Poster's note : obliquely relevant to a range of SRM topics. Paper link
below.

http://m.phys.org/news/2015-05-years-results-secondary-aerosols-uncertainty.html

Years of results regarding secondary organic aerosols reduce uncertainty in
climate projections

May 12, 2015

Contrary to long-standing assumptions, our laboratory and field data show
that SOA particles are highly viscous semi-solids, trap volatile organic
molecules during formation, evaporate orders of magnitude slower than
assumed, and, therefore, are not at equilibrium with the gas phase.For the
past 20 years, a large portion of the particles measured in the atmosphere
were missing from models. At best, models were able to explain one-tenth of
the carbon-rich secondary organic aerosols, or SOA, measured in the air.
The problem turned out to be a series of fundamental assumptions used in
the models due to a lack of experimental data. The models assumed the
particles were liquids that responded to changes in the surrounding
atmosphere by rapid condensation or evaporation and in-particle mixing. The
models predicted the particles, especially the small ones, were rather
short-lived on their journey away from their sources. All of these
assumptions and more were proven false by Dr. Alla Zelenyuk and her
colleagues at Pacific Northwest National Laboratory, Imre Consulting,
University of Washington, and University of California at Irvine.

These particles generated by natural and anthropogenic sources are of
interest because of their effect on air quality and health, and their
impact on climate by scattering and absorbing solar radiation and
influencing the formation and properties of clouds.

Seeking to find the reason that most of the particles found in the
atmosphere are missing from the models, Zelenyuk and her colleagues began
by designing novel approaches to investigate what these particles really
look like and how they evolve in atmosphere. They built SPLAT II, a second
generation single particle mass spectrometer. Highly precise and sensitive,
this instrument allows users to study basic processes and properties of
nanoparticles. Usually located in DOE's EMSL, a national scientific user
facility, the instrument also travels to field sites, working on the ground
and aboard research aircraft. SPLAT II has been flown to many sites in the
United States, South Korea, and Germany.

Using SPLAT II, the researchers measured the shape, size, density,
composition, evaporation rates, and many other relevant properties of
SOA-containing particles in laboratory and field. The results show that SOA
particles are far from the perfect liquid spheres assumed in models. The
actual SOA particles are highly viscous semi-solids that have complex
compositions and multifaceted structures.

The team was the first to directly measure chemical diffusivity of tracer
molecules in SOA particles, determining that these particles are tar-like,
and millions of times more viscous than assumed. This viscous nature allows
the particles to trap toxic polycyclic aromatic hydrocarbons, PAHs, and
other chemicals that would otherwise quickly evaporate. Zelenyuk and her
colleagues discovered a symbiotic relationship between the PAHs and the SOA
particles. The PAHs hitchhike along and, in the process, help the SOA
survive longer. This hitchhiking phenomenon explains how anthropogenic
pollutants from California freeways and biomass burning in Asia can be
transported far away from their sources to the pristine environments, such
as the Arctic.When airborne particles (green) form before pollutants known
as PAHs (yellow) glob on, the particles evaporate quickly (top row). But
when the particles form in the presence of PAHs, which is what likely
happens in nature, the long-lasting particles can take the pollutants for a
long-distance ride (bottom).SOA particles, even without PAHs, are long
lasting. Some scientists believed the particles evaporated nearly
instantaneously at higher levels of humidity. Zelenyuk and her team found,
however, that the particles evaporate orders of magnitude slower under all
atmospherically relevant conditions.Now, Zelenyuk and her team are working
with atmospheric modelers to add this information, independently verified,
into models. The team created a new, measurement-based paradigm of SOA that
now underlies three-dimensional regional and global climate models to
properly represent SOA properties. These models yield significantly higher
loadings and longer atmospheric lifetimes, thus reconciling the
long-standing discrepancy between observations and model predictions.More
information: "Experimental determination of chemical diffusion within
secondary organic aerosol particles."

Physical Chemistry Chemical Physics 15 (8), 2983-2991 (2013). DOI:
10.1039/C2CP44013J

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