Comparison of six approaches to predicting droplet activation of surface active aerosol – Part 2: Strong surfactants

Abstract

Surfactants have been a focus of investigation in atmospheric sciences for decades due to their ability to modify the water uptake and cloud formation potential of aerosols. Surfactants adsorb at the surface and can decrease the surface tension of aqueous solutions. In microscopic aqueous droplets with finite amounts of solute, surface adsorption may simultaneously deplete the droplet bulk of the surfactant. While this mechanism is now broadly accepted, the representation in atmospheric and cloud droplet models is still not well constrained. We compare the predictions of five bulk–surface partitioning models documented in the literature to represent aerosol surface activity in Köhler calculations of cloud droplet activation. The models are applied to common aerosol systems, consisting of strong atmospheric surfactants (sodium myristate or myristic acid) and sodium chloride in a wide range of relative mixing ratios. For the same particles, the partitioning models predict similar critical droplet properties at small surfactant mass fractions, but differences between the model predictions increase significantly with the surfactant mass fraction in the particles. Furthermore, significantly different surface tensions are predicted for growing droplets at given ambient conditions along the Köhler curves. The inter-model variation for these strong surfactant particles is different than previously observed for moderately surface active atmospheric aerosol components. Our results highlight the importance of establishing bulk–surface partitioning effects in Köhler calculations for a wide range of conditions and aerosol types relevant to the atmosphere. In particular, conclusions made for a single type of surface active aerosol and surface activity model may not be immediately generalized.