Multiphase Atmospheric Chemistry: Implications for Climate

  • Robert J. Charlson
  • Jos Lelieveld
Part of the Environmental Science Research book series (ESRH, volume 48)

Abstract

While it has been known for over a century that atmospheric aerosol particles are an important factor governing the interaction of solar radiation with the earth, both through direct influences on solar radiation and indirectly as cloud condensation nuclei, the large degree of variability in both aerosol composition and concentration precluded all but crude global appraisals of the actual climate forcing (W m2). The advent of global chemical reaction/transport/removal models, including parameterizations of heterogeneous processes, has made it possible to estimate the direct climatic forcing for sulfate aerosol and for condensed organic materials from biomass combustion. Thus the study of multiphase atmospheric chemistry has made possible a species-by-species and mechanism-by-mechanism approach to assessing these physical effects. Examination of the generalized heat balance equation for the earth suggests that there must be numerous other important aerosol species and several more mechanisms by which climate is affected. To date, the assessment of effects by anthropogenic sulfate and smoke from biomass combustion indicate that these aerosols cause a climatic forcing that, when averaged over the northern hemisphere, is comparable in magnitude but opposite in sign to the “greenhouse” forcing by CO2, CH4, chlorofluorocarbons, etc. Three steps are involved in these coupled chemical/radiative transfer models: simulation of the geographically, time and height dependent aerosol formation process, prediction of the microphysical properties as functions of the source processes or species characteristics, and coupling of these to geographically dependent radiative transfer calculations. We first present a description of the main aerosol production mechanisms and resultant physical properties. Subsequently we address the direct and indirect (CCN-cloud albedo) radiative forcings, leaving open the important questions of influence of aerosol particles on cloud amount and cloud-droplet longevity. Furthermore, we discuss multiphase chemical processes that affect the abundance of tropospheric O3, the latter being a potent greenhouse gas. We will emphasize the importance of the open scientific questions, concluding that it is not yet possible to quantify climate forcing by anthropogenic or natural aerosols fully. Finally, we describe the approach of the IGAC Multiphase Atmospheric Chemistry (MAC) Activity to improve the understanding of these issues.

