Atmos. Chem. Phys. Discuss., 13, 3533-3573, 2013
www.atmos-chem-phys-discuss.net/13/3533/2013/
doi:10.5194/acpd-13-3533-2013
© Author(s) 2013. 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.
Evaluating the degree of oxygenation of organic aerosol during foggy and hazy days in Hong Kong using high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS)
Y. J. Li1, B. Y. L. Lee1, J. Z. Yu1,2, N. L. Ng3, and C. K. Chan1,4
1Division of Environment, Hong Kong University of Science and Technology, Hong Kong, China
2Department of Chemistry, Hong Kong University of Science and Technology, Hong Kong, China
3School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia, USA
4Department of Chemical and Biomolecular Engineering, Hong Kong University of Science and Technology, Hong Kong, China

Abstract. The chemical characteristics of organic aerosol (OA) are still poorly constrained. Here we present observation results of the degree of oxygenation of OA based on high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) measurements made at a coastal site in Hong Kong from late April to the end of May in 2011. Two foggy periods and one hazy period were chosen for detailed analysis to compare the changes in the degree of oxygenation of OA due to different processes. The Extended Aerosol Inorganic Model (E-AIM) predicted a fine particle liquid water content (LWCfp) up to 85 μg m−3 during the foggy days. Particle concentration as measured by HR-ToF-AMS was up to 60 μg m−3 during the hazy days and up to 30 μg m−3 during the foggy days. The degree of oxygenation of OA, as indicated by several parameters including the fraction of m/z 44 in organic mass spectra (f44), the elemental ratio of oxygen to carbon (O : C), and the carbon oxidation state (OSc), was evaluated against the odd oxygen (Ox) concentration, LWCfp, ionic strength (IS), and in-situ pH (pHis). Results suggest that the high concentration of OA (on average 11 μg m−3) and the high degree of oxygenation (f44 = 0.15, O : C = 0.51, and OSc = −0.31) during the hazy period were mainly due to gas-phase oxidation. During the foggy periods with low photochemical activities, the degree of oxygenation of OA was almost as high as that on the hazy days and significantly higher than that during non-foggy/non-hazy days. However, the OA evolved quite differently in the two foggy periods. The first foggy period in late April saw a larger LWCfp and a lower Ox concentration and the OA was made up of ~ 20% semi-volatile oxygenated organic aerosol (SVOOA) as resolved by positive matrix factorization (PMF). In the second foggy period in mid-May, higher Ox concentration and lower LWCfp were observed, and the OA was found to contain >50% low-volatility oxygenated organic aerosols (LVOOA). An examination of the particle-phase constituents suggests that partitioning may have been the dominating process through which oxygenated species were incorporated into the particle phase during the first foggy period, while oxidation in the aqueous phase may have been the dominating process during the second foggy period. Both physical and chemical processes were found to be important for oxygenated OA formation.

Citation: Li, Y. J., Lee, B. Y. L., Yu, J. Z., Ng, N. L., and Chan, C. K.: Evaluating the degree of oxygenation of organic aerosol during foggy and hazy days in Hong Kong using high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS), Atmos. Chem. Phys. Discuss., 13, 3533-3573, doi:10.5194/acpd-13-3533-2013, 2013.
 
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