Aerosol hygroscopicity in the marine atmosphere: A closure study using high-time-resolution, multiple-RH DASH-SP and size-resolved C-ToF-AMS data

S. P. Hersey, Armin Sorooshian, S. M. Murphy, R. C. Flagan, J. H. Seinfeld

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Abstract

We have conducted the first airborne hygroscopic growth closure study to utilize data from an Aerodyne compact Time-of-Flight Aerosol Mass Spectrometer (C-ToF-AMS) coupled with size-resolved, multiple-RH, high-time-resolution hygroscopic growth factor (GF) 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 characterized by continental origin. These flights exhibited elevated organic volume fractions (VForganic=0.56±0. 19, as opposed to 0.39±0.20 for all other flights), corresponding to significantly suppressed GFs at high RH (1.61±0.14 at 92% RH, as compared with 1.91±0.07 for all other flights), more moderate GF suppression at intermediate RH (1.53±0.10 at 85%, compared with 1.58±0.08 for all other flights), and no measurable GF 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 GF at high RH, but more moderate impacts at lower values of RH. A hygroscopic closure based on a volume-weighted mixing rule provided good agreement with DASH-SP measurements (R2=0.78). Minimization of root mean square error between observations and predictions indicated mission-averaged organic GFs of 1.22, 1.45, and 1.48 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 (mission-averaged O:C=0.92±0.33). Finally, a backward stepwise linear regression revealed that, other than RH, the most important predictor for GF is Vívanlo indicating that a simple emperical model relating GF, RH, and the relative abundance of organic material can provide accurate predictions (R2=0.77) of hygroscopic growth for the California coast.

Original languageEnglish (US)
Pages (from-to)2543-2554
Number of pages12
JournalAtmospheric Chemistry and Physics
Volume9
Issue number7
StatePublished - 2009
Externally publishedYes

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marine atmosphere
hygroscopicity
spectrometer
probe
aerosol
flight
volcanic cloud
sizing
coast
prediction
relative abundance
water
acid

ASJC Scopus subject areas

  • Atmospheric Science

Cite this

Aerosol hygroscopicity in the marine atmosphere : A closure study using high-time-resolution, multiple-RH DASH-SP and size-resolved C-ToF-AMS data. / Hersey, S. P.; Sorooshian, Armin; Murphy, S. M.; Flagan, R. C.; Seinfeld, J. H.

In: Atmospheric Chemistry and Physics, Vol. 9, No. 7, 2009, p. 2543-2554.

Research output: Contribution to journalArticle

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abstract = "We have conducted the first airborne hygroscopic growth closure study to utilize data from an Aerodyne compact Time-of-Flight Aerosol Mass Spectrometer (C-ToF-AMS) coupled with size-resolved, multiple-RH, high-time-resolution hygroscopic growth factor (GF) 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 characterized by continental origin. These flights exhibited elevated organic volume fractions (VForganic=0.56±0. 19, as opposed to 0.39±0.20 for all other flights), corresponding to significantly suppressed GFs at high RH (1.61±0.14 at 92{\%} RH, as compared with 1.91±0.07 for all other flights), more moderate GF suppression at intermediate RH (1.53±0.10 at 85{\%}, compared with 1.58±0.08 for all other flights), and no measurable GF 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 GF at high RH, but more moderate impacts at lower values of RH. A hygroscopic closure based on a volume-weighted mixing rule provided good agreement with DASH-SP measurements (R2=0.78). Minimization of root mean square error between observations and predictions indicated mission-averaged organic GFs of 1.22, 1.45, and 1.48 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 (mission-averaged O:C=0.92±0.33). Finally, a backward stepwise linear regression revealed that, other than RH, the most important predictor for GF is V{\'i}vanlo indicating that a simple emperical model relating GF, RH, and the relative abundance of organic material can provide accurate predictions (R2=0.77) of hygroscopic growth for the California coast.",
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