1Department of Atmospheric Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois, USA
2Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
3Dt. Zentrum für Luft- und Raumfahrt, Inst. für Physik der Atmosphäre, Oberpfaffenhofen, 82234 Wessling, Germany
4Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research, Jülich, Germany
Abstract. This study investigates the evolution of ship-emitted aerosol particles using the stochastic particle-resolved model PartMC-MOSAIC. Comparisons of our results with observations from the QUANTIFY Study in 2007 in the English channel and the Gulf of Biscay showed that the model was able to reproduce the observed evolution of total number concentration and the vanishing of the nucleation mode consisting of sulfate particles. Further process analysis revealed that during the first hour after emission, dilution reduced the total number concentration by four orders of magnitude, while coagulation reduced it by an additional order of magnitude. Neglecting coagulation resulted in an overprediction of more than one order of magnitude in the number concentration of particles smaller than 40 nm at a plume age of 100 s. Coagulation also significantly altered the mixing state of the particles, leading to a continuum of internal mixtures of sulfate and black carbon. The impact on cloud condensation nuclei (CCN) concentrations depended on the supersaturation threshold S at which CCN activity was evaluated. For the base case conditions simulated here, characterized by a low formation rate of secondary aerosol species, neglecting coagulation led to an underestimation of CCN concentrations of about 20% for S=0.6% and of about 40% for S=0.3%. For S=0.1% the differences between simulations including coagulation and neglecting coagulation were negligible.