ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-12-4449-2012 Intercomparison of modal and sectional aerosol microphysics representations within the same 3-D global chemical transport model Mann G. W. 1 2 Carslaw K. S. 2 Ridley D. A. 3 Spracklen D. V. 2 Pringle K. J. 2 Merikanto J. 4 Korhonen H. 5 Schwarz J. P. 6 Lee L. A. 2 Manktelow P. T. 2 8 Woodhouse M. T. 2 Schmidt A. 2 Breider T. J. 7 Emmerson K. M. 2 9 Reddington C. L. 2 Chipperfield M. P. 2 Pickering S. J. 2 National Centre for Atmospheric Science, University of Leeds, Leeds, UK School of Earth and Environment, University of Leeds, Leeds, UK Dept of Atmospheric Science, Colorado State University, Fort Collins, Colorado, USA Department of Physics, University of Helsinki, Helsinki, Finland Finnish Meteorological Institute, Kuopio Unit, Kuopio, Finland Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado, USA School of Engineering and Applied Sciences, Harvard University, Cambridge, MA, USA now at: Halcrow Group Ltd, Headingley, Leeds, UK now at: CSIRO Marine and Atmospheric Research, Aspendale, VIC 3195, Australia 22 05 2012 12 10 4449 4476 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/12/4449/2012/acp-12-4449-2012.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/4449/2012/acp-12-4449-2012.pdf

In the most advanced aerosol-climate models it is common to represent the aerosol particle size distribution in terms of several log-normal modes. This approach, motivated by computational efficiency, makes assumptions about the shape of the particle distribution that may not always capture the properties of global aerosol. Here, a global modal aerosol microphysics module (GLOMAP-mode) is evaluated and improved by comparing against a sectional version (GLOMAP-bin) and observations in the same 3-D global offline chemistry transport model. With both schemes, the model captures the main features of the global particle size distribution, with sub-micron aerosol approximately unimodal in continental regions and bi-modal in marine regions. Initial bin-mode comparisons showed that the current values for two size distribution parameter settings in the modal scheme (mode widths and inter-modal separation sizes) resulted in clear biases compared to the sectional scheme. By adjusting these parameters in the modal scheme, much better agreement is achieved against the bin scheme and observations. Annual mean surface-level mass of sulphate, sea-salt, black carbon (BC) and organic carbon (OC) are within 25% in the two schemes in nearly all regions. Surface level concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), surface area density and condensation sink also compare within 25% in most regions. However, marine CCN concentrations between 30° N and 30° S are systematically 25–60% higher in the modal model, which we attribute to differences in size-resolved particle growth or cloud-processing. Larger differences also exist in regions or seasons dominated by biomass burning and in free-troposphere and high-latitude regions. Indeed, in the free-troposphere, GLOMAP-mode BC is a factor 2–4 higher than GLOMAP-bin, likely due to differences in size-resolved scavenging. Nevertheless, in most parts of the atmosphere, we conclude that bin-mode differences are much less than model-observation differences, although some processes are missing in these runs which may pose a bigger challenge to modal schemes (e.g., boundary layer nucleation and ultra-fine sea-spray). The findings here underline the need for a spectrum of complexity in global models, with size-resolved aerosol properties predicted by modal schemes needing to be continually benchmarked and improved against freely evolving sectional schemes and observations.

