References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-6-4723-2006

Attribution of modeled atmospheric sulfate and SO2 in the Northern Hemisphere for June–July 1997

Benkovitz

C. M.

¹ Schwartz

S. E.

¹ Jensen

M. P.

¹ Miller

M. A.

Brookhaven National Laboratory, P.O. Box 5000, Upton, NY 11973, USA

23 10 2006

6 12 4723 4738

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Anthropogenic sulfate aerosol is a major contributor to shortwave radiative forcing of climate change by direct light scattering and by perturbing cloud properties and to local concentrations of atmospheric particulate matter. Here we analyze results from previously published calculations with an Eulerian transport model for atmospheric sulfur species in the Northern Hemisphere in June–July, 1997 to quantify the absolute and relative contributions of specific source regions (North America, Europe, and Asia) and SO2-to-sulfate conversion mechanisms (gas-phase, aqueous-phase and primary sulfate) to sulfate and SO2 column burdens as a function of location and time. Although material emitted within a given region dominates the sulfate and SO2 column burden in that region, examination of time series at specific locations shows that material imported from outside can make a substantial and occasionally dominant contribution. Frequently the major fraction of these exogenous contributions to the sulfate column burden was present aloft, thus minimally impacting air quality at the surface, but contributing substantially to the burden and, by implication, to radiative forcing and diminution of surface irradiance. Although the dominant sulfate formation pathway in the domain as a whole is aqueous-phase reaction in clouds (62%), in regions with minimum opportunity for aqueous-phase reaction gas-phase oxidation is dominant, albeit with considerable temporal variability depending on meteorological conditions. These calculations highlight the importance of transoceanic transport of sulfate, especially at the western margins of continents under the influence of predominantly westerly transport winds.

References 1

Allan, J. D., Bower, K. N., Coe, H., Boudries, H., Jayne, J. T., Canagaratna, M. R., Millet, D. B., Goldstein, A. H., Quinn, P. K., Weber, R. J., and Worsnop, D. R.: Submicron aerosol composition at Trinidad Head, California, during ITCT 2K2: Its relationship with gas phase volatile organic carbon and assessment of instrument performance, J. Geophys. Res.-Atmos., 109(D23), D23S24, doi:10.1029/2003JD004208, 2004.

Anderson, T. L., Charlson, R. J., Bellouin, N., Boucher, O., Chin, M., Christopher, S. A., Haywood, J., Kaufman, Y. J., Kinne, S., Ogren, J. A., Remer, L. A., Takemura, T., Tanré, D., Torres, O., Trepte, C. R., Wielicki, B. A., Winker, D. M., and Yu, H.: A-Train strategy for quantifying direct climate forcing by anthropogenic aerosols, Bull. Am. Meteorol. Soc., 86, 1795–1809, 2005.

Ansmann, A., Wandinger, U., Wiedensohler, A., and Leiterer, U.: Lindenberg Aerosol Characterization Experiment 1998 (LACE 98): Overview, J. Geophys. Res., 107(D21), 8129, doi:10.1029/2000JD000233, 2002.

Bates, T. S., Lamb, B. K., Guenther, A., Dignon, J., and Stoiber, R. E.: Sulfur Emissions to the Atmosphere from Natural Sources, J. Atmos. Chem., 14, 315–337, 1992.

Bellouin, N., Boucher, O., Haywood, J., and Reddy, M. S.: Global estimate of aerosol direct radiative forcing from satellite measurements, Nature, 438, 1138–1141, doi:10.1038/nature04348, 2005.

Benkovitz, C. M., Berkowitz, C. M., Easter, R. C., Nemesure, S., Wagener, R., and Schwartz, S. E.: Sulfate Over the North Atlantic and Adjacent Continental Regions: Evaluation for October and November, 1986 Using a Three-Dimensional Model Driven by Observation-Derived Meteorology, J. Geophys. Res., 99(D10), 20 725–20 756, 1994.

