions on aerosol properties in global models - an AeroCom experiment, Atmos. Chem. Phys., 7, 4489–4501, 2007. Tsigaridis, K. and Kanakidou, M.: Global modelling of secondary organic aerosol in the troposphere: a sensitivity analysis, Atmos. Chem. Phys., 3, 1849–1869, 2003. Van Der Werf, G. R., Randerson, J. T., Collatz, G. J., Giglio, L., Kasibhatla, P. S., Arellano Jr., A. F., Olsen, S. C., and Kasischke, E. S.: Continental-Scale Partitioning of Fire Emissions during the 1997 to 2001 El Niño/La Niña Period, Science, 303, 73–76, 2004. Vignati, E., Wilson, J., and Stier, P.: M7: An efficient size-resolved aerosol microphysics module for large-scale aerosol transport models, J. Geophys. Res.-Atmos., 109, D22202, doi:10.1029/2003JD004485, 2004. Vignati, E., Facchini, M. C., Rinaldi, M., Scannell, C., Ceburnis, D., Sciare, J., Kanakidou, M., Myriokefalitakis, S., Dentener, F., and O'Dowd, C. D.: Global scale emission and distribution of sea spray aerosol: sea-salt and organic enrichment, Atmos. Environ., 44, 670–677, 2010 Watson, J. G., Chow, J.C., and Chen, L.-W. A.: Summary of organic and elemental carbon/black carbon analysis methods and intercomparisons, Aerosol Air Qual. Res., 5, 65–102, 2005. Weingartner, E., Burtscher, H., and Baltensperger, U.: Hygroscopic properties of carbon and diesel soot particles, Atmos. Environ., 31, 2311–2327, 1997. Wilson, J., Cuvelier, C., and Raes, F.: A modeling study of global mixed aerosol fields, J. Geophys. Res.-Atmos., 106, 34081–34108, 2001. Wolff, G. T., Ruthkosky, M. S., and Stroup, D. P.: Measurements of SO(x), NO(x) and aerosol species on Bermuda, Atmos. Environ. A-Gen, 20, 1229–1239, 1986. Wolff, E. W. and Cachier, H.: Concentrations and seasonal cycle of black carbon in aerosol at a coastal Antarctic station, J. Geophys. Res.-Atmos., 103, 11033–11041, 1998. Yttri, K. E., Aas, W., Bjerke, A., Cape, J. N., Cavalli, F., Ceburnis, D., Dye, C., Emblico, L., Facchini, M. C., Forster, C., Hanssen, J. E., Hansson, H. C., Jennings, S. G., Maenhaut, W., Putaud, J. P., and Tørseth, K.: Elemental and organic carbon in PM$_10$: a one year measurement campaign within the European Monitoring and Evaluation Programme EMEP, Atmos. Chem. Phys., 7, 5711–5725, 2007.