ACP Atmospheric Chemistry and Physics ACP Atmos. Chem. Phys. 1680-7324 Copernicus Publications Göttingen, Germany 10.5194/acp-14-13661-2014 The contribution of plume-scale nucleation to global and regional aerosol and CCN concentrations: evaluation and sensitivity to emissions changes Stevens R. G. https://orcid.org/0000-0002-8737-6988 1 2 Pierce J. R. https://orcid.org/0000-0002-4241-838X 1 2 Department of Physics and Atmospheric Science, Dalhousie University, Halifax, NS, Canada Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA 20 12 2014 14 24 13661 13679 Copyright: © 2014 R. G. Stevens 2014 This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/ This article is available from https://acp.copernicus.org/articles/14/13661/2014/acp-14-13661-2014.html The full text article is available as a PDF file from https://acp.copernicus.org/articles/14/13661/2014/acp-14-13661-2014.pdf

We implement the Predicting Particles Produced in Power-Plant Plumes (P6) sub-grid sulphate parameterization for the first time into a global chemical-transport model with online aerosol microphysics, the GEOS-Chem-TOMAS model. Compared to simulations using two other previous treatments of sub-grid sulphate, simulations using P6 sub-grid sulphate predicted similar or smaller increases (depending on other model assumptions) in globally, annually averaged concentrations of particles larger than 80 nm (N80). We test in simulations using P6 sub-grid sulphate the sensitivity of particle number concentrations to changes in SO<sub>2</sub> or NO<sub>x</sub> emissions to represent recent emissions control changes. For global increases of 50% in emissions of either SO<sub>2</sub> or NO<sub>x</sub>, or both SO<sub>2</sub> and NO<sub>x</sub>, we find that globally, annually averaged N80 increase by 9.00, 1.47, or 10.24% respectively. However, both sub-grid and grid-resolved processes contribute to these changes. Finally, we compare the model results against observations of particle number concentrations. Compared with previous treatments of sub-grid sulphate, use of the P6 parameterization generally improves correlation with observed particle number concentrations. The P6 parameterization is able to resolve spatial heterogeneity in new-particle formation and growth that cannot be resolved by any constant assumptions about sub-grid sulphate. However, the differences in annually averaged aerosol size distributions due to the treatment of sub-grid sulphate at the measurement sites examined here are too small to unambiguously establish P6 as providing better agreement with observations.

 References Aalto, P., Hämeri, K., Becker, E., Weber, R., Salm, J., Mäkelä, J. M., Hoell, C., O'Dowd, C. D., Karlsson, H., Hansson, H.-C., Väkevä, M., Koponen, I. K., Buzorius, G., and Kulmala, M.: Physical characterization of aerosol particles during nucleation events, Tellus B, 53, 344–358, 2001. Adams, P. J. and Seinfeld, J. H.: Predicting global aerosol size distributions in general circulation models, J. Geophys. Res., 107, 1–23, 2002. Adams, P. J. and Seinfeld, J. H.: Disproportionate impact of particulate emissions on global cloud condensation nuclei concentrations, Geophys. Res. Lett., 30, 1239, 2003. Albrecht, B.: Aerosols, cloud microphysics, and fractional cloudiness., Science, 245, 1227–1230, 1989. Arya, S. P.: Air Pollution Meteorology and Dispersion, Oxford University Press, Inc., New York, USA, 1999. 