1Brookhaven National Laboratory, Upton, New York, USA
2Department of Environmental Toxicology, University of California, Davis, California, USA
*now at: Pacific Northwest National Laboratory, Richland, Washington, USA
**now at: Ecole Nationale Supérieure des Mines de Douai, Département Chimie & Environnement, 59508 Douai Cedex, France
***now at: Université Lille Nord de France, 59044 Lille, France
Received: 23 Feb 2013 – Published in Atmos. Chem. Phys. Discuss.: 09 Apr 2013
Abstract. During the Carbonaceous Aerosols and Radiative Effects Study (CARES), activation fraction of size-resolved aerosol particles and aerosol chemical composition were characterized at the T1 site (~60 km downwind of Sacramento, California) from 10 June to 28 June 2010. The hygroscopicity of cloud condensation nuclei (CCN)-active particles (κCCN) with diameter from 100 to 170 nm, derived from the size-resolved activated fraction, varied from 0.10 to 0.21, with an average of 0.15, which was substantially lower than that proposed for continental sites. The low κCCN value was due to the high organic volume fraction, averaged over 80% at the T1 site. The derived κCCN exhibited little diurnal variation, consistent with the relatively constant organic volume fraction observed. At any time, over 90% of the size-selected particles with diameter between 100 and 171 nm were CCN active, suggesting most particles within this size range were aged background particles. Due to the large organic volume fraction, organic hygroscopicity (κorg) strongly impacted particle hygroscopicity and therefore calculated CCN concentration. For the vast majority of the cases, an increase of κorg from 0.03 to 0.18, which are within the typical range, doubled the calculated CCN concentration. Organic hygroscopicity was derived from κCCN and aerosol chemical composition, and its variations with the fraction of total organic mass spectral signal at m / z 44 (f44) and O : C were compared to results from previous studies. Overall, the relationships between κorg and f44 are quite consistent for organic aerosol (OA) observed during field studies and those formed in a smog chamber. Compared to the relationship between κorg and f44, the relationship between κorg and O : C exhibits more significant differences among different studies, suggesting κorg may be better parameterized using f44. A least squares fit yielded κorg = 2.10(±0.07) × f44 − 0.11(±0.01) with a Pearson R2 value of 0.71. One possible explanation for the stronger correlation between κorg and f44 is that the m / z 44 signal (mostly contributed by the CO2+ ion) is more closely related to organic acids, which may dominate the overall κorg due to their relatively high water solubility and hygroscopicity.
Revised: 16 Oct 2013 – Accepted: 30 Oct 2013 – Published: 17 Dec 2013
Citation: Mei, F., Setyan, A., Zhang, Q., and Wang, J.: CCN activity of organic aerosols observed downwind of urban emissions during CARES, Atmos. Chem. Phys., 13, 12155-12169, doi:10.5194/acp-13-12155-2013, 2013.