ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-9-3253-2009 Variable CCN formation potential of regional sulfur emissions Manktelow P. T. 1 Carslaw K. S. 1 Mann G. W. 1 Spracklen D. V. 1 School of Earth and Environment, University of Leeds, Leeds, UK 20 05 2009 9 10 3253 3259 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/9/3253/2009/acp-9-3253-2009.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/9/3253/2009/acp-9-3253-2009.pdf

Aerosols are short lived so their geographical distribution and impact on climate depends on where they are emitted. Previous model studies have shown that the mass of sulfate aerosol produced per unit sulfur emission (the sulfate burden potential) and the associated direct radiative forcing vary regionally because of differences in meteorology and photochemistry. Using a global model of aerosol microphysics, we show that the total number of aerosol particles produced per unit sulfur emission (the aerosol number potential) has a different regional variation to that of sulfate mass. The aerosol number potential of N. American and Asian emissions is calculated to be a factor of 3 to 4 times greater than that of European emissions, even though Europe has a higher sulfate burden potential. Pollution from N. America and Asia tends to reach higher altitudes than European pollution so forms more new particles through nucleation. Regional differences in particle production and growth mean that sulfur emissions from N. America and E. Asia produce 50 nm diameter cloud condensation nuclei up to 70% more efficiently than Europe. For 80 nm diameter CCN, N. America and Europe produce CCN 2.5 times more efficiently than E. Asia. The impact of regional sulfur emissions on particle concentrations is also much more widely spread than the impact on sulfate mass, due to efficient particle production in the free troposphere during long range transport. These results imply that regional sulfur emissions will have different climate forcing potentials through changes in cloud drop number.

 References Adams P. J. and Seinfeld, J. H.: Predicting global aerosol size distributions in general circulation models, J. Geophys. Res., 107(D19), 4370, doi:10.1029/2001JD001010, 2002. Benkovitz, C. M.: Global gridded inventories of anthropogenic emissions of sulfur and nitrogen, J. Geophys. Res., 101, 29239–29253, 1996. Berntsen, T., Fuglestvedt, J. S., Joshi, M., Shine, K. P., Stuber, N., Sausen, R., Li, L., Hauglustaine, D. A., and Ponater, M.: Climate response to regional emissions of ozone precursors: Sensitivities and warming potentials, Tellus, Ser. B, 57, 283–304, 2005. Bond, T. C., Streets, D. G., Yarber, K. F., Nelson, S. M., Woo, J. H., and Kilmont, Z.: A technology-based global inventory of black and organic carbon emissions from combustion, J. Geophys. Res., 109, D14203, doi:10.1029/2003JD003697, 2004. Chin, M., Savoie, D. L., Huebert, B. J., Bandy, A. R., Thornton, D. C., Bates, T. S., Quinn, P. K., Satzmann, E. S., and De Bruyn, W. J.: Atmospheric sulfur cycle simulated in the global model GOCART: Comparison with field observations and regional budgets, J. Geophys. Res., 105(D20), 24689–24712, 2000. Chipperfield, M.: New version of the TOMCAT/SLIMCAT off-line chemical transport model: Intercomparison of stratospheric tracer experiments, Q. J. R. Meteor. Soc., 132(617), 1179–1203, 2006. Clarke, A. and Kapustin, V.: A Pacific Aerosol Survey. Part I: A Decade of Data on Particle Production, Transport, Evolution, and Mixing in the Troposphere, J. Atmos. Sci., 59, 363–382, 2002. Cofala, J., Amann, M., Kilmont, Z., and Schopp, W.: Scenarios of world anthropogenic emissions of SO<sub>2</sub>, NO<sub>x</sub>, and CO up to 2030, internal report, Transboundary Air Pollut. Programme, Int. Inst. for Appl. Syst. Anal., Laxenburg, Austria, 2005. Curtius, J., Lovejoy, E. R., and Froyd, K. D.: Atmospheric ion-induced aerosol nucleation, Space Sci. Rev., 125, 159–167, 2006. Eckhardt, S., Stohl, A., Wernli, H., James, P., Forster, C., and Spichtinger, N.: A 15-year climatology of warm conveyor belts, J. Climate, 17, 218–237, 2004. 