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., Kivekäs, 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., O'Dowd, C., 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, <a href="http://dx.doi.org/10.5194/acp-11-5505-2011">https://doi.org/10.5194/acp-11-5505-2011</a>, 2011. Auvray, M. and Bey, I.: Long-range transport to Europe: Seasonal variations and implications for the European ozone budget, J. Geophys. Res., 110, D11303, 2005. Bey, I., Jacob, D. J., Yantosca, R. M., Logan, J. a., Field, B. D., Fiore, A. M., Li, Q., Liu, H. Y., Mickley, L. J., and Schultz, M. G.: Global modeling of tropospheric chemistry with assimilated meteorology: Model description and evaluation, J. Geophys. Res., 106, 23073, 2001. Boucher, O., Randall, D., Artaxo, P., Bretherton, C., Feingold, G., Forster, P., Kerminen, V.-M., Kondo, Y., Liao, H., Lohmann, U., Rasch, P., Satheesh, S., Sherwood, S., Stevens, B., and Zhang, X.: Clouds and Aerosols, in: Climate Change 2013: The Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, edited by Stocker, T., Qin, D., Plattner, G.-K., Tignor, M., Allen, S., Boschung, J., Nauels, A., Xia, Y., Bex, V., and Midgley, P., chap. 7, pp. 571–657, Cambridge University Press, Cambridge, UK and New York, NY, USA, 2013. Carlton, A. G., Wiedinmyer, C., and Kroll, J. H.: A review of Secondary Organic Aerosol (SOA) formation from isoprene, Atmos. Chem. Phys., 9, 4987–5005, <a href="http://dx.doi.org/10.5194/acp-9-4987-2009">https://doi.org/10.5194/acp-9-4987-2009</a>, 2009. Carlton, A. G., Pinder, R. W., Bhave, P. V., and Pouliot, G. A.: To what extent can biogenic SOA be controlled?, Environ. Sci. Technol., 44, 3376–80, 2010. Charlson, R. J., Schwartz, S. E., Hales, J. M., Cess, R. D., Coakley, J. a., Hansen, J. E., and Hofmann, D. J.: Climate forcing by anthropogenic aerosols., Science, 255, 423–430, 1992. D'Andrea, S. D., Häkkinen, S. A. K., Westervelt, D. M., Kuang, C., Levin, E. J. T., Kanawade, V. P., Leaitch, W. R., Spracklen, D. V., Riipinen, I., and Pierce, J. R.: Understanding global secondary organic aerosol amount and size-resolved condensational behavior, Atmos. Chem. Phys., 13, 11519–11534, <a href="http://dx.doi.org/10.5194/acp-13-11519-2013">https://doi.org/10.5194/acp-13-11519-2013</a>, 2013. 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, <a href="http://dx.doi.org/10.5194/acp-6-4321-2006">https://doi.org/10.5194/acp-6-4321-2006</a>, 2006. Dockery, D., Pope, C., Xu, X., Spengler, J. D., Ware, J. H., Fay, M. E., Ferris, B. G., and Speizer, F. E.: An association between air pollution and mortality in six US cities, New Engl. J. Med., 329, 1753–1759, 1993. 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 cloud-nucleating ability of aerosol particles., Science, 312, 1375–8, 2006. Eisele, F. and Tanner, D.: Measurement of the gas phase concentration of H2SO4 and methane sulfonic acid and estimates of H2SO4 production and loss in the atmosphere, J. Geophys. Res., 98, 9001–9010, 1993. Erupe, M. E., Benson, D. R., Li, J., Young, L.