General Circulation Model Calculations of the Direct Radiative Forcing by Anthropogenic Sulfate and Fossil-Fuel Soot Aerosol

Abstract

A new radiation code within a general circulation model is used to assess the direct solar and thermal radiative forcing by sulfate aerosol of anthropogenic origin and soot aerosol from fossil-fuel burning. The radiative effects of different aerosol profiles, relative humidity parameterizations, chemical compositions, and internal and external mixtures of the two aerosol types are investigated. The contribution to the radiative forcing from cloudy sky regions is found to be negligible for sulfate aerosol; this is in contrast to recent studies where the cloudy sky contribution was estimated using a method in which the spatial correlation between cloud amount and sulfate burden was ignored. However, the radiative forcing due to fossil-fuel soot aerosol is enhanced in cloudy regions if soot aerosol exists within or above the cloud. The global solar radiative forcing due to sulfate aerosol is estimated to be ?0.38 W m?2 and the global thermal radiative forcing is estimated to be +0.01 W m?2. The hemispheric mean radiative forcings vary by only about 10% for reasonable assumptions about the chemical form of the sulfate aerosol and the relative humidity dependence; the uncertainties in the aerosol loading are far more significant. If a soot/sulfate mass ratio of 0.075 is assumed, then the global solar radiative forcing weakens to ?0.18 W m?2 for an external mixture and weakens further for an internal mixture. Additionally, the spatial distribution of the radiative forcing shows strong negative/positive forcing contrasts that may influence the dynamical response of the atmosphere. Although these results are extremely sensitive to the adopted soot/sulfate ratio and the assumed vertical profile, they indicate that fossil-fuel soot aerosol may exert a nonnegligible radiative forcing and emphasize the need to consider each anthropogenic aerosol species.