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Abstract. Organic matter represents an important fraction of the fine particle aerosol, yet our knowledge of the roles of organics in the activation of aerosol particles into cloud droplets is poor. A cloud condensation nucleus (CCN) counter is used to examine the relative growth rates of cloud droplets for case studies from field measurements on the North Pacific Ocean and in a coniferous forest. A model of the condensational growth of water droplets, on particles dissolving according to their solubility in water, is used to simulate the initial scattering of the droplets as they grow in the CCN counter. Simulations of the growth rates of fine particles sampled in the marine boundary layer of the North Pacific Ocean shows no evidence of natural marine organic material contributing to the CCN water uptake but there is an indication of an influence from organics from diesel ship emissions on the size distribution of sulphate and the ability of these particles to act as CCN. Simulations of the observations of water uptake on biogenic organic aerosol particles sampled in a coniferous forest indicate an impact of the organic on the water uptake rates, but one that is still smaller than that of pure sulphate. The existence of organics becomes important in determining the water uptake as the organic mass increases relative to sulphate. The values of the organic component of the hygroscopicity parameter κ that describes the CCN activity were found to be negligible for the marine particles and 0.02-0.05 for the forest particles.

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[1] Because of its complex nature, attempts have been made to parameterize the process of cloud droplet formation and growth. The parameterization developed by Abdul-Razzak et al. [1998] and Abdul-Razzak and Ghan [2000], henceforth referred to as the ARG parameterization, is based on the adiabatic ascent of an air parcel, assuming that each particle is in equilibrium with its environment. Some of the limitations of the equilibrium assumption are evaluated here through direct comparison of a kinetic parcel model with the ARG parameterization. Conditions are described in which the supersaturation and the cloud droplet number concentration are underpredicted by the parameterization. The underprediction happens because of an overestimation of the condensation rate of water onto the larger particles. The effect is significant for conditions of lower updraft velocities (V < 50 cm s À1 ) and higher aerosol number concentrations (N a > 500 cm À3). The parameterization behaves well for higher updraft velocities and lower aerosol number concentrations. The impact of this effect on the activation of sulfate aerosols in the presence of sea salt aerosol is also investigated. Using the ARG parameterization to diagnose N d in the presence of sea salt aerosol leads to a greater reduction in the number of activated sulfate particles in lower updraft conditions than does using the kinetic parcel model. The relative contribution of sulfate particles to total N d is also significantly lower for the ARG parameterization than it is for the parcel model in low to moderate updrafts. The error in the first indirect radiative forcing introduced by the equilibrium assumption is estimated to be 6 to 15 W m À2 for typical marine clouds, depending on the updraft velocity.

Abstract. Organic matter represents an important fraction of the fine particle aerosol, yet our knowledge of the roles of organics in the activation of aerosol particles into cloud droplets is poor. A cloud condensation nucleus (CCN) counter is used to examine the relative growth rates of cloud droplets for case studies from field measurements on the North Pacific Ocean and in a coniferous forest. A model of the condensational growth of water droplets, on particles dissolving according to their solubility in water, is used to simulate the initial scattering of the droplets as they grow in the CCN counter. Simulations of the growth rates of fine particles sampled in the marine boundary layer of the North Pacific Ocean indicate that the main influence of the marine organic material on the water uptake rate is from its effect on the size distribution of the sulphate. Simulations of the observations of water uptake on biogenic organic aerosol particles sampled in a coniferous forest indicate an impact of the organic on the water uptake rates, but one that is still smaller than that of pure sulphate. The solubility of the organic becomes an important factor in determining the water uptake as the organic mass increases relative to sulphate. The values of the organic component of the hygroscopicity parameter κ that describes the CCN activity were found to be negligible for the marine particles and 0.02–0.05 for the forest particles.