An evaluation and comparison of cloud condensation nucleus activity models: Predicting particle critical saturation from growth at subsaturation

Abstract

The ability of particles to activate and form cloud droplets influences the functioning of the Earth's hydrological cycle. This work links the particle water uptake at subsaturation to the critical supersaturation ratio needed for particles to become cloud condensation nuclei (CCN). Five models using the particle hygroscopic growth at subsaturation for predicting the critical supersaturation needed for droplet activation were applied to a laboratory data set of inorganic and organic compounds and mixtures of them. The data set consisted of hygroscopicity tandem differential mobility analyzer measurements and CCN counter measurements. No chemical composition information was used when applying the models. All models tested were based on modifications of Köhler theory and gave similar results. The agreement between predicted and measured critical supersaturations was good, considering the relatively simple models used. A trend of overestimating the critical supersaturations was observed, typically by ∼15%. The best performing model gave on average only a 4% offset from experimental values; the model with the largest deviation was offset by 20%. A comparison was made between the number of soluble entities (ions or nondissociating molecules) estimated from the particle hygroscopic growth at 90% relative humidity (RH) and the number estimated from the particle critical supersaturation; a ∼35% increase was observed in the effective number of entities in solution when going from 90% RH to activation. For many types of aerosols, differences in the model approaches tested do not induce large differences in the predicted critical supersaturation. However, it is most important to follow the recommendations published with the respective models and not use them indiscriminately.