Benkovitz, C. M., Scholtz, M. T., Pacyna, J., Tarrasón, L., Dignon, J., Voldner, E. V., Spiro, P. A., Logan, J. A., and Graedel, T. E.: Global Gridded Inventories of Anthropogenic Emissions of Sulfur and Nitrogen, J. Geophys. Res., 101(D22), 29 239–29 253, 1996.

Benkovitz, C. M., Schwartz, S. E., and Kim, B.-G.: Evaluation of a Chemical Transport Model for Sulfate using ACE-2 Observations and Attribution of Sulfate Mixing Ratios to Source Regions and Formation Processes, Geophys. Res. Lett., 30(12), doi:10.1029/2003GL016942, 2003.

Benkovitz, C. M., Schwartz, S. E., Jensen, M. P., Miller, M. A., Easter, R. C., and Bates, T. S.: Modeling atmospheric sulfur over the Northern Hemisphere during the Aerosol Characterization Experiment 2 experimental period, J. Geophys. Res., 109, D22207, doi:10.1029/2004JD004939, 2004.

Bott, A.: A Positive Definite Advection Scheme Obtained by Nonlinear Renormalization of the Advective Fluxes, Mon. Wea. Rev., 117, 1006–1015, 1989.

Brasseur, G., Hauglustaine, D., Walters, S., Rasch, P., Müller, J., Granier, G., and Tie, X. X.: MOZART: A Global Chemical Transport Model for Ozone and Related Chemical Tracers. 1. Model Description, J. Geophys. Res., 103(D21), 28 265–28 289, 1998.

Charlson, R. J., Schwartz, S. E., Hales, J. M., Cess, R. D., Coakley Jr., J. A., Hansen, J. E., and Hofmann, D. J.: Climate forcing by anthropogenic aerosols, Science, 255, 423–430, 1992.

Damoah, R., Spichtinger, N., Forster, C., James, P., Mattis, I., Wandinger, U., Beirle, S., Wagner, T., and Stohl, A.: Around the World in 17 days – Hemispheric-Scale Transport of Forest Fire Smoke from Russia in May 2003, Atmos. Chem. Phys., 4, 1311–1321, 2004.

Dore, A. J., Johnson, D. W., Osborne, S. R., Choularton, T. W., Bower, K. N., Andreae, M. O., and Bandy, B. J.: Evolution of Boundary-Layer Aerosol Particles Due to In-Cloud Chemical Reactions During the 2nd Lagrangian Experiment of ACE-2, Tellus, 52B(2), 452–462, 2000.

Easter, R. C.: Two Modified Versions of Bott's Positive Definite Numerical Advection Scheme, Mon. Wea. Rev., 121, 297–304, 1993.

Easter, R. C. and Luecken, D. J.: A Simulation of Sulfur Wet Deposition and Its Dependence on the Inflow of Sulfur Species to Storms, Atmos. Environ., 22(12), 2715–2739, 1988.

European Centre for Medium-Range Weather Forecasts: IFS Documentation Cycle CY25r1 Parts I–VII, European Centre for Medium-Range Weather Forecasts, Reading, England, 2003.

Forster, C., Wandinger, U., Wotawa, G., James, P., Mattis, I., Althausen, D., Simmonds, P., O'Doherty, S., Jennings, S. G., Kleefeld, C., Schneider, J., Trickl, T., Kreipl, S., Jäger, H., and Stohl, A.: Transport of Boreal Forest Fire Emissions from Canada to Europe, J. Geophys. Res., 106(D19), 22 887–22 906, 2001.

Graf, H.-F., Feichter, J., and Langmann, B.: Volcanic Sulfur Emissions: Estimates of Source Strenght and Its Contribution to the Global Sulfate Distribution, J. Geophys. Res., 102(D9), 10 727–10 738, 1997.

