ACPD Atmospheric Chemistry and Physics Discussions ACPD 1680-7375 Copernicus GmbH Göttingen, Germany 10.5194/acpd-9-22365-2009 Sulfur cycle and sulfate radiative forcing simulated from a coupled global climate-chemistry model Tsai I.-C. 1 Chen J.-P. 1 Lin P.-Y. 1 Wang W.-C. 2 Isaksen I. S. A. 3 Department of Atmospheric Sciences, National Taiwan University, Taiwan Atmospheric Sciences Research Center, State University of New York at Albany, USA Department of Geosciences, University of Oslo, Norway 22 10 2009 9 5 22365 22406 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-discuss.net/9/22365/2009/acpd-9-22365-2009.html The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/9/22365/2009/acpd-9-22365-2009.pdf

The sulfur cycle and radiative effects of sulfate aerosol on climate are studied with a Global tropospheric Climate-Chemistry Model in which chemistry, radiation and dynamics are fully coupled. Production and removal mechanisms of sulfate are analyzed for the conditions of natural and anthropogenic sulfur emissions. Results show that the 1985 anthropogenic emission doubled the global SO<sub>2</sub> and sulfate loadings from its natural value of 0.15 and 0.27 Tg S, respectively. Under natural conditions, the fraction of sulfate produced in-cloud is 87%, and the lifetime of SO<sub>2</sub> and sulfate are 1.8 and 4.0 days, respectively; whereas with anthropogenic emissions, changes in in-cloud sulfate production are small, while SO<sub>2</sub> and sulfate lifetimes are significant reduced (1.0 and 2.4 days, respectively). The doubling of sulfate results in a direct radiative forcing of &minus;0.32 and &minus;0.14 W m<sup>&minus;2</sup> under clear-sky and all-sky conditions, respectively, and a significant first indirect forcing of &minus;1.69 W m<sup>&minus;2</sup>. The first indirect forcing is sensitive to the relationship between aerosol concentration and cloud droplet number concentration. Two aspects of chemistry-climate interaction are addressed. Firstly, the coupling effects lead to 10% and 2% decreases in sulfate loading, respectively, for the cases of natural and anthropogenic added sulfur emissions. Secondly, only the indirect effect of sulfate aerosols yields significantly stronger signals in changes of near surface temperature and sulfate loading than changes due to intrinsic climate variability, while other responses to the indirect effect and all responses to the direct effect are weak.

 References Albrecht,~B A.: Aerosols, cloud microphysics, and fractional cloudiness, Science, 245, 1227–1230, 1989. Amels,~P., Elias,~H., Götz,~U., Steingens,~U., and Wannowius,~K J.: Kinetic investigation of the stability of peroxonitric acid and of its reaction with sulfur (IV) in aqueous solution, in: Heterogeneous and Liquid Phase Processes, Springer-Verlag, New York, 77–88, 1996. Anderson,~T L., Charlson,~R J., Schwartz,~S E., Knutti,~R., Boucher,~O., Rodhe,~H., and Heintzenberg,~J.: Climate forcing by aerosols – a~hazy picture, Science, 300, 1103–1104, 2003. Audiffren,~N., Buisson,~E., Cautenet,~S., and Chaumerliac,~N.: Photolytic impact of a~stratocumulus cloud layer upon the chemistry of an offshore advected plume of pollutants during the NARE 1993 intensive experiment: a~numerical study, Atmos. Res., 70, 89–108, 2004. Benkovitz,~C M., Scholtz,~M T., Pacyna,~J., Tarraso'n,~L., Dignon,~J., Voldner,~E C., Spiro,~P A., Logan,~J A., and Graedel,~T E.: Global gridded inventories of anthropogenic emissions of sulfur and nitrogen, J. Geophys. Res., 101, 29239–29253, 1996. 