ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-8-3721-2008 Source-receptor relationships between East Asian sulfur dioxide emissions and Northern Hemisphere sulfate concentrations Liu J. 1 Mauzerall D. L. 1 Horowitz L. W. 2 Woodrow Wilson School of Public and International Affairs, Princeton University, Princeton, NJ, USA Geophysical Fluid Dynamics Laboratory, Princeton, NJ, USA 15 07 2008 8 14 3721 3733 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/8/3721/2008/acp-8-3721-2008.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/8/3721/2008/acp-8-3721-2008.pdf

We analyze the effect of varying East Asian (EA) sulfur emissions on sulfate concentrations in the Northern Hemisphere, using a global coupled oxidant-aerosol model (MOZART-2). We conduct a base and five sensitivity simulations, in which sulfur emissions from each continent are tagged, to establish the source-receptor (S-R) relationship between EA sulfur emissions and sulfate concentrations over source and downwind regions. We find that from west to east across the North Pacific, EA sulfate contributes approximately 80%–20% of sulfate at the surface, but at least 50% at 500 hPa. Surface sulfate concentrations are dominated by local anthropogenic sources. Of the sulfate produced from sources other than local anthropogenic emissions (defined here as "background" sulfate), EA sources account for approximately 30%–50% (over the Western US) and 10%–20% (over the Eastern US). The surface concentrations of sulfate from EA sources over the Western US are highest in MAM (up to 0.15 μg/m<sup>3</sup>), and lowest in DJF (less than 0.06 μg/m<sup>3</sup>). Reducing EA SO<sub>2</sub> emissions will significantly decrease the spatial extent of the EA sulfate influence (represented by the areas where at least 0.1 μg m<sup>&minus;3</sup> of sulfate originates from EA) over the North Pacific both at the surface and at 500 hPa in all seasons, but the extent of influence is insensitive to emission increases, particularly in DJF and JJA. We find that EA sulfate concentrations over most downwind regions respond nearly linearly to changes in EA SO<sub>2</sub> emissions, but sulfate concentrations over the EA source region increase more slowly than SO<sub>2</sub> emissions, particularly at the surface and in winter, due to limited availability of oxidants (in particular of H<sub>2</sub>O<sub>2</sub>, which oxidizes SO<sub>2</sub> to sulfate in the aqueous phase). We find that similar estimates of the S-R relationship for trans-Pacific transport of EA sulfate would be obtained using either sensitivity (i.e., varying emissions from a region to examine the effects on downwind concentrations) or tagging techniques. Our findings suggest that future changes in EA sulfur emissions may cause little change in the sulfate-induced health impact over downwind continents. However, SO<sub>2</sub> emission reductions may significantly reduce the sulfate concentrations and the resulting negative radiative forcing over the North Pacific and the United States, thus providing a warming tendency.

 References Berglen, T. F., Berntsen, T. K., Isaksen, I. S. A., and Sundet, J. K.: A global model of the coupled sulfur/oxidant chemistry in the troposphere: the sulfur cycle, J. Geophys. Res.-Atmos., 109, D19310, doi:10.1029/2003JD003948, 2004. Brasseur, G. P., Orlando, J. J., Tyndall, G. S., and National Center for Atmospheric Research (US): Atmospheric chemistry and global change, Topics in environmental chemistry, Oxford University Press, New York, USA, 18, 654 pp., 1999. Carlson, C., Burtraw, D., Cropper, M., and Palmer, K. L.: Sulfur dioxide control by electric utilities: what are the gains from trade?, J. Politic. Econ., 108, 1292–1326, 2000. Chin, M., Diehl, T., Ginoux, P., and Malm, W.: Intercontinental transport of pollution and dust aerosols: implications for regional air quality, Atmos. Chem. Phys., 7, 5501–5517, 2007. Conrad, K. and Kohn, R. E.: The US market for SO<sub>2</sub> permits: policy implications of the low price and trading volume, Energy Policy, 24, 1051–1059, 