 References Adams,~P J. and Seinfeld,~J H.: Predicting global aerosol size distributions in general circulation models,~J. Geophys. Res., 107, 4370, http://dx.doi.org/10.1029/2001JD001010doi:10.1029/2001JD001010, 2002. Alexander,~B., Park,~R J., Jacob,~D J., and Gong~S.: Transition metal-catalyzed oxidation of atmospheric sulfur: Global implications for the sulfur budget,~J. Geophys. Res., 114, D02309, http://dx.doi.org/10.1029/2008JD010486doi:10.1029/2008JD010486, 2009. Arnold,~S., Chipperfield,~M., and Blitz,~M.: A three-dimensional model study of the effect of new temperature-dependent quantum yields for acetone photolysis,~J. Geophys. Res., 110, D22305, http://dx.doi.org/10.1029/2005JD005998doi:10.1029/2005JD005998, 2005. Asmi,~A., Wiedensohler,~A., Laj,~P., Fjaeraa,~A.-M., Sellegri,~K., Birmili,~W., Weingartner,~E., Baltensperger,~U., Zdimal,~V. Zikova,~N., Putaud,~J.-P., Marinoni,~A., Tunved,~P., Hansson,~H.-C., Fiebig,~M., Kivekas,~N., Lihavainen,~H., Asmi,~E., Ulevicius,~V., Aalto,~P P., Swietlicki,~E., Kristensson,~A., Mihalopoulos,~N. Kalivitis,~N., Kalapov,~I., Kiss,~G., de~Leeuw,~G., Henzing,~B., Harrison,~R M., Beddows,~D., Dowd,~C O. Jennings,~S G., Flentje,~H., Weinhold,~K., Meinhardt,~F., Ries,~L., and Kulmala,~M.: Number size distributions and seasonality of submicron particles in Europe 2008–2009, Atmos. Chem. Phys., 11, 5505–5538, http://dx.doi.org/10.5194/acp-11-5505-2011doi:10.5194/acp-11-5505-2011, 2011. Ayers,~G. and Gras,~J.: Seasonal relationship between cloud condensation nuclei and aerosol methanesulphonate in marine air, Nature, 353, 834–835, 1991. Ayers,~G., Ivey,~J., and Gillett,~R.: Coherence between seasonal cycles of dimethylsulfide, methanesulfonate, and sulfate in marine air, Nature, 349, 404–406, 1991. Bauer,~S E. and Koch,~D.: Impact of heterogeneous sulfate formation at mineral dust surfaces on aerosol loads and radiative forcing in the Goddard Institute for Space Studies general circulation model,~J. Geophys. Res., 110, D17202, http://dx.doi.org/10.1029/2005JD005870doi:10.1029/2005JD005870, 2005. Bauer,~S E., Wright,~D L., Koch,~D., Lewis,~E R., McGraw,~R., Chang,~L.-S., Schwartz,~S E., and Ruedy,~R.: MATRIX (Multiconfiguration Aerosol TRacker of mIXing state): an aerosol microphysical module for global atmospheric models, Atmos. Chem. Phys., 8, 6003–6035, http://dx.doi.org/10.5194/acp-8-6003-2008doi:10.5194/acp-8-6003-2008, 2008. Bergman, T., Kerminen, V.-M., Korhonen, H., Lehtinen, K. J., Makkonen, R., Arola, A., Mielonen, T., Romakkaniemi, S., Kulmala, M., and Kokkola, H.: Evaluation of the sectional aerosol microphysics module SALSA implementation in ECHAM5-HAM aerosol-climate model, Geosci. Model Dev. Discuss., 4, 3623–3690, http://dx.doi.org/10.5194/gmdd-4-3623-2011doi:10.5194/gmdd-4-3623-2011, 2011. Birmili,~W., Wiedensohler,~A., Heintzenberg,~J., and Lehmann,~K.: Atmospheric particle number size distirbution in Central Europe: Statistical relations to air masses and meterology,~J. Geophys. Res., 106, 32005–32018, 2001. Carver,~G D. and Stott,~P A.: IMPACT: an implicit time integration scheme for chemical species and families, Ann. Geophys., 18, 337–346, http://dx.doi.org/10.1007/s00585-000-0337-ydoi:10.1007/s00585-000-0337-y, 2000. Carver,~G