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., 109, D19310, doi:10.1029/2003JD003948, 2004. Berntsen,~T K. and Isaksen,~I S A.: A~global 3-D chemical transport model for the troposphere; 1. Model description and CO and ozone results, J. Geophys. Res., 102, 21239–21280, 1997. Boucher,~O. and Anderson,~T L.: General circulation model assessment of the sensitivity of direct climate forcing by anthropogenic sulfate aerosols to aerosol size and chemistry, J. Geophys. Res., 100(D12), 26117–26134, 1995. Boucher,~O. and Lohmann,~U.: The sulfate-CCN-cloud albedo effect: A~sensitivity study with two general circulation models, Tellus, 47B, 281–300, 1995. Cerveny,~R S. and Balling Jr.,~R C.: Weekly cycles of air pollutants, precipitation and tropical cyclones in the coastal NW Atlantic region, Nature, 394, 561–563, 1998. Chen, Y. and Penner, J. E.: Uncertainty analysis for estimates of the first indirect aerosol effect, Atmos. Chem. Phys., 5, 2935–2948, 2005. Chin,~M., Jacob,~D J., Gardner,~G M., Foreman-Fowler,~M S., Spiro,~P A., and Savoie,~D L.: A~global three-dimensional model of tropospheric sulfate, J. Geophys. Res., 101, 18667–18690, 1996. Chin,~M., Savoie,~D L., Huebert,~B J., Bandy,~A R., Thornton,~D C., Bates,~T S., Quinn,~P K., Saltzman,~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, 24689–24712, 2000. Chou,~C., Neelin,~J D., Lohmann,~U., and Feichter,~J.: Local and remote impacts of aerosol climate forcing on tropical precipitation, J. Climate, 18, 4621–4636, 2005. Chuang,~C C., Penner,~J E., Taylor,~K E., Grossman,~A S., and Walton,~J. ~J.: An assessment of the radiative effects of anthropogenic sulfate, J. Geophys. Res., 102(D3), 3761–3778, 1997. DeMore,~W B., Sander,~S P., Golden,~D M., Hampson,~R F., Kurylo,~M J., Howard,~C J., Ravishankara,~A R., Kolb,~C E., and Molina,~M J.: Chemical kinetics and photochemical data for use in stratospheric modeling, Tech. Rep. 97–4, Jet Propulsion Lab., Pasadena, Calif., 1997. Endresen, Ø., Sørg&aring;rd,~E., Sundet,~J K., Dalsøren,~S B., Isaksen,~I S A., Berglen,~T F., and Gravir,~G.: Emission from international sea transportation and environment impact, J. Geophys. Res., 108(D17), 4560, doi:10.1029/2002JD002898, 2003. Eyring,~V., Köhler,~H W., van Aardenne,~J., and Lauer,~A.: Emission from international shipping: 1. The last 50 years, J. Geophys. Res., 110, D17305, doi:10.1029/2004JD005619, 2005. Feichter,~J., Kjellström,~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(10–11), 1693–1707, 1996. Gates,~W L., Boyle,~J., Covey,~C., Dease,~C., Doutriaux,~C., Drach,~R., Fiorino,~M., Gleckler,~P., Hnilo,~J., Marlais,~S., Phillips,~T., Potter,~G., Santer,~B., Sperber,~K., Taylor,~K., and Williams,~D.: An overview of the results of the Atmospheric Model Intercomparison Project (AMIP I), Bull. Am. Meteorol. Soc., 80, 29–55, 1999. Ghan,~S., Easter,~R., Chapman,~E., Abdul-Razzak,~H., Zhang,~Y., Leung,~R., Laulainen,~N., Saylor,~R D., and Zaveri,~R.: A~physically-based estimate of radiative forcing by anthropogenic sulphate aerosol, J. Geophys. Res., 106(D6), 5279–5294, doi:10.1029/2000JD900503, 2001. Graft,~H., Feichter,~J., and