Keywords

Biomass Combustion Formaldehyde Dioxide Dust 

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References

  1. Aitken, J., 1880-1, On dust, fogs and clouds, Trans. Roy. Soc. Edinb., 30:337.Google Scholar
  2. Ångström, A., 1929, On the atmospheric transmission of sun radiation and dust in the air, Geograph. Annal., 11:156–166.CrossRefGoogle Scholar
  3. Ball, R.J. and G.D. Robinson, 1982, The origin of haze in the central U.S. and its effects on solar radiation, J. Appl. Meteorol., 21:171–188.CrossRefGoogle Scholar
  4. Behra, P. and L. Sigg, 1990, Evidence for redox cycling of iron in atmospheric water droplets, Nature, 344:419–CrossRefGoogle Scholar
  5. Bergeron, T., 1928, “Über die dreidimensional verknüpfende Wetter analyse,” Geof. Pub, V, No. 16, Oslo.Google Scholar
  6. Bolin, B. and R. J. Charlson, 1976, On the role of the tropospheric sulfur cycle in the short wave radiative climate of the earth, Ambio, 2:4754.Google Scholar
  7. Charlson, R.J., J. Langner, H. Rodhe, C.B. Leovy and S.G. Warren, 1991, Perturbation of the northern hemisphere radiative balance by backscattering from anthropogenic sulfate aerosols, Tellus, 43AB:152–163.Google Scholar
  8. Charlson, R.J., S.E. Schwartz, J.M. Hales, R.D. Cess, J.A. Coakley, Jr., J.E. Hansen and D.J. Hofmann, 1992, Climate forcing by anthropogenic aerosols, Science, 255:423–430.PubMedCrossRefGoogle Scholar
  9. Crutzen, P.J. and P.H. Zimmermann, 1991, The changing photochemistry of the troposphere, Tellus, 43AB:136–151.Google Scholar
  10. Dentener, F. and P.J. Crutzen, 1993, Reaction of N2Q5 on tropospheric aerosols: impact on the global distributions of NOX, O3 and OH, J. Geophys. Res., in press.Google Scholar
  11. Flowers, E.C., R.A. McCormick and K.R. Kurtis, 1969, Turbidity over the United States 1961-1966, J. Appl. Meteorol., 8:955–962.CrossRefGoogle Scholar
  12. Hegg, D.A., 1985, The importance of liquid-phase oxidation of SO2 in the troposphere, J. Geophys. Res., 90:3773–3779.CrossRefGoogle Scholar
  13. Herrmann, H., M. Esner and H. Zellner, 1992, Laser based studies of reactions of the nitrate radical in aqueous solution, Ber. Bunsenges. Phys. Chem., 96:470–485.CrossRefGoogle Scholar
  14. Köhler, H., 1926, Zur Kondensation des Wasser dampfes in der Atmosphäre, Geofys. Publ., 2, 3, 6, 26.Google Scholar
  15. Langner, J and H. Rodhe, 1991, A global three-dimensional model of the tropospheric sulfur cycle, J. Atm. Chem, 13:225–263.CrossRefGoogle Scholar
  16. Lelieveld, J., 1993, Multi-phase processes in the atmospheric sulfur cycle, in: “Interactions of C, N, P and S biogeochemical cycles and global change,” H. Wollast, F. T. Mackenzie and L. Chou (eds.), NATO ASI Series I, Vol. 4, Springer Verlag, Berlin, pgs. 305–331.CrossRefGoogle Scholar
  17. Lelieveld, J. and P.J. Crutzen, 1990, Influences of cloud photochemical processes on tropospheric ozone, Nature, 343:221–233.CrossRefGoogle Scholar
  18. Lelieveld, J. and J. Heintzenberg, 1992, Sulfate cooling effect on climate through in-cloud oxidation of anthropogenic SO4= Science, 258:117–120.PubMedCrossRefGoogle Scholar
  19. Mayewski, P.A., W.B. Lyons, M.J. Spencer, M.S. Twickler, C.F. Buck and S. Whitlow, 1990, An ice-core record of atmospheric response to anthropogenic sulfate and nitrate, Nature, 346: 554–556.CrossRefGoogle Scholar
  20. Ogren, J.A. and R.J. Charlson, 1992, Implications for models and measurements of chemical inhomogeneities among cloud droplets, Tellus, 44B:208–225.Google Scholar
  21. Platt, U.F., A.M. Winer, H.W. Biermann, R. Atkinson and J.N. Pitts Jr., 1984, Measurement of nitrate radical concentrations in continental air, Environ. Sci. Technol., 18:356–369.CrossRefGoogle Scholar
  22. Pruppacher, H.R. and J.D. Klett, 1980, “Microphysics of Clouds and Precipitation,” Reidel, Dordrecht, 714 pp.Google Scholar
  23. Raes, F., 1992, private communication.Google Scholar
  24. Sievering, H., J. Boatman, E. Gorman, Y. Kim, L. Anderson, G. Ennis, M. Luria and S. Pandis, 1992, Removal of sulfur from the marine boundary layer by ozone oxidation in sea-salt aerosols, Nature, 360:571–573.CrossRefGoogle Scholar
  25. Twomey, S., 1977, “Atmospheric Aerosols,” Elsevier, Amsterdam, 302 pp.Google Scholar
  26. Tyndall, J. (1861) On the absorption and radiation of heat by gases and vapors, and on the physical connexion of radiation, absorption and conduction, Phil. Mag. &, 4,22, No. 446.Google Scholar

Copyright information

© Springer Science+Business Media New York 1994

Authors and Affiliations

  • Robert J. Charlson
    • 1
  • Jos Lelieveld
    • 2
  1. 1.Department of Atmospheric SciencesUniversity of Washington/BG-10SeattleUSA
  2. 2.Atmospheric Chemistry DivisionMax-Planck-Institut for ChemistryGermany

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