Importance of aerosol composition and mixing state for cloud droplet activation over the Arctic pack ice in summer

Abstract. Concentrations of cloud condensation nuclei (CCN) were measured throughout an expedition by icebreaker around the central Arctic Ocean, including a 3 week ice drift operation at 87° N, from 3 August to 9 September 2008. In agreement with previous observations in the area and season, median daily CCN concentrations at 0.2% water vapour supersaturation (SS) were typically in the range of 15 to 30 cm⁻³, but concentrations varied by 2 to 3 orders of magnitude over the expedition and were occasionally below 1 cm⁻³. The CCN concentrations were highest near the ice edge and fell by a factor of 3 in the first 48 h of transport from the open sea into the pack ice region. For longer transport times they increased again, indicating a local source over the pack ice, suggested to be polymer gels, via drops injected into the air by bubbles bursting on open leads. We inferred the properties of the unexplained non-water soluble aerosol fraction that was necessary for reproducing the observed concentrations of CCN. This was made possible by assuming Köhler theory and simulating the cloud nucleation process using a Lagrangian adiabatic air parcel model that solves the kinetic formulation for condensation of water on size resolved aerosol particles. We propose that the portion of the internally/externally mixed water insoluble particles was larger in the corresponding smaller aerosol size ranges. These particles were physically and chemically behaving as polymer gels: the interaction of the hydrophilic and hydrophobic entities on the structures of polymer gels during cloud droplet activation would at first only show a partial wetting character and only weak hygroscopic growth. Given time, a high CCN activation efficiency is achieved, which is promoted by the hydrophilicity or surface-active properties of the gels. Thus the result in this study argues that the behaviour of the high Arctic aerosol in CCN-counters operating at water vapour SSs > 0.4% (high relative humidities) may not be properly explained by conventional Köhler theory.