Direct shortwave forcing of climate by the anthropogenic sulfate aerosol: Sensitivity to particle size, composition, and relative humidity

Recent estimates of global or hemispheric average forcing of climate by anthropogenic sulfate aerosol caused by scattering of shortwave radiation (“direct” effect) are uncertain by somewhat more than a factor of 2. The principal sources of this uncertainty are atmospheric chemistry properties (yield, residence time), and microphysical properties (scattering efficiency, upscatter fraction, and the dependence of these properties on particle size, composition, and relative humidity, (RH)). This paper examines the sensitivity of forcing to these microphysical properties to identify and improve understanding of the properties required to reduce the uncertainty in the forcing. The relations between aerosol loading and forcing developed here are suitable for comparing modeled and measured aerosol forcing at specific locations and for use in climate models, provided aerosol composition and microphysical properties are known, calculated, or assumed. Results are presented showing the dependence of scattering efficiency, upscatter fraction, and normalized forcing (W m−2/g(SO24−) m−2 or W g(SO24−)−1) on dry particle size (expressed as mole(sulfate) per particle), composition ((NH4)2SO4, NH4HSO4, H2SO4), solar zenith angle, latitude, and season. Forcing is strongly dependent on dry particle size and RH but is relatively insensitive to composition. The normalized forcing can be integrated over a known or assumed size distribution to evaluate the sulfate aerosol forcing. Global and annual average values of the normalized forcing are evaluated as a function of particle size and RH. Depending on values of these variables, normalized forcing may be less than, intermediate to, or greater than the range of previous estimates of sulfate aerosol forcing.

[1]  R. Charlson,et al.  Sulphate aerosol and climate , 1990, Nature.

[2]  Warren J. Wiscombe,et al.  The backscattered fraction in two-stream approximations. , 1976 .

[3]  J. A. Garland Condensation on ammonium sulphate particles and its effect on visibility , 1969 .

[4]  Olivier Boucher,et al.  General circulation model assessment of the sensitivity of direct climate forcing by anthropogenic sulfate aerosols to aerosol size and chemistry , 1995 .

[5]  K. E. Taylor,et al.  Response of the climate system to atmospheric aerosols and greenhouse gases , 1994, Nature.

[6]  K. T. Whitby THE PHYSICAL CHARACTERISTICS OF SULFUR AEROSOLS , 1978 .

[7]  Robert D. Cess,et al.  The Effect of Tropospheric Aerosols on the Earth's Radiation Budget: A Parameterization for Climate Models , 1983 .

[8]  J. Kiehl,et al.  The Relative Roles of Sulfate Aerosols and Greenhouse Gases in Climate Forcing , 1993, Science.

[9]  I. Tang,et al.  Aerosol growth studies—III ammonium bisulfate aerosols in a moist atmosphere , 1977 .

[10]  S. Schwartz,et al.  Seasonal, latitudinal, and secular variations in temperature trend: Evidence for influence of anthropogenic sulfate , 1993 .

[11]  S. Schwartz Are global cloud albedo and climate controlled by marine phytoplankton? , 1988, Nature.

[12]  B. Holben,et al.  Hemispherical backscattering by biomass burning and sulfate particles derived from sky measurements , 1996 .

[13]  T. Wigley,et al.  Implications for climate and sea level of revised IPCC emissions scenarios , 1992, Nature.

[14]  J. Penner,et al.  Quantifying and minimizing uncertainty of climate forcing by anthropogenic aerosols , 1994 .

[15]  T. Larson,et al.  Ubiquitous nature of ambient metastable aerosol , 1989, Nature.

[16]  J. Hansen,et al.  Light scattering in planetary atmospheres , 1974 .

[17]  W. John,et al.  Modes in the size distributions of atmospheric inorganic aerosol , 1990 .

[18]  J. Haywood,et al.  The effect of anthropogenic sulfate and soot aerosol on the clear sky planetary radiation budget , 1995 .

[19]  I. Tang,et al.  Water activities, densities, and refractive indices of aqueous sulfates and sodium nitrate droplets of atmospheric importance , 1994 .

[20]  Robert J. Charlson,et al.  Perturbation of the northern hemisphere radiative balance by backscattering from anthropogenic sulfate aerosols , 1991 .

[21]  J. Coakley,et al.  Climate Forcing by Anthropogenic Aerosols , 1992, Science.

[22]  S. Schwartz The whitehouse effect—Shortwave radiative forcing of climate by anthropogenic aerosols: an overview , 1996 .

[23]  Christine A. O'Neill,et al.  Effects of Aerosol from Biomass Burning on the Global Radiation Budget , 1992, Science.

[24]  J. W. Fitzgerald,et al.  Aerosol size distributions and optical properties found in the marine boundary layer over the Atlantic Ocean , 1990 .

[25]  T. L. Wolfe,et al.  An assessment of the impact of pollution on global cloud albedo , 1984 .

[26]  P. Hobbs,et al.  Light scattering and cloud condensation nucleus activity of sulfate aerosol measured over the northeast Atlantic Ocean , 1993 .