D., Brown,~P D., and Wild,~O.: The ASAD atmospheric chemistry integration package and chemical reaction database, Comp. Phys. Comm., 105, 197–215, 1997. Chipperfield,~M P.: New version of the TOMCAT/SLIMCAT off-line chemistry transport model,~Q J. Roy. Meteor. Soc., 132, 1179–1203, 2006. Clarke,~A D.: Atmospheric nuclei in the Pacific Midtroposphere: their nature, concentration, and evolution, J. Geophys. Res., 98, 20633–20647, 1993. Clarke,~A D. and Kapustin,~V N.: A Pacific aerosol survey. Part 1: A decade of data on particle production, transport, evolution and mixing in the troposphere,~J. Atmos. Sci., 59, 363–382, 2002. 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, http://dx.doi.org/10.5194/acp-6-4287-2006doi:10.5194/acp-6-4287-2006, 2006. 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, http://dx.doi.org/10.5194/acp-6-4321-2006doi:10.5194/acp-6-4321-2006, 2006. Easter,~R C., Ghan,~S J., Zhang,~Y., Saylor,~R D., Chapman,~E G., Laulainen,~N S., Abdul-Razzak,~H., Leung,~R., Bian,~X. and Zaveri,~R A.: MIRAGE: Model description and evaluation of aerosols and trace gases,~J. Geophys. Res., 109, D20210, http://dx.doi.org/10.1029/2004JD004571doi:10.1029/2004JD004571, 2004. Forster,~P., Ramaswamy,~V., Artaxo,~P., Berntsen,~T., Betts,~R., Fahey,~D W., Haywood,~J., Lean,~J., Lowe,~D C., Myhre,~G., Nganga,~J., Prinn,~R., Raga,~G., Schulz,~M., and Van Dorland,~R.: Climate change 2007: the physical science basis, in: Changes in Atmospheric Constituents and in Radiative Forcing, Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, Cambridge University Press, Cambridge, New York, 129–234, 2007. Fuller,~E N., Schetller,~P D., and Giddings,~J C.: A new method for the prediction of binary gas phase diffusion coefficients, Ind. Eng. Chem., 58, 5, 18–27, 1966. Gelbard,~F., Tambour,~Y., and Seinfeld,~J H.: Sectional representations for simulating aerosol dynamics,~J. Coll. Int. Sci., 76, 363–382, 1980. Ghan,~S., Laulainen,~N., Easter,~R., Wagener,~R., Nemesure,~S., Chapman,~E., Zhang,~Y., and Leung,~R.: Evaluation of aerosol direct radiative forcing in MIRAGE,~J. Geophys. Res., 106, 5295–5316, 2001. Ghan,~S J. and Schwartz,~S E.: Aerosol properties and processes: a path from field and laboratory measurements to global climate models, B. Am. Meteorol. Soc., 1059–1083, http://dx.doi.org/10.1175/BAMS-88-7-1059doi:10.1175/BAMS-88-7-1059, 2007. Heintzenberg,~J., Covert,~D C., and Van Dingenen,~R.: Size distribution and chemical composition of marine aerosols: a compilation and review, Tellus B, 52, 1104–1122, 2000. Herzog,~M., Weisenstein,~D K., and Penner,~J E.: A dynamic aerosol module for global chemical transport models: Model description, J. Geophys. Res., 109, D18202, http://dx.doi.org/10.1029/2003JD004405doi:10.1029/2003JD004405, 2004. Hofmann,~D J.: Twenty years of balloon-borne tropospheric aerosol measurements at Laramie, Wyoming,~J. Geophys. Res., 98, 12753–12776, 1993. Holland,~D M., Principe P P., and Sickles II,~J E.: Trends in atmospheric sulfur and nitrogen species in the Eastern United States for 1989 to 1995, Atmos. Environ., 33, 37–49, 1999. Hoppel,~W A., Frick,~G M., Fitzgerald,~J W., and Larson,~R E.: Marine boundary-layer measurements of new particle formation and the effects nonprecipitating clouds have on aerosol size distribution,~J. Geophys. Res., 99, 14443–14459, 1994. Holtslag,~A. and Boville,~B.: Local versus nonlocal boundary layer diffusion in a global climate model,~J. Climate, 6, 1825–1842, 