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@ARTICLE{Tian:155387,
author = {Tian, J. and Riemer, N. and West, M. and Pfaffenberger, L.
and Schlager, H. and Petzold, A.},
title = {{M}odeling the evolution of aerosol particles in a ship
plume using {P}art{MC}-{MOSAIC}},
journal = {Atmospheric chemistry and physics},
volume = {14},
number = {11},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2014-04556},
pages = {5327 - 5347},
year = {2014},
abstract = {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 S 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 S
= $0.3\%$ 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 S = $1\%.$ For S 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 S = $0.6\%.$ 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 $0.3\%.$},
cin = {IEK-8},
ddc = {550},
cid = {I:(DE-Juel1)IEK-8-20101013},
pnm = {233 - Trace gas and aerosol processes in the troposphere
(POF2-233)},
pid = {G:(DE-HGF)POF2-233},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000337803100005},
doi = {10.5194/acp-14-5327-2014},
url = {https://juser.fz-juelich.de/record/155387},
}