Horowitz, L. W., Walters, S., Mauzerall, D., Emmons, L., Rasch, P., Granier, C., Tie, X., Lamarque, J. F., Schultz, M., and Brasseur, G.: A global simulation of tropospheric ozone and related tracers: Description and evaluation of MOZART, version 2, J. Geophys. Res., 108(D24), 4784, doi:10.1029/2002JD002853, 2003.

Husar, R. B., Tratt, D. M., Schichtel, B. A., Falke, S. R., Li, F., Jaffe, D., Gassó, S., Gill, T., Laulainen, N. S., Lu, F., Reheis, M. C., Chun, Y., Westphal, D., Holben, B. N., Gueymard, C., McKendry, I., Kuring, N., Feldman, G. C., McClain, C., Frouin, R. J., Merrill, J., DuBois, D., Vignola, F., Murayama, T., Nickovic, S., Wilson, W. E., Sassen, K., Sugimoto, N., and Malm, W. C.: Asian dust events of April 1998, J. Geophys. Res., 106(D16), 18 317–18 330, doi:10.1029/2000JD900788, 2001.

Jaffe, D., Anderson, T., Covert, D., Kotchenruther, R., Trost, B., Danielson, J., Simpson, W., Berntsen, T., Karlsdottir, S., Blake, D., Harris, J., Carmichael, G., and Uno, I.: Transport of Asian Air Pollution to North America, Geophys. Res. Lett., 26(6), 711–714, 1999.

Jaffe, D., McKendry, I., Anderson, T., and Price, H.: Six `New' Episodes of Trans-Pacific Transport of Air Pollutants, Atmos. Environ., 37, 391–404, 2003.

Jaffe, D., Bertschi, I., Jaeglé, L., Novelli, P., Reid, J. S., Tanimoto, H., Vingarzan, R., and Westphal, D. L.: Long-Range Transport of Siberian Biomass Burning Emissions and Impact on Surface Ozone in Western North America, Geophys. Res. Lett., 31, L16106, doi:10.1029/2004GL020093, 2004.

Johnson, D. W., Osborne, S., Wood, R., Suhre, K., Johnson, R., Businger, S., Quinn, P. K., Wiedensohler, A., Durkee, P. A., Russell, L. M., Andreae, M. O., O'Dowd, C., Noone, K. J., Bandy, B., Rudolph, J., and Rapsomanikis, S.: An Overview of the Lagrangian Experiments Undertaken During the North Atlantic Aeorosol Characterisation Experiment (ACE-2), Tellus, 52B(2), 290–320, 2000a.

Johnson, R., Businger, S., and Baerman, A.: Lagrangian Air Mass Tracking with Smart Balloons During ACE-2, Tellus, 52B(2), 321–334, 2000b.

Kettle, A. J., Andreae, M. O., Amoroux, D., Andreae, T. W., Bates, T. S., Berresheim, H., Bingemer, H., Boniforti, R., Curran, M. A. J., DiTullio, G. R., Helas, G., Jones, G. B., Keller, M. D., Kiene, R. P., Leck, C., Levasseur, M., Malin, G., Maspero, M., Matrai, P., McTaggart, A. R., Mihalopoulos, N., Nguyen, B. C., Nuovo, A., Putaud, J. P., Rapsomanikis, S., Roberts, G., Schbeske, G., Sharma, S., Simo, R., Staubes, R., Turner, S., and Uher, G.: A Global DataBase of Sea Surface Dimethyl Sulfide (DMS) Measurements and a Procedure to Predict Sea Surface DMS as a Function of Latitude, Longitude, and Month, Global Biogeochem. Cycles, 13, 399–444, 1999.

Liepert, B. G.: Observed Reductions of Surface Solar Radiation at Sites in the United States and Worldwide from 1961 to 1990, Geophys. Res. Lett., 29(10), 1421, doi:10.1029/2002GL014910, 2002.

Liss, P. S. and Merlivat, L.: Air-Sea Gas Exchange Rates: Introduction and Synthesis, in: The Rate of Air-Sea Exchange in Geochemical Cycling, edited by: Buat-Menard, P., D. Reidel Publishing Company, Dordrecht, p. 113–127, 1986.