Langmann,~B.: Volcanic sulfur emissions: Estimates of sources strength and its contribution to the global sulfate distribution, J. Geophys. Res., 102, 10727–10738, 1997. Gu,~Y., Liou,~K N., Xue,~Y., Mechoso,~C R., Li,~W., and Luo,~Y.: Climatic effects of different aerosol types in China simulated by the UCLA general circulation model, J. Geophys. Res., 111, D15201, doi:10.1029/2005JD006312, 2006. Hack,~J J., Kiehl,~J T., and Hurrell,~J W.: The hydrologic and thermodynamic characteristics of the NCAR CCM3, J. Climate, 11, 1179–1206, 1998. Hansen,~J., Sato,~M., and Ruedy,~R.: Radiative forcing and climate response, J. Geophys. Res., 102(D6), 6831–6864, 1997. Haywood,~J M. and Shine,~K P.: Multi-spectral calculations of the direct radiative forcing of tropospheric sulphate and soot aerosols using a~column model,~Q J Roy. Meteorol. Soc., 123, 1907–1930, 1997. Haywood,~J M., Ramaswamy,~V., and Soden,~B J.: Tropospheric aerosol climate forcing in clear-sky satellite observations over the oceans, Science, 283, 1299–1305, 1999. Huang,~Y., Chameides,~W L., and Dickinson,~R E.: Direct and indirect effects of anthropogenic aerosols on regional precipitation over east Asia, J. Geophys. Res., 112, D03212, doi:10.1029/2006JD007114, 2007. 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 Univ. Press, Cambridge, UK, and New York, USA, 2007. Isaksen,~I S A. and Hov,~Ø.: Calculations of trends in the tropospheric concentrations of \chemO_3, OH, CO, \chemCH_4, and \chemNO_x, Tellus B, 39, 271–283, 1987. Iversen,~T., Kirkev&aring;g,~A., Kristjansson,~J E., and Seland, Ø.: Climate effects of sulphate and black carbon estimated in a~global climate model. in: Air Pollution Modeling and its Application XIV, Kluwer/Plenum Publishers, New York, 335–342, 2000. Iversen,~T. and Seland, Ø.: A~scheme for process-tagged SO4 and BC aerosols in NCAR CCM3: Validation and sensitivity to cloud processes, J. Geophys. Res., 107(D24), 4751, doi:10.1029/2001JD000885, 2002. Jacobson,~M Z.: Global direct radiative forcing due to multicomponent anthropogenic and natural aerosols, J. Geophys. Res., 106, 1551–1568, 2001. Jones,~A., Roberts,~D L., and Woodage,~M J.: Indirect sulphate aerosol forcing in a climate model with an interactive sulfur cycle, J. Geophys. Res., 106, 20293–20310, 2001. Jones,~A., Haywood,~J M., and Boucher,~O.: Aerosol forcing, climate response and climate sensitivity in the Hadley Centre climate model, J. Geophys. Res., 112, D20211, doi:10.1029/2007JD008688, 2007. Kaufman,~Y J. and Fraser,~R S.: The effect of smoke particles on clouds and climate forcing, Science, 277(5332), 1636–1638, 1997. Kettle, A. J., Andreae, M. O., Amouroux, 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., Novo, A., Putaud, J. P., Rapsomanikis, S., Roberts, G., Schebeske, G., Sharma, S., Simó, R., Staubes, R., Turner, S., and Uher, G.: A~global database of sea surface dimethylsulfide (DMS) measurements and a~procedure to predict sea surface DMS as a~function of latitude, longitude and month, Global Biogeochem. Cy., 13(2), 399–444, 1999. Kettle,~A J. and Andreae,~M O.: Flux of dimethylsulfide from the oceans: A~comparison of updated data seas and flux models, J. Geophys. Res., 105(D22), 26793–26808, 399–444, 2000. Kiehl,~J T. and Briegleb,~B P.: The relative roles of sulfate aerosols and greenhouse gases