-H., Verheggen, B., Al-Refai, M., Tahboub, O., Cunningham, V., Frimpong, F., Viggiano, A. a., and Lee, S.-H.: Correlation of aerosol nucleation rate with sulfuric acid and ammonia in Kent, Ohio: An atmospheric observation, J. Geophys. Res., 115, D23216, 2010. Guenther, A., Karl, T., Harley, P., Wiedinmyer, C., Palmer, P. I., and Geron, C.: Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature), Atmos. Chem. Phys., 6, 3181–3210, <a href="http://dx.doi.org/10.5194/acp-6-3181-2006">https://doi.org/10.5194/acp-6-3181-2006</a>, 2006. Heald, C. L., Coe, H., Jimenez, J. L., Weber, R. J., Bahreini, R., Middlebrook, A. M., Russell, L. M., Jolleys, M., Fu, T.-M., Allan, J. D., Bower, K. N., Capes, G., Crosier, J., Morgan, W. T., Robinson, N. H., Williams, P. I., Cubison, M. J., DeCarlo, P. F., and Dunlea, E. J.: Exploring the vertical profile of atmospheric organic aerosol: comparing 17 aircraft field campaigns with a global model, Atmos. Chem. Phys., 11, 12673–12696, <a href="http://dx.doi.org/10.5194/acp-11-12673-2011">https://doi.org/10.5194/acp-11-12673-2011</a>, 2011. Heald, C. L., Collett Jr., J. L., Lee, T., Benedict, K. B., Schwandner, F. M., Li, Y., Clarisse, L., Hurtmans, D. R., Van Damme, M., Clerbaux, C., Coheur, P.-F., Philip, S., Martin, R. V., and Pye, H. O. T.: Atmospheric ammonia and particulate inorganic nitrogen over the United States, Atmos. Chem. Phys., 12, 10295–10312, <a href="http://dx.doi.org/10.5194/acp-12-10295-2012">https://doi.org/10.5194/acp-12-10295-2012</a>, 2012. Jung, J., Fountoukis, C., Adams, P. J., and Pandis, S. N.: Simulation of in situ ultrafine particle formation in the eastern United States using PMCAMx-UF, J. Geophys. Res. Atmos., 115, <a href="http://dx.doi.org/10.1029/2009JD012313">https://doi.org/10.1029/2009JD012313</a>, 2010. Junkermann, W., Vogel, B., and Sutton, M. A.: The climate penalty for clean fossil fuel combustion, Atmos. Chem. Phys., 11, 12917–12924, <a href="http://dx.doi.org/10.5194/acp-11-12917-2011">https://doi.org/10.5194/acp-11-12917-2011</a>, 2011. Kanawade, V. P., Benson, D. R., and Lee, S.-H.: Statistical analysis of 4-year observations of aerosol sizes in a semi-rural continental environment, Atmos. Environ., 59, 30–38, 2012. Kerminen, V.-M., and Kulmala, M.: Analytical formulae connecting the "real" and the "apparent" nucleation rate and the nuclei number concentration for atmospheric nucleation events, J. Aerosol Sci., 33, 609–622, <a href="http://dx.doi.org/10.1016/S0021-8502(01)00194-X">https://doi.org/10.1016/S0021-8502(01)00194-X</a>, 2002. Khairoutdinov, M. and Randall, D.: Cloud resolving modeling of the ARM summer 1997 IOP: Model formulation, results, uncertainties, and sensitivities, J. Atmos. Sci., 60, 607–626, 2003. Kuhns, H., Green, M., and Etyemezian, V.: Big Bend Regional Aerosol and Visibility Observational (BRAVO) Study Emissions Inventory, technical report prepared for the BRAVO Steering Committee, Tech. Rep. 702, 2001. Kulmala, M. and Kerminen, V.