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@ARTICLE{Collins:188301,
author = {Collins, D. B. and Zhao, Defeng and Ruppel, M. J. and
Laskina, O. and Grandquist, J. R. and Modini, R. L. and
Stokes, M. D. and Russell, L. M. and Bertram, T. H. and
Grassian, V. H. and Deane, G. B. and Prather, K. A.},
title = {{D}irect aerosol chemical composition measurements to
evaluate the physicochemical differences between controlled
sea spray aerosol generation schemes},
journal = {Atmospheric measurement techniques},
volume = {7},
number = {11},
issn = {1867-8548},
address = {Katlenburg-Lindau},
publisher = {Copernicus},
reportid = {FZJ-2015-01721},
pages = {3667 - 3683},
year = {2014},
abstract = {Controlled laboratory studies of the physical and chemical
properties of sea spray aerosol (SSA) must be under-pinned
by a physically and chemically accurate representation of
the bubble-mediated production of nascent SSA particles.
Bubble bursting is sensitive to the physico-chemical
properties of seawater. For a sample of seawater, any
important differences in the SSA production mechanism are
projected into the composition of the aerosol particles
produced. Using direct chemical measurements of SSA at the
single-particle level, this study presents an
intercomparison of three laboratory-based, bubble-mediated
SSA production schemes: gas forced through submerged
sintered glass filters ("frits"), a pulsed
plunging-waterfall apparatus, and breaking waves in a wave
channel filled with natural seawater. The size-resolved
chemical composition of SSA particles produced by breaking
waves is more similar to particles produced by the plunging
waterfall than those produced by sintered glass filters.
Aerosol generated by disintegrating foam produced by
sintered glass filters contained a larger fraction of
organic-enriched particles and a different size-resolved
elemental composition, especially in the 0.8–2 μm dry
diameter range. Interestingly, chemical differences between
the methods only emerged when the particles were chemically
analyzed at the single-particle level as a function of size;
averaging the elemental composition of all particles across
all sizes masked the differences between the SSA samples.
When dried, SSA generated by the sintered glass filters had
the highest fraction of particles with spherical morphology
compared to the more cubic structure expected for pure NaCl
particles produced when the particle contains relatively
little organic carbon. In addition to an intercomparison of
three SSA production methods, the role of the episodic or
"pulsed" nature of the waterfall method on SSA composition
was under-taken. In organic-enriched seawater, the
continuous operation of the plunging waterfall resulted in
the accumulation of surface foam and an over-expression of
organic matter in SSA particles compared to those produced
by a pulsed plunging waterfall. Throughout this set of
experiments, comparative differences in the SSA number size
distribution were coincident with differences in aerosol
particle composition, indicating that the production
mechanism of SSA exerts important controls on both the
physical and chemical properties of the resulting aerosol
with respect to both the internal and external mixing state
of particles. This study provides insight into the
inextricable physicochemical differences between each of the
bubble-mediated SSA generation mechanisms tested and the
aerosol particles that they produce, and also serves as a
guideline for future laboratory studies of SSA particles.},
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:000345781000004},
doi = {10.5194/amt-7-3667-2014},
url = {https://juser.fz-juelich.de/record/188301},
}