Anthropogenic contribution to cloud condensation nuclei and the first aerosol indirect climate effect

Atmospheric particles influence the climate indirectly by acting as cloud condensation nuclei (CCN). The first aerosol indirect radiative forcing (FAIRF) constitutes the largest uncertainty among the radiative forcings quantified by the latest IPCC report (IPCC2007) and is a major source of uncertainty in predicting climate change. Here, we investigate the anthropogenic contribution to CCN and associated FAIRF using a state-of-the-art global chemical transport and aerosol model (GEOS-Chem/APM) that contains a number of advanced features (including sectional particle microphysics, online comprehensive chemistry, consideration of all major aerosol species, online aerosol-cloud-radiation calculation, and usage of more accurate assimilated meteorology). The model captures the absolute values and spatial distributions of CCN concentrations measured in situ around the globe. We show that anthropogenic emissions increase the global mean CCN in the lower troposphere by similar to 60-80% and cloud droplet number concentration by similar to 40%. The global mean FAIRF based on GEOS-Chem/APM is -0.75 W m(-2), close to the median values of both IPCC2007 and post-IPCC2007 studies. To the best of our knowledge, this is the first time that a global sectional aerosol model with full online chemistry and considering all major aerosol species (including nitrate, ammonium, and second organic aerosols) has been used used to calculate FAIRF.