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Organic Enrichment, Physical Phase State, and Surface Tension Depression of Nascent Core–Shell Sea Spray Aerosols during Two Phytoplankton Blooms
journal contribution
posted on 2020-03-13, 21:43 authored by Hansol
D. Lee, Holly S. Morris, Olga Laskina, Camille M. Sultana, Christopher Lee, Thilina Jayarathne, Joshua L. Cox, Xiaofei Wang, Elias S. Hasenecz, Paul J. DeMott, Timothy H. Bertram, Christopher D. Cappa, Elizabeth A. Stone, Kimberly A. Prather, Vicki H. Grassian, Alexei V. TivanskiSea spray aerosols (SSAs) affect
the Earth’s climate directly
by scattering solar radiation and indirectly by acting as ice and
cloud condensation nuclei. The relative magnitude of these effects
remains uncertain, in part, from substantial compositional and morphological
variability between individual particles. Here, the evolving heterogeneity
within populations of primary SSAs produced from wave breaking of
natural seawater within a wave flume is investigated. Over the course
of the study, two successive phytoplankton blooms were induced in
the seawater. The morphology, organic volume fraction, hygroscopicity,
phase state, and surface tension of individual SSAs collected via
deposition on a substrate were characterized using atomic force microscopy.
Particles between ca. 0.3 and 1 μm in volume equivalent diameter
displayed a distinctive morphology revealing an inorganic core coated
with an organic shell. The inferred organic volume fraction was the
largest at the peak of the first bloom. The corresponding shell thicknesses
ranged from 21 to 40 nm at 20% relative humidity (RH). The organic
shell phase state of the majority of the particles during both blooms
was semisolid at 20% and 60% RH. At 20% RH, a minor fraction of the
organic shells behaved as a solid, while at 60% RH some behaved as
liquids during the first bloom. Similar results were evident at 20%
RH for the second bloom but with no observed liquid particles at 60%
RH. The thick, semisolid organic coatings could potentially reduce
atmospheric water and gas uptake efficiencies onto SSAs at lower RH,
along with the potential for ice nucleating activity. However, at
80% RH, the SSAs deliquesced and exhibited liquid-like behavior with
surface tension values measured over individual particles of 41–87
mN m–1, demonstrating high particle-to-particle
variability. The suppressed surface tension at 80% RH relative to
pure water is attributed to the high concentrations of surface-active
organic compounds, potentially further limiting the diffusion rate
of gas molecules through the interface.