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This study investigates the evolution of ship-emitted aerosolparticles using the stochastic particle-resolved modelPartMC-MOSAIC (Particle Monte Carlo model-Model for Simulating Aerosol Interactions and Chemistry). Comparisons of our results with observations from theQUANTIFY (Quantifying the Climate Impact of Globaland European Transport Systems) study in 2007 in the English Channel and the Gulf of Biscayshowed that the model was able to reproduce the observed evolutionof total number concentration and the vanishing of the nucleationmode consisting of sulfate particles. Further process analysisrevealed that during the first hour after emission, dilution reducedthe total number concentration by four orders of magnitude, whilecoagulation reduced it by an additional order ofmagnitude. Neglecting coagulation resulted in an overprediction ofmore than one order of magnitude in the number concentration ofparticles smaller than 40 nm at a plume age of 100 s. Coagulationalso significantly altered the mixing state of the particles,leading to a continuum of internal mixtures of sulfate and blackcarbon. The impact on cloud condensation nuclei (CCN) concentrationsdepended on the supersaturation threshold S at which CCN activitywas evaluated. For the base case conditions, characterizedby a low formation rate of secondary aerosol species, neglectingcoagulation, but simulating condensation, led to anunderestimation of CCN concentrations of about 37% for S = 0.3%at the end of the 14-h simulation. In contrast, forsupersaturations higher than 0.7%, neglecting coagulationresulted in an overestimation of CCN concentration, about 75% forS = 1%. For S lower than 0.2% the differences betweensimulations including coagulation and neglecting coagulation werenegligible. Neglecting condensation, but simulating coagulationdid not impact the CCN concentrations below 0.2% and resulted inan underestimation of CCN concentrations for largersupersaturations, e.g., 18% for S = 0.6%. We also explored therole of nucleation for the CCN concentrations in the shipplume. For the base case the impact of nucleation on CCNconcentrations was limited, but for a sensitivity case with higherformation rates of secondary aerosol over several hours, the CCNconcentrations increased by an order of magnitude forsupersaturation thresholds above 0.3%

Modeling the evolution of aerosol particles in a ship plume using PartMC-MOSAIC