Modeling the Interactions between Aerosols and Liquid Water Clouds with a Self-Consistent Cloud Scheme in a General Circulation Model

Abstract To model aerosol–cloud interactions in general circulation models (GCMs), a prognostic cloud scheme of cloud liquid water and amount is expanded to include droplet number concentration (Nd) in a way that allows them to be calculated using the same large-scale and convective updraft velocity field. In the scheme, the evolution of droplets fully interacts with the model meteorology. An explicit treatment of cloud condensation nuclei (CCN) activation enables the scheme to take into account the contributions to Nd of multiple aerosol species (i.e., sulfate, organic, and sea-salt aerosols) and to consider kinetic limitations of the activation process. An implementation of the prognostic scheme in the Geophysical Fluid Dynamics Laboratory (GFDL) AM2 GCM yields a vertical distribution of Nd with a characteristic maximum in the lower troposphere; this feature differs from the profile that would be obtained if Nd is diagnosed from the sulfate mass concentration based on an often-used empirical relationship. Prognosticated Nd exhibits large variations with respect to the sulfate mass concentration. The mean values are generally consistent with the empirical relationship over ocean, but show negative biases over the Northern Hemisphere midlatitude land, perhaps owing to the neglect of subgrid variations of large-scale ascents and inadequate convective sources. The prognostic scheme leads to a substantial improvement in the agreement of model-predicted present-day liquid water path (LWP) and cloud forcing with satellite measurements compared to using the empirical relationship. The simulations with preindustrial and present-day aerosols show that the combined first and second indirect effects of anthropogenic sulfate and organic aerosols give rise to a steady-state global annual mean flux change of −1.8 W m−2, consisting of −2.0 W m−2 in shortwave and 0.2 W m−2 in longwave. The ratios of the flux changes in the Northern Hemisphere (NH) to that in Southern Hemisphere (SH) and of the flux changes over ocean to that over land are 2.9 and 0.73, respectively. These estimates are consistent with the averages of values from previous studies stated in a recent review. The model response to higher Nd alters the cloud field; LWP and total cloud amount increase by 19% and 0.6%, respectively. Largely owing to high sulfate concentrations from fossil fuel burning, the NH midlatitude land and oceans experience strong radiative cooling. So does the tropical land, which is dominated by biomass burning–derived organic aerosol. The computed annual, zonal-mean flux changes are determined to be statistically significant, exceeding the model’s natural variations in the NH low and midlatitudes and in the SH low latitudes. This study reaffirms the major role of sulfate in providing CCN for cloud formation.