-M.: On the formation and growth of atmospheric nanoparticles, Atmos. Res., 90, 132–150, 2008. Kulmala, M., Lehtinen, K. E. J., and Laaksonen, A.: Cluster activation theory as an explanation of the linear dependence between formation rate of 3nm particles and sulphuric acid concentration, Atmos. Chem. Phys., 6, 787–793, <a href="http://dx.doi.org/10.5194/acp-6-787-2006">https://doi.org/10.5194/acp-6-787-2006</a>, 2006. Leaitch, W. R., Sharma, S., Huang, L., Toom-Sauntry, D., Chivulescu, A., Macdonald, A. M., von Salzen, K., Pierce, J. R., Bertram, A. K., Schroder, J. C., Shantz, N. C., Chang, R. Y.-W., and Norman, A.-L.: Dimethyl sulfide control of the clean summertime Arctic aerosol and cloud, Elementa: Science of the Anthropocene, 1, 000017, 2013. Lee, L. A., Pringle, K. J., Reddington, C. L., Mann, G. W., Stier, P., Spracklen, D. V., Pierce, J. R., and Carslaw, K. S.: The magnitude and causes of uncertainty in global model simulations of cloud condensation nuclei, Atmos. Chem. Phys., 13, 8879–8914, <a href="http://dx.doi.org/10.5194/acp-13-8879-2013">https://doi.org/10.5194/acp-13-8879-2013</a>, 2013. Lee, Y. H. and Adams, P. J.: A Fast and Efficient Version of the TwO-Moment Aerosol Sectional (TOMAS) Global Aerosol Microphysics Model, Aerosol Sci. Tech., 46, 678–689, 2012. Levin, E., Kreidenweis, S., McMeeking, G., Carrico, C., Collett Jr., J., and Malm, W.: Aerosol physical, chemical and optical properties during the Rocky Mountain Airborne Nitrogen and Sulfur study, Atmos. Environ., 43, 1932–1939, 2009. Levin, E. J. T., Prenni, a. J., Petters, M. D., Kreidenweis, S. M., Sullivan, R. C., Atwood, S. a., Ortega, J., DeMott, P. J., and Smith, J. N.: An annual cycle of size-resolved aerosol hygroscopicity at a forested site in Colorado, J. Geophys. Res., 117, D06201, 2012. Lonsdale, C. R., Stevens, R. G., Brock, C. A., Makar, P. A., Knipping, E. M., and Pierce, J. R.: The effect of coal-fired power-plant SO<sub>2</sub> and NO<sub>x</sub> control technologies on aerosol nucleation in the source plumes, Atmos. Chem. Phys., 12, 11519–11531, <a href="http://dx.doi.org/10.5194/acp-12-11519-2012">https://doi.org/10.5194/acp-12-11519-2012</a>, 2012. Luo, G. and Yu, F.: Sensitivity of global cloud condensation nuclei concentrations to primary sulfate emission parameterizations, Atmos. Chem. Phys., 11, 1949–1959, <a href="http://dx.doi.org/10.5194/acp-11-1949-2011">https://doi.org/10.5194/acp-11-1949-2011</a>, 2011. Makkonen, R., Asmi, A., Korhonen, H., Kokkola, H., Järvenoja, S., Räisänen, P., Lehtinen, K. E. J., Laaksonen, A., Kerminen, V.-M., Järvinen, H., Lohmann, U., Bennartz, R., Feichter, J., and Kulmala, M.: Sensitivity of aerosol concentrations and cloud properties to nucleation and secondary organic distribution in ECHAM5-HAM global circulation model, Atmos. Chem. Phys., 9, 1747–1766, <a href="http://dx.doi.org/10.5194/acp-9-1747-2009">https://doi.org/10.5194/acp-9-1747-2009</a>, 2009. Mesinger, F., DiMego, G., Kalnay, E., Mitchell, K., Shafran, P. C., Ebisuzaki, W., Jović, D., Woollen, J., Rogers, E., Berbery, E. H., Ek, M. B., Fan, Y., Grumbine, R., Higgins, W., Li, H., Lin, Y., Manikin, G., Parrish, D., and Shi, W.: North American Regional Reanalysis, B. Am. Meteorol. Soc., 87, 343–360, 2006. Napari, I., Noppel, M., Vehkamäki, H., and Kulmala, M.: Parametrization of ternary nucleation rates for H<sub>2</sub>SO<sub>4</sub>-NH<sub>3</sub>-H<sub>2</sub>O