1993. Johnson,~C E., Mann,~G W., Bellouin,~N. O'Connor,~F M. and Dalvi,~M.: Comparison between UKCA-MODE and CLASSIC aerosol schemes in HadGEM3, Integrated Climate Programme Deliverable M3.2, Report CR-ICP-2007–2012 to DECC, Defra & MoD, available online at: http://www.ukca.ac.uk/wiki/images/f/f8/ICP.pdf (last access: 18 February 2011) 2010. Jones,~A., Roberts,~D L., Woodage,~M J., and Johnson,~C E.: Indirect sulfate aerosol forcing in a climate model with an interactive sulfur cycle,~J. Geophys. Res., 106, 20293–20310, 2001. Jourdain,~B. and Legrand,~M.: Seasonal variations of atmospheric dimethylsulfide, dimethylsulfoxide, sulfur dioxide, methanesulfonate, and non-sea-salt sulfate aerosols at Dumont d'Urville (coastal Antartctica) (December 1998 to July 1999),~J. Geophys. Res., 106, 14391–14408, 2001. Kokkola,~H., Korhonen,~H., Lehtinen,~K E J., Makkonen,~R., Asmi,~A., Järvenoja,~S., Anttila,~T., Partanen,~A.-I., Kulmala,~M., Järvinen,~H., Laaksonen,~A., and Kerminen,~V.-M.: SALSA – a Sectional Aerosol module for Large Scale Applications, Atmos. Chem. Phys., 8, 2469–2483, http://dx.doi.org/10.5194/acp-8-2469-2008doi:10.5194/acp-8-2469-2008, 2008. Kokkola,~H., Hommel,~R., Kazil,~J., Niemeier,~U., Partanen,~A.-I., Feichter,~J., and Timmreck,~C.: Aerosol microphysics modules in the framework of the ECHAM5 climate model – intercomparison under stratospheric conditions, Geosci. Model Dev., 2, 97–112, http://dx.doi.org/10.5194/gmd-2-97-2009doi:10.5194/gmd-2-97-2009, 2009. Korhonen,~H., Carslaw,~K S., Spracklen,~D V., Ridley,~D A., and Ström,~J. : A global model study of processes controlling aerosol size distributions in the Arctic spring and summer,~J. Geophys. Res., 113, D08211, http://dx.doi.org/10.1029/2007JD009114doi:10.1029/2007JD009114, 2008. Kulmala, M., Laaksonen, A., and Pirjola, L.: Parameterizations for sulfuric acid/water nucleation rates, J. Geophys. Res., 103, 8301–8307, 1998. Kulmala,~M., Vehkamäkki,~H., Petäjä,~T., Dal Maso,~M., Lauri,~A., Kerminen,~V.-M., Birmili,~W., and McMurry,~P H.: Formation and growth rates of ultrafine atmospheric particles: a review of observations,~J. Aerosol Sci., 35, 143–176, 2004. Kulmala, M., Asmi, A., Lappalainen, H. K., Baltensperger, U., Brenguier, J.-L., Facchini, M. C., Hansson, H.-C., Hov, Ø., O'Dowd, C. D., Pöschl, U., Wiedensohler, A., Boers, R., Boucher, O., de Leeuw, G., Denier van der Gon, H. A. C., Feichter, J., Krejci, R., Laj, P., Lihavainen, H., Lohmann, U., McFiggans, G., Mentel, T., Pilinis, C., Riipinen, I., Schulz, M., Stohl, A., Swietlicki, E., Vignati, E., Alves, C., Amann, M., Ammann, M., Arabas, S., Artaxo, P., Baars, H., Beddows, D. C. S., Bergström, R., Beukes, J. P., Bilde, M., Burkhart, J. F., Canonaco, F., Clegg, S. L., Coe, H., Crumeyrolle, S., D'Anna, B., Decesari, S., Gilardoni, S., Fischer, M., Fjaeraa, A. M., Fountoukis, C., George, C., Gomes, L., Halloran, P., Hamburger, T., Harrison, R. M., Herrmann, H., Hoffmann, T., Hoose, C., Hu, M., Hyvärinen, A., Hõrrak, U., Iinuma, Y., Iversen, T., Josipovic, M., Kanakidou, M., Kiendler-Scharr, A., Kirkevåg, A., Kiss, G., Klimont, Z., Kolmonen, P., Komppula, M., Kristjánsson, J.-E., Laakso, L., Laaksonen, A., Labonnote, L., Lanz, V. A., Lehtinen, K. E. J., Rizzo, L. V., Makkonen, R., Manninen, H. E., McMeeking, G., Merikanto, J., Minikin, A., Mirme, S., Morgan, W. T., Nemitz, E., O'Donnell, D., Panwar, T. S., Pawlowska, H., Petzold, A., Pienaar, J. J., Pio, C., Plass-Duelmer, C., Prévôt, A. S. H., Pryor, S., Reddington, C. L., Roberts, G., Rosenfeld, D., Schwarz, J., Seland, Ø., Sellegri, K., Shen, X. J., Shiraiwa, M., Siebert, H., Sierau, B., Simpson, D., Sun, J. Y., Topping, D., Tunved, P., Vaattovaara, P., Vakkari, V., Veefkind, J. P., Visschedijk, A., Vuollekoski, H., Vuolo, R., Wehner, B., Wildt, J., Woodward, S., Worsnop, D. R., van Zadelhoff, G.