Atmospheric Chemistry and Physics
www.atmos-chem-phys.net
1680-7316
1680-7324
9
6
2009
10.5194/acp-9-1907-2009
http://www.atmos-chem-phys.net/9/1907/2009/
http://www.atmos-chem-phys.net/9/1907/2009/acp-9-1907-2009.html
http://www.atmos-chem-phys.net/9/1907/2009/acp-9-1907-2009.pdf
1907
1928
2009-03-19
Secondary Organic Aerosol Formation from Acetylene (C<sub>2</sub>H<sub>2</sub>): seed effect on SOA yields due to organic photochemistry in the aerosol aqueous phase
R. Volkamer
rainer.volkamer@colorado.edu
P. J. Ziemann
M. J. Molina
Dept. of Chemistry and Biochemistry and CIRES, University of Colorado at Boulder, CO, USA
Dept. of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA, USA
Air Pollution Research Center, University of California, Riverside, Riverside, CA, USA
The lightest Non Methane HydroCarbon (NMHC), i.e., acetylene
(C<sub>2</sub>H<sub>2</sub>) is found to form secondary organic aerosol (SOA). Contrary
to current belief, the number of carbon atoms, <i>n</i>, for a NMHC to act as SOA
precursor is lowered to <i>n</i>=2 here. The OH-radical initiated oxidation of
C<sub>2</sub>H<sub>2</sub> forms glyoxal (CHOCHO) as the highest yield product, and
>99% of the SOA from C<sub>2</sub>H<sub>2</sub> is attributed to CHOCHO. SOA
formation from C<sub>2</sub>H<sub>2</sub> and CHOCHO was studied in a photochemical and
a dark simulation chamber. Further, the experimental conditions were varied
with respect to the chemical composition of the seed aerosols, mild
acidification with sulphuric acid (SA, 3<pH<4), and relative humidity
(10<RH<90%). The rate of SOA formation is found enhanced by several
orders of magnitude in the photochemical system. The SOA yields (<i>Y</i><sub>SOA</sub>)
ranged from 1% to 24% and did not correlate with the organic mass
portion of the seed, but increased linearly with liquid water content (LWC)
of the seed. For fixed LWC, <i>Y</i><sub>SOA</sub> varied by more than a factor of five.
Water soluble organic carbon (WSOC) photochemistry in the liquid water
associated with internally mixed inorganic/WSOC seed aerosols is found
responsible for this seed effect. WSOC photochemistry enhances the SOA
source from CHOCHO, while seeds containing amino acids (AA) and/or SA showed
among the lowest of all <i>Y</i><sub>SOA</sub> values, and largely suppress the
photochemical enhancement on the rate of CHOCHO uptake. Our results give
first evidence for the importance of heterogeneous photochemistry of CHOCHO
in SOA formation, and identify a potential bias in the currently available
<i>Y</i><sub>SOA</sub> data for other SOA precursor NMHCs. We demonstrate that SOA
formation via the aqueous phase is not limited to cloud droplets, but
proceeds also in the absence of clouds, i.e., does not stop once a cloud
droplet evaporates. Atmospheric models need to be expanded to include SOA
formation from WSOC photochemistry of CHOCHO, and possibly other α-dicarbonyls, in aqueous aerosols.
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