vapors, J. Geophys. Res., 107, 4381, 2002. Offenberg, J. H., Lewandowski, M., Edney, E. O., Kleindienst, T. E., and Jaoui, M.: Influence of aerosol acidity on the formation of secondary organic aerosol from biogenic precursor hydrocarbons., Environ. Sci. Technol., 43, 7742–7, 2009. Olivier, J. G. J., Bouwman, A. F., Van der Maas, C. W. M., Berdowski, J. J. M., Veldt, C., Bloos, J. P. J., Visschedijk, A. J. H., Zandveld, P. Y. J., and Haverlag, J. L.: RIVM report nr. 771060002 / TNO-MEP report nr. R96/119: Description of EDGAR Version 2.0: A set of global emission inventories of greenhouse gases and ozone-depleting substances for all anthropogenic and most natural sources on a per country basis and on $1° \times 1°$ grid., Tech. rep., Netherlands Organization for Applied Scientific Research (TNO), 1996. Olson, J. R., Crawford, J. H., Chen, G., Brune, W. H., Faloona, I. C., Tan, D., Harder, H., and Martinez, M.: A reevaluation of airborne HO<sub>x</sub> observations from NASA field campaigns, J. Geophys. Res., 111, D10301, 2006. Peng, R. D., Dominici, F., Pastor-Barriuso, R., Zeger, S. L., and Samet, J. M.: Seasonal analyses of air pollution and mortality in 100 US cities., Am. J. Epidemiol., 161, 585–94, 2005. Peters, A., Wichmann, H. E., Tuch, T., Heinrich, J., and Heyder, J.: Respiratory effects are associated with the number of ultrafine particles., Am. J. Resp. Crit. Care, 155, 1376–1383, 1997. Pierce, J. R. and Adams, P. J.: Global evaluation of CCN formation by direct emission of sea salt and growth of ultrafine sea salt, J. Geophys. Res., 111, D06203, 2006. Pierce, J. R. and Adams, P. J.: Uncertainty in global CCN concentrations from uncertain aerosol nucleation and primary emission rates, Atmos. Chem. Phys., 9, 1339–1356, <a href="http://dx.doi.org/10.5194/acp-9-1339-2009">https://doi.org/10.5194/acp-9-1339-2009</a>, 2009. Pierce, J. R., Chen, K., and Adams, P. J.: Contribution of primary carbonaceous aerosol to cloud condensation nuclei: processes and uncertainties evaluated with a global aerosol microphysics model, Atmos. Chem. Phys., 7, 5447–5466, <a href="http://dx.doi.org/10.5194/acp-7-5447-2007">https://doi.org/10.5194/acp-7-5447-2007</a>, 2007. Pierce, J. R., Leaitch, W. R., Liggio, J., Westervelt, D. M., Wainwright, C. D., Abbatt, J. P. D., Ahlm, L., Al-Basheer, W., Cziczo, D. J., Hayden, K. L., Lee, A. K. Y., Li, S.-M., Russell, L. M., Sjostedt, S. J., Strawbridge, K. B., Travis, M., Vlasenko, A., Wentzell, J. J. B., Wiebe, H. A., Wong, J. P. S., and Macdonald, A. M.: Nucleation and condensational growth to CCN sizes during a sustained pristine biogenic SOA event in a forested mountain valley, Atmos. Chem. Phys., 12, 3147–3163, <a href="http://dx.doi.org/10.5194/acp-12-3147-2012">https://doi.org/10.5194/acp-12-3147-2012</a>, 2012. Pierce, J. R., Evans, M. J., Scott, C. E., D'Andrea, S. D., Farmer, D. K., Swietlicki, E., and Spracklen, D. V.: Weak global sensitivity of cloud condensation nuclei and the aerosol indirect effect to Criegee + SO<sub>2</sub> chemistry, Atmos. Chem. Phys., 13, 3163–3176, <a href="http://dx.doi.org/10.5194/acp-13-3163-2013">https://doi.org/10.5194/acp-13-3163-2013</a>, 2013. 