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. Halmer, M., Schmincke, H., and Graf, H.: The annual volcanic gas input into the atmosphere, in particular into the stratosphere: A global data-set for the past 100 years, J. Volca. Geotherm. Res., 115, 511–-528, 2002. Hermann, M., Brenninkmeijer, C. A. M., Slemr, F., et al.: Submicrometer aerosol particle distributions in the upper troposphere over the mid-latitude North Atlantic – Results from the third route of "CARIBIC", Tellus B, 60(1), 106–117, 2008. IPCC: Climate Change 2007: The Physical Science Basis, Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K. B., Tignor, M., and Miller, H. L., Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 996 pp., 2007. Kettle, A. J. and Andreae, M. O.: Flux of dimethylsulfide from the oceans: A comparison of updated data sets and flux models, J. Geophys. Res., 105(D22), 26793–26808, 2000. 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., 112, D02205, doi:10.1029/2005JD007024, 2007. Kulmala, M., Laaksonen, A., and Pirjola, L.: Parameterizations for sulfuric acid/water nucleation rates, J. Geophys. Res.-Atmos., 103, 8301–8307, 1998. Lee, S. H., Reeves, J. M., Wilson, J. C., Hunton, D. E., Viggiano, A. A., Miller, T. M., Ballenthin, J. O., and Lait, L. R.: Particle formation by ion nucleation in the upper troposphere and lower stratosphere, Science, 301, 1886–1889, 2003. Lucas, D. D. and Prinn, R. G.: Tropospheric distributions of sulfuric acid-water vapor aerosol nucleation rates from dimethylsulfide oxidation, Geophys. Res. Lett., 30(22), 2136, doi:10.1029/2003GL018370, 2003. Manktelow, P. T., Mann, G. W., Carslaw, K. S., Spracklen, D. V., and Chipperfield, M. P.: Regional and global trends in sulfate aerosol since the 1980s, Geophys. Res. Lett., 34, L14803, doi:10.1029/2006GL028668, 2007. Nightingale, P. D., Malin, G., Law, C. S., Watson, A. J., Liss, P. S., Liddicoat, M. I., Boutin, J., and Upstill-Goddard, R. C.: In situ evaluation of air-sea gas exchange parameterizations using novel conservative and volatile tracers, Global Biogeochem. Cy., 14, 373–388, doi:10.1029/1999GB900091, 2000. Olivier, J. G. J. and Berdowski, J. J. M.: Global emissions sources and sinks, in The Climate System, edited by: Berdowski, J., Guicherit, R., and Heij, B. J., 33–78, A A Balkema, Brookfield, Vt, 2001. Rasch, P. J., Barth, M. C., Kiehl, J. T., Schwartz, S. E., and Benkovitz, C. M.: A description of the global sulfur cycle and its controlling processes in the National Center for Atmospheric Research Community Climate Model, Version 3, J. Geophys. Res., 105(D1), 1367–1385, 2000. Rypdal, K., Berntsen, T., Fuglestvedt, J. S., Torvanger, A., Aunan, K., Stordal, F., and Nygaard, L. P.: Tropospheric ozone and aerosols in climate agreements: Scientific and political challenges, Environ. Sci. Policy, 8, 29–43, 2005. Schröder, F.P., Kärcher, B., Fiebig, M., and Petzold, A.: Aerosol states in the free troposphere at northern midlatitudes, J. Geophys. Res., 107(D21), 8126, doi:1029/2000JD000194, 2002. Shine, K. P., Berntsen, T. K., Fuglestvedt, J. S., and Sausen, R.: Scientific issues in the design of metrics for inclusion of oxides of nitrogen in global climate agreements, Proc. Natl. Acad. Sci., 102, 15768–15773, 2005. 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, 2005a. 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, 2005b. 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, doi:10.1029/2007GL033038, 2008. 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. Stohl, A.: A 1-year Lagrangian "climatology" of airstreams in the Northern Hemisphere troposphere and lowermost stratosphere, J. Geophys. Res., 106(D7), 7263–7279, 2001. Stohl, A., Eckhardt, S., Forster, C., James, P., and Spichtinger, N.: On the pathways and timescales of intercontinental air pollution transport, J. Geophys. Res., 107(D23), 4684, doi:10.1029/2001JD001396, 2002. 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, 2008. Unger, N., Shindell, D. T., Koch, D. M., and Streets, D. J.: Air pollution radiative forcing from specific emissions sectors at 2030, J. Geophys. Res., 113, D02306, doi:10.1029/2007JD008683, 2008. Van der Werf, G. R., Randerson, J. T., Collatz, G. J., and Giglio, L.: Carbon emissions from fires in tropical and subtropical ecosystems, Global Change Biol., 9, 547–562, 2003. Vehkamäki, H., Kulmala, M., Napari, I., Lehtinen, K., Timmreck, C., Noppel, M., and Laaksonen, A.: An improved parametrization for sulfuric acid-water nucleation rates for tropospheric and stratospheric conditions, J. Geophys. Res., 107, 4622–4631, 2002. Yu, F.: From molecular clusters to nanoparticles: second-generation ion-mediated nucleation model, Atmos. Chem. Phys., 6, 5193–5211, 2006.