Sensitivity of direct climate forcing by atmospheric aerosols to aerosol size and composition

Abstract

We evaluate, using a box model, the sensitivity of direct climate forcing by atmospheric aerosols for a “global mean” aerosol that consists of fine and coarse modes to aerosol composition, aerosol size distribution, relative humidity (RH), aerosol mixing state (internal versus external mixture), deliquescence/crystallization hysteresis, and solar zenith angle. We also examine the dependence of aerosol upscatter fraction on aerosol size, solar zenith angle, and wavelength and the dependence of single scatter albedo on wavelength and aerosol composition. The single most important parameter in determining direct aerosol forcing is relative humidity, and the most important process is the increase of the aerosol mass as a result of water uptake. An increase of the relative humidity from 40 to 80% is estimated for the global mean aerosol considered to result in an increase of the radiative forcing by a factor of 2.1. Forcing is relatively insensitive to the fine mode diameter increase due to hygroscopic growth, as long as this mode remains inside the efficient scattering size region. The hysteresis/deliquescence region introduces additional uncertainty but, in general, errors less than 20% result by the use of the average of the two curves to predict forcing. For fine aerosol mode mean diameters in the 0.2–0.5 μm range direct aerosol forcing is relatively insensitive (errors less than 20%) to variations of the mean diameter. Estimation of the coarse mode diameter within a factor of 2 is generally sufficient for the estimation of the total aerosol radiative forcing within 20%. Moreover, the coarse mode, which represents the nonanthropogenic fraction of the aerosol, is estimated to contribute less than 10% of the total radiative forcing for all RHs of interest. Aerosol chemical composition is important to direct radiative forcing as it determines (1) water uptake with RH, and (2) optical properties. The effect of absorption by aerosol components on forcing is found to be significant even for single scatter albedo values of ω=0.93–0.97. The absorbing aerosol component reduces the aerosol forcing from that in its absence by roughly 30% at 60% RH and 20% at 90% RH. The mixing state of the aerosol (internal versus external) for the particular aerosol considered here is found to be of secondary importance. While sulfate mass scattering efficiency (m² (g SO₄²⁻)⁻¹) and the normalized sulfate forcing (W (g SO₄²⁻)⁻¹) increase strongly with RH, total mass scattering efficiency (m² g⁻¹) and normalized forcing (W g⁻¹) are relatively insensitive to RH, wherein the mass of all species, including water, are accounted for. Following S. Nemesure et al. (Direct shortwave forcing of climate by anthropogenic sulfate aerosol: sensitivity to particle size, composition, and relative humidity, submitted to Journal of Geophysical Research, 1995), we find that aerosol feeing achieves a maximum at a particular solar zenith angle, reflecting a balance between increasing upscatter fraction with increasing solar zenith angle and decreasing solar flux (from Rayleigh scattering) with increasing solar zenith angle.