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, <a href="http://dx.doi.org/10.5194/acp-11-12007-2011">https://doi.org/10.5194/acp-11-12007-2011</a>, 2011. Rienecker, M.: File Specification for GEOS-5 DAS Gridded Output, Tech. rep., Global Modeling and Assimilation Office, Goddard Space Flight Center, Greenbelt, Maryland, 2006. Riipinen, I., Pierce, J. R., Yli-Juuti, T., Nieminen, T., Häkkinen, S., Ehn, M., Junninen, H., Lehtipalo, K., Petäjä, T., Slowik, J., Chang, R., Shantz, N. C., Abbatt, J., Leaitch, W. R., Kerminen, V.-M., Worsnop, D. R., Pandis, S. N., Donahue, N. M., and Kulmala, M.: Organic condensation: a vital link connecting aerosol formation to cloud condensation nuclei (CCN) concentrations, Atmos. Chem. Phys., 11, 3865–3878, <a href="http://dx.doi.org/10.5194/acp-11-3865-2011">https://doi.org/10.5194/acp-11-3865-2011</a>, 2011. Sihto, S.-L., Kulmala, M., Kerminen, V.-M., Dal Maso, M., Petäjä, T., Riipinen, I., Korhonen, H., Arnold, F., Janson, R., Boy, M., Laaksonen, A., and Lehtinen, K. E. J.: Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms, Atmos. Chem. Phys., 6, 4079–4091, <a href="http://dx.doi.org/10.5194/acp-6-4079-2006">https://doi.org/10.5194/acp-6-4079-2006</a>, 2006. Snow-Kropla, E. J., Pierce, J. R., Westervelt, D. M., and Trivitayanurak, W.: Cosmic rays, aerosol formation and cloud-condensation nuclei: sensitivities to model uncertainties, Atmos. Chem. Phys., 11, 4001–4013, <a href="http://dx.doi.org/10.5194/acp-11-4001-2011">https://doi.org/10.5194/acp-11-4001-2011</a>, 2011. 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: II. Identification of key uncertainties, Atmos. Chem. Phys., 5, 3233–3250, <a href="http://dx.doi.org/10.5194/acp-5-3233-2005">https://doi.org/10.5194/acp-5-3233-2005</a>, 2005. Spracklen, D. V., Jimenez, J. L., Carslaw, K. S., Worsnop, D. R., Evans, M. J., Mann, G. W., Zhang, Q., Canagaratna, M. R., Allan, J., Coe, H., McFiggans, G., Rap, A., and Forster, P.: Aerosol mass spectrometer constraint on the global secondary organic aerosol budget, Atmos. Chem. Phys., 11, 12109–12136, <a href="http://dx.doi.org/10.5194/acp-11-12109-2011">https://doi.org/10.5194/acp-11-12109-2011</a>, 2011. Srivastava, R. K., Miller, C. a., Erickson, C., and Jambhekar, R.: Emissions of sulfur trioxide from coal-fired power plants., J. Air Waste Manage., 54, 750–62, 2004. Stevens, R. G. and Pierce, J. R.: A parameterization of sub-grid particle formation in sulfur-rich plumes for global- and regional-scale models, Atmos. Chem. Phys., 13, 12117–12133, <a href="http://dx.doi.org/10.5194/acp-13-12117-2013">https://doi.org/10.5194/acp-13-12117-2013</a>, 2013. Stevens, R. G., Pierce, J. R., Brock, C. A., Reed, M. K., Crawford, J. H., Holloway, J. S., Ryerson, T. B., Huey, L. G., and Nowak, J. B.: Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology, Atmos. Chem. Phys., 12, 189–206, <a href="http://dx.doi.org/10.5194/acp-12-189-2012">https://doi.org/10.5194/acp-12-189-2012</a>, 2012. Stieb, D. M., Judek, S., and Burnett, R. T.: Meta-analysis of time-series studies of air pollution and mortality: effects of gases and particles and the influence of cause of death, age, and season., J. Air Waste Manage., 52, 470–484, 2002. Streets, D. G., Bond, T. C., Carmichael, G. R., Fernandes, S. D., Fu, Q., He, D., Klimont, Z., Nelson, S. M., Tsai, N. Y., Wang, M. Q., Woo, J.