Atmospheric Chemistry and Physics Discussions
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10.5194/acpd-8-16789-2008
http://www.atmos-chem-phys-discuss.net/8/16789/2008/
http://www.atmos-chem-phys-discuss.net/8/16789/2008/acpd-8-16789-2008.html
http://www.atmos-chem-phys-discuss.net/8/16789/2008/acpd-8-16789-2008.pdf
16789
16817
2008-09-04
Aerosol hygroscopicity in the marine atmosphere: a closure study using high-resolution, size-resolved AMS and multiple-RH DASH-SP data
S. P. Hersey
A. Sorooshian
S. M. Murphy
R. C. Flagan
J. H. Seinfeld
seinfeld@caltech.edu
Departments of Chemical Engineering and Environmental Science and Engineering, Caltech, 1200 E. California Blvd, Pasadena, CA, 91125, USA
We have conducted the first closure study to couple high-resolution aerosol
mass spectrometer (AMS) composition data with size-resolved, multiple-RH,
high-time-resolution hygroscopic growth factor (<i>GF</i>) measurements from the
differential aerosol sizing and hygroscopicity spectrometer probe (DASH-SP).
These data were collected off the coast of Central California during seven of
the 16 flights carried out during the MASE-II field campaign in July 2007.
Two of the seven flights were conducted in airmasses that originated over the
continental United States. These flights exhibited elevated organic volume
fractions (<i>VF</i><sub>organic</sub>=0.46±0.22, as opposed to
0.24±0.18 for all other flights), corresponding to significantly
suppressed <i>GFs</i> at high RH (1.61±0.14 at 92% RH, as compared with
1.91±0.07 for all other flights), more moderate <i>GF</i> suppression at
intermediate RH (1.53±0.10 at 85%, compared with 1.58±0.08 for
all other flights, and no measurable <i>GF</i> suppression at low RH
(1.31±0.06 at 74%, compared with 1.31±0.07 for all other
flights). Organic loadings were slightly elevated in above-cloud aerosols, as
compared with below-cloud aerosols, and corresponded to a similar trend of
significantly suppressed <i>GF</i> at high RH, but more moderate impacts at lower
values of RH. A hygroscopic closure based on a volume-weighted mixing rule
provided excellent agreement with DASH-SP measurements (<i>R</i><sup>2</sup>=0.79).
Minimization of root mean square error between observations and predictions
indicated mission-averaged organic <i>GFs</i> of 1.20, 1.43, and 1.46 at 74, 85,
and 92% RH, respectively. These values agree with previously reported values
for water-soluble organics such as dicarboxylic and multifunctional acids,
and correspond to a highly oxidized, presumably water-soluble, organic
fraction (O:C=0.92±0.33). Finally, a backward stepwise linear
regression revealed that, other than RH, the most important predictor for
<i>GF</i> is <i>VF</i><sub>organic</sub>, indicating that a simple emperical model relating
<i>GF</i>, RH, and the relative abundance of organic material can provide accurate
predictions of hygroscopic growth in the marine atmosphere.
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