-J., Zardini, A. A., Zhang, K., van Zyl, P. G., Kerminen, V.-M., S Carslaw, K., and Pandis, S. N.: General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) – integrating aerosol research from nano to global scales, Atmos. Chem. Phys., 11, 13061–13143, http://dx.doi.org/10.5194/acp-11-13061-2011doi:10.5194/acp-11-13061-2011, 2011. Lauer,~A., Hendricks,~J., Ackermann,~I., 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, http://dx.doi.org/10.5194/acp-5-3251-2005doi:10.5194/acp-5-3251-2005, 2005. Lehtinen,~K E J., Korhonen,~H., Dal Maso,~M., and Kulmala,~M.: On the concept of condensation sink diameter, Boreal Environ. Res., 8, 405–411, 2003. Liu,~X., Penner,~J E., and Herzog,~M.: Global modeling of aerosol dynamics: Model description, evaluation, and interactions between sulfate and nonsulfate aerosols,~J. Geophys. Res., 110, D18206, http://dx.doi.org/10.1029/2004JD005674doi:10.1029/2004JD005674, 2005. Loevblad,~G., Tarrason,~L., and Torseth,~K.: Sulphur, in: EMEP Assessment, Part 1: European Perspective, edited by: Loevblad,~G., Tarrason,~L., Torseth,~K., and Dutchak,~S., Norwegian Meteorol. Inst., Oslo, 15–46, 2004. Luo,~G. and Yu,~F.: Sensitivity of global cloud condensation nuclei concentrations to primary sulfate emission parameterizations, Atmos. Chem. Phys., 11, 1949–1959, http://dx.doi.org/10.5194/acp-11-1949-2011doi:10.5194/acp-11-1949-2011, 2011. Makela,~J M., Aalto,~P., Jokinen,~V., Pohja,~T., Nissinen,~A., Palmroth,~S., Markkanen,~T., Seitsonen,~K., Lihavainen,~H., and Kulmala,~M.: Observations of ultrafine aerosol particle formation and growth in boreal forest, Geophys. Res. Lett., 24, 1219–1222, 1997. Malm,~W C., Schichtel,~B A., Ames,~R B., and Gebhart,~K A.: A 10-year spatial and temporal trend of sulfate across the United States,~J. Geophys. Res., 107, 4627, http://dx.doi.org/10.1029/2002JD002107doi:10.1029/2002JD002107, 2002. Mann,~G W., Carslaw,~K S., Spracklen,~D V., Ridley,~D A., Manktelow,~P T., Chipperfield,~M P., Pickering,~S J., and Johnson,~C E.: Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model, Geosci. Model Dev., 3, 519–551, http://dx.doi.org/10.5194/gmd-3-519-2010doi:10.5194/gmd-3-519-2010, 2010. McGraw,~R.: Description of Aerosol Dynamics by the Quadrature Method of Moments, Aerosol Sci. Technol., 27, 255–265, 1997. Merikanto,~J., Spracklen,~D V., Mann,~G W., Pickering,~S J., and Carslaw,~K S.: Impact of nucleation on global CCN, Atmos. Chem. Phys., 9, 8601–8616, http://dx.doi.org/10.5194/acp-9-8601-2009doi:10.5194/acp-9-8601-2009, 2009. Morgenstern,~O., Braesicke,~P., O'Connor,~F M., Bushell,~A C., Johnson,~C E., Osprey,~S M., and Pyle,~J A.: Evaluation of the new UKCA climate-composition model – Part 1: The stratosphere, Geosci. Model Dev., 2, 43–57, http://dx.doi.org/10.5194/gmd-2-43-2009doi:10.5194/gmd-2-43-2009, 2009. Nguyen,~B., Mihalopoulos,~N., Putaud,~J., Gaudry,~A. and Gallet,~L.: Covariations in oceanic dimethyl sulfide, its oxidation products and rain acidity at Amsterdam Island in the Southern Indian Ocean,~J. Atmos. Chem., 15, 39–53, 1992. Penner,~J E., Andreae,~M., Annegarn,~H., Barrie,~L., Feichter,~J., Hegg,~D., Jayaraman,~A., Leaitch,~R., Murphy,~D., Nganga,~J., and