in climate forcing, Science, 260, 311–314, 1993. Kiehl,~J T. and Rodhe,~H.: Modeling geographical and seasonal forcing due to aerosols, in: Aerosol Forcing of Climate,~J. Wiley and Sons Ltd, 281–296, 1995. Kiehl,~J T., Schneider,~T L., Rasch,~P J., Barth,~M C., and Wong,~J.: Radiative forcing due to sulfate aerosols from simulations with the National Center for Atmospheric Research Community Climate Model, Version 3, J. Geophys. Res., 105(D1), 1441–1457, 2000. Koch,~D., Jacob,~D J., Tegen,~I., Rind,~D., and Chin,~M.: Tropospheric sulfur simulation and sulfate direct radiative forcing in the Goddard Institute for Space Studies general circulation model, J. Geophys. Res., 104, 23799–23822, 1999. Koch,~D.: Transport and direct radiative forcing of carbonaceous and sulfate aerosols in the GISS GCM, J. Geophys. Res., 106(D17), 20311–20332, 2001. Langner,~J. and Rodhe,~H.: A~global three-dimensional model of the tropospheric sulfur cycle, J. Atmos. Chem., 13, 225–263, 1991. Lau,~K.-M., Kim,~J H., and Sud,~Y.: Intercomparison of hydrological processes in AMIP GCMs, Bull. Am. Meteorol. Soc., 77, 2209–2227, 1996. Lelieveld,~J.: Modeling of heterogeneous chemistry in the global troposphere. In: Chemistry of Aquatic Systems: Local and Global perspective, Kluwer Academic Publ., Dordrecht, 73–95, 1994. Liss,~P S. and Merlivat,~L.: Air-sea gas exchange rates: Introduction and synthesis, in: The Role of Air-Sea Exchange in Geochemical Cycling,~D. Reidel, Norwell, Mass., 113–127, 1986. Liu,~Y., Sun,~J., and Yang,~B.: The Effects of black carbon and sulfate aerosols in China regions on East Asia monsoons, Tellus B, 61(4), 642–656, 2009. Lohmann, U. and Feichter, J.: Global indirect aerosol effects: a review, Atmos. Chem. Phys., 5, 715–737, 2005. Martin,~G M., Johnson,~D W., and Spice,~A.: The measurements and parameterization of effective radius of droplets in warm stratocumulus clouds, J. Atmos. Sci., 51, 1823–1842, 1994. Martin,~L R. and Damschen,~D E.: Aqueous oxidation of sulfur dioxide by hydrogen peroxide at low pH, Atmos. Environ., 15, 1615–1621, 1981. Mickley,~L J., Murti,~P P., Jacob,~D J., Logan,~J A., Koch,~D M., and Rind,~D.: Radiative forcing from tropospheric ozone calculated with a~unified chemistry-climate model, J. Geophys. Res., 104, 30153–30172, 1999. Mitchell,~J F B., Johns,~T C., Gregory,~J M., and Tett,~F B.: Climate response to increasing levels of greenhouse gases and sulphate aerosols, Nature, 376, 501–504, 1995. Moller,~D.: Kinetic model of atmospheric \chemSO_2 oxidation based on published data, Atmos. Environ., 14, 1067–1076, 1980. Myhre,~G., Stordal,~F., Restad,~K., and Isaksen,~I S A.: Estimation of the direct radiative forcing due to sulphate and soot aerosols, Tellus, 50B, 463–477, 1998. Jöckel, P., Sander, R., Kerkweg, A., Tost, H., and Lelieveld, J.: Technical Note: The Modular Earth Submodel System (MESSy) – a new approach towards Earth System Modeling, Atmos. Chem. Phys., 5, 433-444, 2005. Penner,~J E., Chuang,~C C., and Grant,~K.: Climate forcing by carbonaceous and sulphate aerosols, Clim. Dynam., 14, 839–851, 1998 Quaas,~J. and Boucher,~O.: Constraining the first aerosol indirect radiative forcing in the LMDZ GCM using POLDER and MODIS satellite data, Geophys. Res. Lett., 32, L17814, doi:10.1029/2005GL023850, 2005. Ramanathan,~V., Crutzen,~P J., Kiehl,~J T., and Rosenfeld,~D.: Aerosols, climate, and the hydrological cycle, Science, 294, 2119–2124, 2001. Restad,~K., Isaksen,~I S A., and Berntsen,~T K.: Global distribution of sulfate in the troposphere: A~three-dimensional model study, Atmos. Environ., 32, 3593–3609, 1998. Rodhe,~H., and Isaksen,~I S A.: Global distribution of sulfur compounds in the troposphere estimated in a~height/latitude transport model,~J. Geophys. Res., 85, 7401–7409, 1980. Roelofs,~G.