1996. Dutkiewicz, V. A., Das, M., and Husain, L.: The relationship between regional SO<sub>2</sub> emissions and downwind aerosol sulfate concentrations in the Northeastern US, Atmos. Environ., 34, 1821–1832, 2000. Feichter, J., Kjellstrom, E., Rodhe, H., Dentener, F., Lelieveld, J., and Roelofs, G. J.: Simulation of the tropospheric sulfur cycle in a global climate model, Atmos. Environ., 30, 1693–1707, 1996. Ginoux, P., Horowitz, L. W., Ramaswamy, V., Geogdzhayev, I. V., Holben, B. N., Stenchikov, G., and Tie, X.: Evaluation of aerosol distribution and optical depth in the geophysical fluid dynamics laboratory coupled model cm2.1 for present climate, J. Geophys. Res.-Atmos., 111, D22210, doi:10.1029/2005JD006707, 2006. Giorgi, F., Bi, X. Q., and Qian, Y.: Indirect vs. direct effects of anthropogenic sulfate on the climate of east asia as simulated with a regional coupled climate-chemistry/aerosol model, Clim. Change, 58, 345–376, 2003. Gunther, A. J.: A chemical survey of remote lakes of the Alagnak and Naknek river systems, Southwest Alaska, USA, Arctic Alpine Res., 24, 64–68, 1992. Hao, J. M., Wang, S. X., Liu, B. J., and He, K. B.: Plotting of acid rain and sulfur dioxide pollution control zones and integrated control planning in china, Water Air Soil Poll., 130, 259–264, 2001. Heald, C. L., Jacob, D. J., Park, R. J., Alexander, B., Fairlie, T. D., Yantosca, R. M., and Chu, D. A.: Transpacific transport of Asian anthropogenic aerosols and its impact on surface air quality in the United States, J. Geophys. Res.-Atmos., 111, D14310, doi:10.1029/2005JD006847, 2006. Hilst, G. R.: Proportionality between SO<sub>2</sub> emissions and wet SO4<sup>2</sup>-concentrations: the effect of area of averaging, Atmos. Environ. A-Gen., 26, 1413–1420, 1992. Horowitz, L. W., Walters, S., Mauzerall, D. L., Emmons, L. K., Rasch, P. J., Granier, C., Tie, X. X., Lamarque, J. F., Schultz, M. G., Tyndall, G. S., Orlando, J. J., and Brasseur, G. P.: A global simulation of tropospheric ozone and related tracers: Description and evaluation of Mozart – Version 2, J. Geophys. Res.-Atmos., 108(D24), 4784, doi:10.1029/2002JD002853, 2003. Horowitz, L. W.: Past, present, and future concentrations of tropospheric ozone and aerosols: methodology, ozone evaluation, and sensitivity to aerosol wet removal, J. Geophys. Res.-Atmos., 111, D22211, doi:10.1029/2005JD006937, 2006. Jaffe, D., Tamura, S., and Harris, J.: Seasonal cycle and composition of background fine particles along the West Coast of the US, Atmos. Environ., 39, 297–306, 2005. Klimont, Z., Cofala, J., Schopp, W., Amann, M., Streets, D. G., Ichikawa, Y., and Fujita, S.: Projections of SO<sub>2</sub>, NO<sub>x</sub>, NH<sub>3</sub> and VOC emissions in East Asia up to 2030, Water Air Soil Pollut., 130, 193–198, 2001. Koch, D., Bond, T. C., Streets, D., and Unger, N.: Linking future aerosol radiative forcing to shifts in source activities, Geophys. Res. Lett., 34, L05821, doi:10.1029/2006GL028360, 2007a. 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, 2007b. Kritz, M. A., Le Roulley, J. C., and Danielsen, E. F.: The china clipper: Fast advective transport of radon-rich air from the asian boundary layer to the upper troposphere near California, Tellus B, 42, 46–61, 1990. Levy, H., Schwarzkopf, M. D., Horowitz, L. W., Ramaswamy, V., and Findell, K.: Strong sensitivity of late 21st century climate to projected changes in short-lived air pollutants, J. Geophys. Res.-Atmos., 113, D06102, doi:10.1029/2007JD009176, 2008. Liu, H. Y., Jacob, D. J., Bey, I., Yantosca, R. M., Duncan, B. N., and Sachse, G. W.: Transport pathways for Asian pollution outflow over the Pacific: interannual and seasonal variations, J. Geophys. Res.-Atmos., 108(D20), 8786, doi:10.1029/2002JD003102, 2003. Liu, J. F. and Mauzerall, D. L.: Estimating the average time for inter-continental transport of air pollutants, Geophys. Res. Lett., 32, L11814, doi:10.1029/2005GL022619, 2005. Liu, J. F., Mauzerall, D. L., and Horowitz, L. W.: Analysis of seasonal and interannual variability in transpacific transport, J. Geophys. Res.