Malcom, A. L., Derwent, R. G., and Maryon, R. H.: Modeling the Long-Range Transport of Secondary PM$_10$ to the UK, Atmos. Environ., 34(6), 881–894, 2000.

Martin, B. D., Fuelberg, H. E., Blake, N. J., Crawford, J. H., Logan, J. A., Blake, D. R., and Sachse, G. W.: Long-Range Transport of Asian Overflow to the Equatorial Pacific, J. Geophys. Res., 108(D2), 8322, doi:10.1029/2001JD001418, 2003.

NASA: Chemical Kinetics and Photochemical Data for Use in Stratospheric Modeling. Evaluation #12., pp. 266, National Aeronautics and Space Administration, Jet Propulsion Laboratory, Pasadena, 1997.

Olivier, J. G. J., Peters, J. A. H. W., Bakker, J., Berdowski, J. J. M., Visschedijk, A. J. H., and Bloos, J. P. J.: Applications of EDGAR: Emissions Database for Global Atmospheric Research, pp. 151, National Institute for Public Health and the Environment (RIVM)/Netherlands Organization for Applied Scientific Research (TNO), Bilthoven, The Netherlands, 2002.

Osborne, S. R., Johnson, D. W., Wood, R., Bandy, B. A., Andreae, M. O., O'Dowd, C. D., Glantz, P., Noone, K. J., Gerbig, C., Rudolph, J., Bates, T. S., and Quinn, P.: Evolution of the Aerosol, Cloud and Boundary-Layer Dynamic and Thermodynamic Characteristics During the 2nd Lagrangian Experiment of ACE-2, Tellus, 52B(2), 375–400, 2000.

Penner, J., Andreae, M., Annegarn, H., Barrie, L., Feichter, J., Hegg, D., Jayraman, A., Leaitch, R., Murphy, D., Nganga, J., and Pitari, G.: Aerosols, their Direct and Indirect Effects, in: Climate Change 2001: The Scientific Basis, edited by: Houghton, J. T., Din, Y., Griggs, D. J., Noguer, M., v. d. Linden, P. J., Dai, X., Maskell, K., and Johnson, C. A., Cambridge University Press, Cambridge, UK, p. 289–348, 2001.

Perry, K. D., Cahill, T. A., Schnell, R. C., and Harris, J. M.: Long-Range Transport of Anthropogenic Aerosols to the National Oceanic and Atmospheric Administration Baseline Station at Mauna Loa Observatory, Hawaii, J. Geophys. Res., 104(D15), 18 521–18 535, 1999.

Pielke, R. A., Cotton, W. R., Walko, R. L., Tremback, C. J., Lyons, W. A., Grasso, L. D., Nicholls, M. E., Moran, M. D., Wesley, D. A., Lee, T. J., and Copeland, J. H.: A comprehensive meteorological modeling system – RAMS, Meteorol. Atmos. Phys., 49, 69–91, 1992.

Piketh, S. J., Swap, R. J., Maenhaut, W., Annegarn, H. J., and Formetti, P.: Chemical Evidence of Long-Range Atmospheric Transport over Southern Africa, J. Geophys. Res., 107(D24), 4817, doi:10.1029/2002JD-2056, 2002.

Prospero, J. M.: Long-Term Measurements of the Transport of African Mineral Dust to the Southeastern United States: Implications for Regional Air Quality, J. Geophys. Res., 104(D13), 15 917–15 927, 1999.

Raes, F. and Bates, T.: ACE-2 North Atlantic Regional Aerosol Characterization Experiement, Office for Official Publications of the European Communities, Brussels-Luxembourg, 1995.

