ACP Atmospheric Chemistry and Physics ACP Atmos. Chem. Phys. 1680-7324 Copernicus Publications Göttingen, Germany 10.5194/acp-14-5327-2014 Modeling the evolution of aerosol particles in a ship plume using PartMC-MOSAIC Tian J. 1 Riemer N. https://orcid.org/0000-0002-3220-3457 1 West M. 2 Pfaffenberger L. 3 Schlager H. 4 Petzold A. https://orcid.org/0000-0002-2504-1680 5 Department of Atmospheric Sciences, University of Illinois at Urbana-Champaign, Urbana, Illinois, USA Department of Mechanical Science and Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois, USA Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland Dt. Zentrum für Luft- und Raumfahrt, Inst. für Physik der Atmosphäre, Oberpfaffenhofen, 82234 Wessling, Germany Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research, IEK-8-Troposphere, Jülich, Germany 03 06 2014 14 11 5327 5347 Copyright: © 2014 J. Tian et al. 2014 This work is licensed under the Creative Commons Attribution 3.0 Unported License. To view a copy of this licence, visit https://creativecommons.org/licenses/by/3.0/ This article is available from https://acp.copernicus.org/articles/14/5327/2014/acp-14-5327-2014.html The full text article is available as a PDF file from https://acp.copernicus.org/articles/14/5327/2014/acp-14-5327-2014.pdf

This study investigates the evolution of ship-emitted aerosol particles using the stochastic particle-resolved model PartMC-MOSAIC (Particle Monte Carlo model-Model for Simulating Aerosol Interactions and Chemistry). Comparisons of our results with observations from the QUANTIFY (Quantifying the Climate Impact of Global and European Transport Systems) 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 <i>S</i> at which CCN activity was evaluated. For the base case conditions, characterized by a low formation rate of secondary aerosol species, neglecting coagulation, but simulating condensation, led to an underestimation of CCN concentrations of about 37% for <i>S</i> = 0.3% at the end of the 14-h simulation. In contrast, for supersaturations higher than 0.7%, neglecting coagulation resulted in an overestimation of CCN concentration, about 75% for <i>S</i> = 1%. For <i>S</i> lower than 0.2% the differences between simulations including coagulation and neglecting coagulation were negligible. Neglecting condensation, but simulating coagulation did not impact the CCN concentrations below 0.2% and resulted in an underestimation of CCN concentrations for larger supersaturations, e.g., 18% for <i>S</i> = 0.6%. We also explored the role of nucleation for the CCN concentrations in the ship plume. For the base case the impact of nucleation on CCN concentrations was limited, but for a sensitivity case with higher formation rates of secondary aerosol over several hours, the CCN concentrations increased by an order of magnitude for supersaturation thresholds above 0.3%.

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