-J., Lelieveld,~J., and Ganzeveld,~L.: Simulation of global sulfate distribution and the influence on effective cloud drop radii with a~coupled photochemistry-sulfur cycle model, Tellus B, 50, 224–242, 1998. Rosenfeld,~D.: Suppression of rain and snow by urban and industrial air pollution, Science, 287(5459), 1793–1796, 2000. Rotstayn,~L D. and Penner,~J E.: Indirect aerosol forcing, quasi-forcing, and climate response, J. Climate, 14, 2960–2975, 2001. Schulz, M., Textor, C., Kinne, S., Balkanski, Y., Bauer, S., Berntsen, T., Berglen, T., Boucher, O., Dentener, F., Guibert, S., Isaksen, I. S. A., Iversen, T., Koch, D., Kirkev&aring;g, A., Liu, X., Montanaro, V., Myhre, G., Penner, J. E., Pitari, G., Reddy, S., Seland, Ø., Stier, P., and Takemura, T.: Radiative forcing by aerosols as derived from the AeroCom present-day and pre-industrial simulations, Atmos. Chem. Phys., 6, 5225–5246, 2006. Senior,~C A. and Mitchell,~J F B.: Carbon dioxide and climate: The impact of cloud parameterization, J. Climate, 6, 393–418, 1993. Shindell,~D T., Grenfell,~J L., Rind,~D., Grewe,~V., and Price,~C.: Chemistry-climate interaction in the GISS general circulation model: 1. Tropospheric chemistry model description and evaluation, J. Geophys. Res., 106, 8047–8076, 2001. Spiro,~P A., Jacob,~D J., and Logan,~J A.: Global inventory of sulfur emission with 1$^\circ \times 1^\circ$ resolution, J. Geophys. Res., 97, 6023–6036, 1992. Twomey,~S.: Pollution and the planetary albedo, Atmos. Environ., 8, 1251–1256, 1974. Van Dorland,~R., Dentener,~F J., and Lelieveld,~J.: Radiative forcing due to tropospheric ozone and sulfate aerosols, J. Geophys. Res., 102(D23), 28079–28100, 1997. Williams,~K D., Jones,~A., Roberts,~D L., Senior,~C A., and Woodage,~M. ~J.: The response of the climate system to the indirect effects of anthropogenic sulfate aerosols, Clim. Dynam., 17, 845–856, 2001. Wang,~W.-C., Liang,~X Z., Dudek,~M P., Pollard,~D., and Thompson,~S L.: Atmospheric ozone as a~climate gas, Atmos. Res., 37, 247–256, 1995. Wong,~S. and Wang,~W.-C.: Interhemispheric asymmetry in the seasonal variation of the zonal mean tropopause, J. Geophys. Res., 105, 26645–26659, 2000. Wong,~S. and Wang,~W.-C.: Tropical-extratropical connection in interannual variation of the tropopause: Comparison between NCEP/NCAR reanalysis and an atmospheric general circulation model, J. Geophys. Res., 108(D2), 4043, doi:10.1029/2001JD002016, 2003. Wong,~S., Wang,~W.-C., Isaksen,~I S A., Berntsen~T K., and Sundet,~J K.: A~global climate-chemistry model study of present-day tropospheric chemistry and radiative forcing from changes in tropospheric \chemO_3 since the preindustrial period, J. Geophys. Res., 109, D11309, doi:10.1029/2003JD003998, 2004. Zhang, Y.: Online-coupled meteorology and chemistry models: history, current status, and outlook, Atmos. Chem. Phys., 8, 2895–2932, 2008.