Pitari, G.: Aerosols, their direct and indirect effects, in: Climate Change 2001: The Scientific Basis. Contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Houghton,~J T., Ding,~Y., Griggs,~D J., Noguer,~M., van der Linden,~P J., Dai,~X., Maskell,~K., and Johnson,~C A., Cambridge University Press, Cambridge, New York, 289–348, 2001. Petters,~M D. and Kreidenweis,~S M.: A single parameter representation of hygroscopic growth and cloud condensation nucleus activity, Atmos. Chem. Phys., 7, 1961–1971, http://dx.doi.org/10.5194/acp-7-1961-2007doi:10.5194/acp-7-1961-2007, 2007. Petzold,~A., Fiebig,~M., Flentje,~H., Keil,~A., Leiterer,~U., Schroeder,~F., Stifter~A., Wendisch,~M., and Wendling~P.: Vertical variability of aerosol properties observed at a continental site during the Lindenberg Aerosol Characterization Experiment (LACE98),~J. Geophys. Res., 107, 8128, http://dx.doi.org/10.1029/2001JD001043doi:10.1029/2001JD001043, 2002. Pirjola,~L., Kulmala,~M., Wilck,~M., Bischoff,~A., Stratmann,~F., and Otto,~E.: Formation of sulphuric acid aerosols and cloud \mboxcondensation nuclei: An expression for significant nucleation and model comparison, J. Aerosol Sci., 30, 1079–1094, 1999. Poling,~B E., Prausnitz,~J M., and O'Connell,~J P.: The properties of gases and liquids, McGraw-Hill, 768~pp., 2001. Pringle,~K J., Tost,~H., Metzger,~S. Steil,~B., Giannadaki,~D., Nenes,~A., Fontoukis,~C., Stier,~P., Vignati,~E., and Lelieveld,~J.: Description and evaluation of GMXe: a new aerosol submodel for global simulations (v1), Geosci. Model Dev., 3, 391–412, http://dx.doi.org/10.5194/gmd-3-391-2010doi:10.5194/gmd-3-391-2010, 2010. Raes,~F.: Entrainment of free tropospheric aerosol as a regulating mechanism for cloud condensation nuclei in the remote marine boundary layer,~J. Geophys. Res., 100, 2893–2903, 1995. Raes,~F., Van Dingenen,~R., Vignati,~E., Wilson,~J., Putaud,~J.-P., Seinfeld,~J H., and Adams,~P.: Formation and cycling of aerosols in the global troposphere, Atmos. Environ., 34, 4215–4240, 2000. Rasch,~P J., Feichter,~J., Law,~K., Mahowald,~N., Penner,~J., Benkowitz,~C., Genthon,~C., Giannakopoulos,~C., Kasibhatla,~P., Koch,~D., Levy,~H., Maki,~T., Prather,~M., Roberts,~D L., Roelofs,~G.-J., Stevenson,~D., Stockwell,~Z., Taguchi,~S., Kritz,~M., Chipperfield,~M., Baldocchi,~D., McMurry,~P., Barrie,~L., Balkanski,~Y., Chatfield,~R., Kjellstrom,~E., Lawrence,~M., Lee,~H N., Lelieveld,~J., Noone,~K J., Seinfeld,~J., Stenchikov,~G., Schwartz,~S., Walcek,~C., and Williamson,~D.: A comparison of scavenging and deposition processes in global models: results from the WCRP Cambridge Workshop of 1995, Tellus B, 52, 1025–1056, 2000. Reade,~L., Jennings,~S G., and McSweeney,~G.: Cloud condensation nuclei measurements at Mace Head, Ireland, over the period 1994–2002, Atmos. Res., 82, 610–621, 2006. Reddington,~C L., Carslaw,~K S., Spracklen,~D V., Frontoso,~M G., Collins,~L., Merikanto,~J., Minikin,~A., Hamburger,~T., Coe,~H., Kulmala,~M., Aalto,~P., Flentje,~H., Plass-Dülmer,~C., Birmili,~W., Wiedensohler,~A., Wehner,~B., Tuch,~T., Sonntag,~A., O'Dowd,~C D., Jennings,~S G., Dupuy,~R., Baltensperger,~U., Weingartner,~E., Hansson,~H.-C., Tunved,~P., Laj,~P., Sellegri,~K., Boulon,~J., Putaud,~J.