Beschreibung:
Abstract. Twelve months of measurements collected during the Two-ColumnAerosol Project field campaign at Cape Cod, Massachusetts, which started inthe summer of 2012, were used to investigate aerosol physical, optical, andchemical properties and their influences on the dependence of clouddevelopment on thermodynamic (i.e., lower tropospheric stability, LTS)conditions. Relationships between aerosol loading and cloud properties underdifferent dominant air-mass conditions and the magnitude of the firstindirect effect (FIE), as well as the sensitivity of the FIE to differentaerosol compositions, are examined. The seasonal variation in aerosol numberconcentration (Na) was not consistent with variations in aerosoloptical properties (i.e., scattering coefficient, σs, andcolumnar aerosol optical depth). Organics were found to have a largecontribution to small particle sizes. This contribution decreased during theparticle growth period. Under low-aerosol-loading conditions, the liquidwater path (LWP) and droplet effective radius (DER) significantly increasedwith increasing LTS, but, under high-aerosol-loading conditions, LWP and DERchanged little, indicating that aerosols significantly weakened thedependence of cloud development on LTS. The reduction in LWP and DER fromlow- to high-aerosol-loading conditions was greater in stable environments,suggesting that clouds under stable conditions are more susceptible toaerosol perturbations than those under more unstable conditions. Highaerosol loading weakened the increase in DER as LWP increased andstrengthened the increase in cloud optical depth (COD) with increasing LWP,resulting in changes in the interdependence of cloud properties. Under bothcontinental and marine air-mass conditions, high aerosol loading cansignificantly increase COD and decrease LWP and DER, narrowing theirdistributions. Magnitudes of the FIE estimated under continental air-massconditions ranged from 0.07±0.03 to 0.26±0.09 with a meanvalue of 0.16±0.03 and showed an increasing trend as LWP increased.The calculated FIE values for aerosols with a low fraction of organics aregreater than those for aerosols with a high fraction of organics. Thisimplies that clouds over regions dominated by aerosol particles containingmostly inorganics are more susceptible to aerosol perturbations, resultingin larger climate forcing, than clouds over regions dominated by organicaerosol particles.