Atmos. Chem. Phys. Discuss., 8, 10105-10151, 2008
www.atmos-chem-phys-discuss.net/8/10105/2008/
doi:10.5194/acpd-8-10105-2008
© Author(s) 2008. This work is distributed
under the Creative Commons Attribution 3.0 License.
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Relating CCN activity, volatility, and droplet growth kinetics of β-caryophyllene secondary organic aerosol
A. Asa-Awuku1, G. J. Engelhart2, B. H. Lee2, S. N. Pandis2,3, and A. Nenes1,4
1School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia, USA
2Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh,\newline Pennsylvania, USA
3Department of Chemical Engineering, University of Patras, Patra, Greece
4School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia, USA

Abstract. This study investigates the droplet formation characteristics of secondary organic aerosol (SOA) formed during the ozonolysis of sesquiterpene β-caryophyllene (with and without hydroxyl radicals present). Emphasis is placed on understanding the role of semi-volatile material on Cloud Condensation Nucleus (CCN) activity and droplet growth kinetics. Aging of β-caryophyllene SOA significantly affects all CCN-relevant properties measured throughout the experiments. Using a thermodenuder and two CCN instruments, we find that CCN activity is a strong function of temperature (activation diameter at ~0.6% supersaturation: 100±10 nm at 20°C and 130±10 nm at 35°C), suggesting that the hygroscopic fraction of the SOA is volatile. The water-soluble organic carbon (WSOC) is extracted from the SOA and characterized with Köhler Theory Analysis (KTA); the results suggest that the WSOC is composed of low molecular weight (<200 g mol−1) slightly surface-active material that constitute 5–15% of the SOA mass. These properties are similar to the water-soluble fraction of monoterpene SOA, suggesting that predictive understanding of SOA CCN activity requires knowledge of the WSOC fraction but not its exact speciation. Droplet growth kinetics of the CCN are found to be strongly anticorrelated with WSOC fraction, suggesting that the insoluble material in the SOA forms a kinetic barrier that delays droplet growth. These results have important implications for the droplet formation characteristics of SOA, and the atmospheric relevance of CCN measurements carried out at temperatures different from ambient.

Citation: Asa-Awuku, A., Engelhart, G. J., Lee, B. H., Pandis, S. N., and Nenes, A.: Relating CCN activity, volatility, and droplet growth kinetics of β-caryophyllene secondary organic aerosol, Atmos. Chem. Phys. Discuss., 8, 10105-10151, doi:10.5194/acpd-8-10105-2008, 2008.
 
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