-P., Gruening,~C., Swietlicki,~E., Roldin,~P., Henzing,~J S., Moerman,~M., Mihalopoulos,~N., Kouvarakis,~G., Ždímal,~V., Zíková,~N., Marinoni,~A., Bonasoni,~P., and Duchi,~R.: Primary versus secondary contributions to particle number concentrations in the European boundary layer, Atmos. Chem. Phys., 11, 12007–12036, http://dx.doi.org/10.5194/acp-11-12007-2011doi:10.5194/acp-11-12007-2011, 2011. Reddy,~M S., Boucher,~O., Bellouin,~N., Schulz,~M., Balkanski,~Y., Dufresne,~J L., and Pham, M.: Estimates of global multicomponent aerosol optical depth and direct radiative perturbation in the Laboratoire de Meteorologie Dynamique general circulation model,~J. Geophys. Res., 110, D10S16, http://dx.doi.org/10.1029/2004JD004757doi:10.1029/2004JD004757, 2005. Rossow,~W. and Schiffer,~R.: Advances in understanding clouds from ISCCP, B. Am. Meteorol. Soc., 80, 2261–2287, 1999. Schimel,~D., Alves,~D., Enting,~I., Heimann,~M., Joos,~R., Raynaud,~D., Wigley,~T., Prather,~M., Derwent,~R., Ehhalt,~D., Eraser,~R., Sanhueza,~E., Zhou,~X., Jonas,~R., Charlson,~R., Rodhe,~H., Sadasivan,~S., Shine,~K R., Fouquart,~Y., Ramaswamy,~V., Solomon,~S., Srinivasan,~J., Albritton,~D., Derwent,~R., Isaksen,~L., Lal,~M., and Wuebbles,~D.: Radiative forcing of climate change, in: Climate Change 1996, Contribution of Working Group I to the 2nd Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Houghton,~J T., Meira Filho,~L G., Callander,~B A., Harris,~N., Kattenberg,~A., and Maskell,~K., Cambridge University Press, Cambridge, New York, 1996. Schwarz,~J P., Gao,~R S., Spackman,~J R., Watts,~L A., Thomson,~D S., Fahey,~D W., Ryerson,~T B., Peischl,~J., Holloway,~J S., Trainer,~M., Frost,~G J., Baynard,~T., Lack,~D A., de Gouw,~J A., Warneke,~C., and Del Negro,~L A.: Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions, Geophys. Res. Lett., 35, L13810, http://dx.doi.org/10.1029/2008GL033968doi:10.1029/2008GL033968, 2008. Schwarz,~J P., Spackman,~J R., Gao,~R S., Watts,~L A., Stier,~P., Schulz,~M., Davis,~S M., Wofsy,~S C., and Fahey,~D W.: Global-scale black carbon profiles observed in the remote atmosphere and compared to models, Geophys. Res. Lett., 37, L18812, http://dx.doi.org/10.1029/2010GL044372doi:10.1029/2010GL044372, 2010. Seigneur,~C., Hudischewskyj,~A B., Seinfeld,~J H., Whitby,~K T., Whitby,~E R., Brock,~J R., and Barnes,~H M.: Simulation of aerosol dynamics: a comparative review of mathematical models, Aerosol Sci. Technol., 5, 205–222, 1986. Seinfeld,~J H. and Pandis,~S N.: Atmospheric Chemistry and Physics: From Air Pollution to Climate Change, Wiley-Interscience, 1326~pp., 1998. Spracklen,~D V., Pringle,~K J., Carslaw,~K S., Chipperfield,~M P., and Mann,~G W.: A global off-line model of size-resolved aerosol microphysics: I. Model development and prediction of aerosol properties, Atmos. Chem. Phys., 5, 2227–2252, http://dx.doi.org/10.5194/acp-5-2227-2005doi:10.5194/acp-5-2227-2005, 2005. Spracklen,~D V., Carslaw,~K S., Kulmala,~M., Kerminen,~V.-M., Mann,~G W., and Sihto,~S.-L.: The contribution of boundary layer nucleation events to total particle concentrations on regional and global scales, Atmos. Chem. Phys., 6, 5631–5648, http://dx.doi.org/10.5194/acp-6-5631-2006doi:10.5194/acp-6-5631-2006, 2006. Spracklen,~D V., Carslaw,~K S., Kulmala,~M., Kerminen,~V.-M., Sihto,~S.