-Atmos., 110, D04302, doi:10.1029/2004JD005207, 2005. Liu, J. F. and Mauzerall, D. L.: Potential influence of inter-continental transport of sulfate aerosols on air quality, Environ. Res. Lett., 2, 045029, doi:10.1088/1748-9326/1082/1084/045029, 2007. Marmer, E., Langmann, B., Fagerli, H., and Vestreng, V.: Direct shortwave radiative forcing of sulfate aerosol over Europe from 1900 to 2000, J. Geophys. Res.-Atmos., 112, D23S17, doi:10.1029/2006JD008037, 2007. Martin, L. R. and Damschen, D. E.: Aqueous oxidation of sulfur-dioxide by hydrogen-peroxide at low ph, Atmos. Environ., 15, 1615–1621, 1981. Moldan, F., Wright, R. F., Lofgren, S., Forsius, M., Ruoho-Airola, T., and Skjelkvale, B. L.: Long-term changes in acidification and recovery at nine calibrated catchments in Norway, Sweden and Finland, Hydrol. Earth Syst. Sc., 5, 339–349, 2001. NAPAP: National Acid Precipitation Assessment Program Report to Congress: an integrated assessment, Washington D.C., USA, available at: http://ny.cf.er.usgs.gov/napap/Information/NAPAP%20Report%208-22-05.pdf, 2005. 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.: Description of edgar version 2.0: a set of global emission inventories of greenhous gases and ozone-depleting substances for all anthropogenic and most natural sources on a per country basis and on 1ox1o grid, National Institute of Public Health and the Environment, The Netherlands, (RIVM) report no. 771060 771002 / TNO-MEP report no. R771096/771119. , 1996. Oppenheimer, M., Epstein, C. B., and Yuhnke, R. E.: Acid deposition, smelter emissions, and the linearity issue in the Western United States, Science, 229, 859–862, 1985. Park, R. J., Jacob, D. J., Field, B. D., Yantosca, R. M., and Chin, M.: Natural and transboundary pollution influences on sulfate-nitrate-ammonium aerosols in the United States: implications for policy, J. Geophys. Res.-Atmos., 109, D15204, doi:10.1029/2003JD004473, 2004. Pope, C., Burnett, R., Thun, M., Calle, E., Krewski, D., Ito, K., and Thurston, G.: Lung cancer, cardiopulmonary mortality, and long-term exposure to fine particulate air pollution, JAMA-J. Am. Med. Assoc., 287, 1132–1141, 2002. Pope, C., Burnett, R., Thurston, G., Thun, M., Calle, E., Krewski, D., and Godleski, J.: Cardiovascular mortality and long-term exposure to particulate air pollution: epidemiological evidence of general pathophysiological pathways of disease, Circulation, 109, 71–77, 2004. Prospero, J. M.: The atmospheric transport of particles to the ocean, in: Particle flux in the ocean, Scope 57, edited by: Ittekkot, V., Schäfer, P., Honjo, S., and Depetris, P. J., Wiley, New York, USA, 19–52, 1996. Prospero, J. M., Savoie, D. L., and Arimoto, R.: Long-term record of nss-sulfate and nitrate in aerosols on Midway Island 1981–2000: evidence of increased (now decreasing?) anthropogenic emissions from Asia, J. Geophys. Res.-Atmos., 108(D1), 4019, doi:10.1029/2001JD001524, 2003. Schwartz, J., Coull, B., Laden, F., and Ryan, L.: The effect of dose and timing of dose on the association between airborne particles and survival, Environ. Health Persp., 116, 64–69, 2008. Seinfeld, J. H. and Pandis, S. N.: Atmospheric chemistry and physics: from air pollution to climate change, Wiley, New York, USA, 1326 pp., 1998. Stohl, A.: A 1-year lagrangian "climatology" of airstreams in the Northern Hemisphere troposphere and lowermost stratosphere, J. Geophys. Res.-Atmos., 106, 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.-Atmos., 107(D23), 4684, doi:10.1029/2001JD001396, 2002. Streets, D. G.: Dissecting future aerosol emissions: warming tendencies and mitigation opportunities, Climatic Change, 81, 313–330, 2007. Tie, X., Brasseur, G., Emmons, L., Horowitz, L., and Kinnison, D.: Effects of aerosols on tropospheric oxidants: a global model study, J. Geophys. Res.-Atmos., 106, 22 931–22 964, 2001. Tie, X., Madronich, S., Walters, S., Edwards, D. P., Ginoux, P., Mahowald, N., Zhang, R. Y., Lou, C., and Brasseur, G.: Assessment of the global impact of aerosols on tropospheric oxidants, J. Geophys. Res.-Atmos., 110, D03204, doi:10.1029/2004JD005359, 2005.