-H., and Yarber, K. F.: An inventory of gaseous and primary aerosol emissions in Asia in the year 2000, J. Geophys. Res., 108, 8809, 2003. Surratt, J. D., Lewandowski, M., Offenberg, J. H., Jaoui, M., Kleindienst, T. E., Edney, E. O., and Seinfeld, J. H.: Effect of acidity on secondary organic aerosol formation from isoprene., Environ. Sci. Technol., 41, 5363–9, 2007. 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, <a href="http://dx.doi.org/10.5194/acp-8-3149-2008">https://doi.org/10.5194/acp-8-3149-2008</a>, 2008. Twomey, S.: Pollution and planetary albedo, Atmos. Environ., 8, 1251–1256, 1974. United States Environmental Protection Agency: Clean Air Markets: Data and Maps, <a href="http://ampd.epa.gov/ampd/">http://ampd.epa.gov/ampd/</a> (last access: March 2013), 2012. van der Werf, G. R., Randerson, J. T., Giglio, L., Collatz, G. J., Mu, M., Kasibhatla, P. S., Morton, D. C., DeFries, R. S., Jin, Y., and van Leeuwen, T. T.: Global fire emissions and the contribution of deforestation, savanna, forest, agricultural, and peat fires (1997–2009), Atmos. Chem. Phys., 10, 11707–11735, <a href="http://dx.doi.org/10.5194/acp-10-11707-2010">https://doi.org/10.5194/acp-10-11707-2010</a>, 2010. Vehkamäki, H., Kulmala, M., Napari, I., Lehtinen, K. E. J., Timmreck, C., Noppel, M., and Laaksonen, A.: An improved parameterization for sulfuric acid–water nucleation rates for tropospheric and stratospheric conditions, J. Geophys. Res., 107, 4622, 2002. Walker, J. M., Philip, S., Martin, R. V., and Seinfeld, J. H.: Simulation of nitrate, sulfate, and ammonium aerosols over the United States, Atmos. Chem. Phys., 12, 11213–11227, <a href="http://dx.doi.org/10.5194/acp-12-11213-2012">https://doi.org/10.5194/acp-12-11213-2012</a>, 2012. Wang, M. and Penner, J. E.: Aerosol indirect forcing in a global model with particle nucleation, Atmos. Chem. Phys., 9, 239–260, <a href="http://dx.doi.org/10.5194/acp-9-239-2009">https://doi.org/10.5194/acp-9-239-2009</a>, 2009. Wang, S. C. and Flagan, R. C.: Scanning Electrical Mobility Spectrometer, Aerosol Sci. Tech., 13, 230–240, 1990. Westervelt, D. M., Pierce, J. R., Riipinen, I., Trivitayanurak, W., Hamed, A., Kulmala, M., Laaksonen, A., Decesari, S., and Adams, P. J.: Formation and growth of nucleated particles into cloud condensation nuclei: model–measurement comparison, Atmos. Chem. Phys., 13, 7645–7663, <a href="http://dx.doi.org/10.5194/acp-13-7645-2013">https://doi.org/10.5194/acp-13-7645-2013</a>, 2013. Westervelt, D. M., Pierce, J. R., and Adams, P. J.: Analysis of feedbacks between nucleation rate, survival probability and cloud condensation nuclei formation, Atmos. Chem. Phys., 14, 5577–5597, <a href="http://dx.doi.org/10.5194/acp-14-5577-2014">https://doi.org/10.5194/acp-14-5577-2014</a>, 2014. Yu, F. and Luo, G.: Simulation of particle size distribution with a global aerosol model: contribution of nucleation to aerosol and CCN number concentrations, Atmos. Chem. Phys., 9, 7691–7710, <a href="http://dx.doi.org/10.5194/acp-9-7691-2009">https://doi.org/10.5194/acp-9-7691-2009</a>, 2009.