-L., Riipinen,~I., Merikanto,~J., Mann,~G W., Chipperfield,~M P., Wiedensohler,~A., Birmili,~W., and Lihavainen,~H.: Contribution of particle formation to global cloud condensation nuclei concentrations, Geophys. Res. Lett., 35, L06808, http://dx.doi.org/10.1029/2007GL033038doi:10.1029/2007GL033038, 2008 Spracklen,~D V., Carslaw,~K S., Merikanto,~J., Mann,~G W., Reddington,~C L., Pickering,~S., Ogren,~J A., Andrews,~E., Baltensperger,~U., Weingartner,~E., Boy,~M., Kulmala,~M., Laakso,~L., Lihavainen,~H., Kivekäs,~N., Komppula,~M., Mihalopoulos,~N., Kouvarakis,~G., Jennings,~S G., O'Dowd,~C., Birmili,~W., Wiedensohler,~A., Weller,~R., Gras,~J., Laj,~P., Sellegri,~K., Bonn,~B., Krejci,~R., Laaksonen,~A., Hamed,~A., Minikin,~A., Harrison,~R M., Talbot,~R., and Sun,~J.: Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation, Atmos. Chem. Phys., 10, 4775–4793, http://dx.doi.org/10.5194/acp-10-4775-2010doi:10.5194/acp-10-4775-2010, 2010. Spracklen,~D V., Carslaw,~K S., Pöschl,~U., Rap,~A., and Forster,~P M.: Global cloud condensation nuclei influenced by carbonaceous combustion aerosol, Atmos. Chem. Phys., 11, 9067–9087, http://dx.doi.org/10.5194/acp-11-9067-2011doi:10.5194/acp-11-9067-2011, 2011. 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, http://dx.doi.org/10.5194/acp-5-1125-2005doi:10.5194/acp-5-1125-2005, 2005. Taylor,~K E.: Summarizing multiple aspects of model performance in a single diagram,~J. Geophys. Res., 106, 7183–7192, 2001. Telford,~P., Braesicke,~P., Morgenstern,~O., and Pyle,~J.: Reassessment of causes of ozone column variability following the eruption of Mount Pinatubo using a nudged CCM, Atmos. Chem. Phys., 9, 4251–4260, http://dx.doi.org/10.5194/acp-9-4251-2009doi:10.5194/acp-9-4251-2009, 2009. 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., Kirkevåg,~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, http://dx.doi.org/10.5194/acp-6-1777-2006doi:10.5194/acp-6-1777-2006, 2006. Tiedtke,~M.: A comprehensive mass flux scheme for cumulus parameterization in large-scale models, Mon. Weather Rev., 117, 1779–1800, 1989. Trivitayanurak,~W., Adams,~P J., Spracklen,~D V., and Carslaw,~K S.: Tropospheric aerosol microphysics simulation with assimilated meteorology: model description and intermodel comparison, Atmos. Chem. Phys., 8, 3149–3168, http://dx.doi.org/10.5194/acp-8-3149-2008doi:10.5194/acp-8-3149-2008, 2008. 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, http://dx.doi.org/10.1029/2003JD004485doi:10.1029/2003JD004485, 2004. \hack Vignati,~E., Karl,~M., Krol,~M., Wilson,~J., Stier,~P., and Cavalli,~F.: Sources of uncertainties in modelling black carbon at the global scale, Atmos. Chem. Phys., 10, 2595–2611, http://dx.doi.org/10.5194/acp-10-2595-2010doi:10.5194/acp-10-2595-2010, 2010. Weisenstein, D. K., Penner, J. E., Herzog, M., and Liu, X.: Global 2-D intercomparison of sectional and modal aerosol modules, Atmos. Chem. Phys., 7, 2339–2355, http://dx.doi.org/10.5194/acp-7-2339-2007doi:10.5194/acp-7-2339-2007, 2007. Whitby,~K T.: The physical characteristics of sulfur aerosols, Atmos. Environ., 12, 135–159, 1978. Whitby,~K T.: Determination of aerosol growth rates in the atmosphere using lumped mode aerosol dynamics,~J. Aerosol Sci., 12, 173–178, 1981. Wilson,~J., Cuvelier,~C., and Raes,~F.: A modeling study of global mixed aerosol fields,~J. Geophys. Res., 106, 34081–34108, 2001. Zhang,~Y., Seigneur,~C., Seinfeld,~J H., and Jacobson,~M Z.: Simulation of aerosol dynamics: a comparative review of algorithms used in air quality models, Aerosol Sci. Technol., 31, 487–514, 1999. Zhang, K., Wan, H., Wang, B., Zhang, M., Feichter, J., and Liu, X.: Tropospheric aerosol size distributions simulated by three online global aerosol models using the M7 microphysics module, Atmos. Chem. Phys., 10, 6409–6434, http://dx.doi.org/10.5194/acp-10-6409-2010doi:10.5194/acp-10-6409-2010, 2010.