Ramaswamy, V., Boucher, O., Haigh, J., Hauglustaine, D., Haywood, J., Myhre, G., Nakajima, T., Shi, G. Y., and Solomon, S.: Radiative Forcing of Climate Change, in: Climate Change 2001: The Scientific Basis, edited by: Houghton, J. T., Din, Y., Griggs, D. J., Noguer, M., v. d. Linden, P. J., Dai, X., Maskell, K., and Johnson, C. A., Cambridge University Press, Cambridge, UK, p. 349–416, 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 NCAR CCM3., J. Geophys. Res., 105(D1), 1367–1385, 2000.

Schwartz, S. E.: Mass-Transport Limitation to the Rate of In-Cloud Oxidation of SO2: Re-Examination in the Light of New Data, Atmos. Environ., 22(11), 2491–2499, 1988.

Schwartz, S. E., Harshvardhan, and Benkovitz, C. M.: Influence of anthropogenic aerosol on cloud optical depth and albedo shown by satellite measurements and chemical transport modeling, Proc. Natl. Acad. Sci. USA, 99, 1784–1789, 2002.

Sheih, C. M., Wesely, M. L., and Walcek, C. J.: A Dry Deposition Module for Regional Acid Deposition, U.S. Environmental Protection Agency, Research Triangle Park, NC, 1986.

Stanhill, G. and Cohen, S.: Global Dimming: a Review of the Evidence for a Widespread and Significant Reduction in Global Radiation with Discussion of its Probable Causes and Possible Agricultural Consequences, Agric. and Forest Met., 107, 255–278, 2001.

U.S. Environmental Protection Agency: National Air Quality and Emissions Trends Report, 1999, p. 237, U.S. Environmental Protection Agency, Office of Air Quality Planning and Standards, Research Triangle Park, NC, 2001.

Uno, I., Carmichael, G. R., Streets, D. G., Tang, Y., Yienger, J. J., Satake, S., Wang, Z., Woo, J.-H., Guttikunda, S., Uematsu, M., Matsumoto, K., Tanimoto, H., Yoshioka, K., and Iida, T.: Regional Chemical Weather Forecasting System CFORS: Model Descriptions and Analysis of Surface Observations at Japanese Island Statons During the ACE-Asia Experiment, J. Geophys. Res., 108(D23), 8668, doi:10.1029/2002JD002845, 2003.

Walcek, C. J. and Taylor, G. R.: A Theoretical Method for Computing Vertical Distributions of Acidity and Sulfate Production Within Cumulus Clouds, J. Atmos. Sci., 43, 339–355, 1986.

Wandinger, U., Müller, D., Böckmann, C., Althausen, D., Matthias, V., Bösenberg, J., Weiß, V., Fiebig, M., Wendisch, M., Stohl, A., and Ansmann, A.: Optical and Microphysical Characterization of Biomass-Burning and Industrial-Pollution Aerosols from Multiwavelength Lidar and Aircraft Measurements, J. Geophys. Res., 107(D21), 8125, doi:10.1029/2000JD000202, 2002.

Wesely, M.: Parameterization of Surface Resistances to Gaseous Dry Deposition in Regional-Scale Numerical Models, Atmos. Environ., 23, 1293–1304, 1989.

Wotawa, G. and Trainer, M.: The Influence of Canadian Forest Fires on Pollutant Concentrations in the United States, Science, 288, 324–328, 2000.

Yienger, J. J., Galanter, M., Holloway, T. A., Phadnis, M. J., Guttikunda, S. K., Carmichael, G. R., Moximm, W. M., and II, H. L.: The Episodic Nature of Air Pollution Transport from Asia to North America, J. Geophys. Res., 105(D22), 26 931–26 946, 2000.

Yin, F., Grosjean, D., Flagan, R. C., and Seinfeld, J. H.: Photooxidation of Dimethyl Sulfide and Dimethyl Disulfide. II: Mechanism Evaluation, J. Atmos. Chem., 11, 365–399, 1990a.

Yin, F., Grosjean, D., and Seinfeld, J. H.: Photooxidation of Dimethyl Sulfide and Dimethyl Disulfide. I: Mechanism Development, J. Atmos. Chem., 11, 309–364, 1990b.