1State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, China
2Department of Environmental Toxicology, University of California, Davis, California, USA
3Atmospheric Sciences Research Center, State University of New York, Albany, New York, USA
4Research Center for Environmental Changes, Academia Sinica, Taipei, Taiwan
5Environmental Engineering Department, Mokpo National University, South of Korea
6Department of Atmospheric Sciences, National Taiwan University, Taipei, Taiwan
Received: 02 Sep 2011 – Discussion started: 15 Sep 2011
Abstract. We have investigated an aerosol processing and evolution event from 21–22 July during the summer 2009 Field Intensive Study at Queens College in New York City (NYC). The evolution processes are characterized by three consecutive stages: (1) aerosol wet scavenging, (2) nighttime nitrate formation, and (3) photochemical production and evolution of secondary aerosol species. Our results suggest that wet scavenging of aerosol species tends to be strongly related to their hygroscopicities and also mixing states. The scavenging leads to a significant change in bulk aerosol composition and average carbon oxidation state because of scavenging efficiencies in the following order: sulfate > low-volatility oxygenated organic aerosol (LV-OOA) > semi-volatile OOA (SV-OOA) > hydrocarbon-like OA (HOA). The second stage involves a quick formation of nitrate from heterogeneous reactions at nighttime. During the third stage, simultaneous increases of sulfate and SV-OOA were observed shortly after sunrise, indicating secondary aerosol formation. Organic aerosols become highly oxidized in ~ half day as the result of photochemical processing, consistent with previously reported results from the CO-tracer method (OA/ΔCO). The photochemical reactions appear to progress gradually associated with a transformation of SV- OOA to low-volatility species based on the evolution trends of oxygen-to-carbon (O/C) ratio, relationship between f44 (fraction of m/z 44 in OA) and f43 (fraction of m/z 43 in OA), and size evolution of OOA and HOA. Aerosols appear to become more internally mixed during the processing. Our results suggest that functionalization by incorporation of both C and O plays a major role in the early period of OA oxidation (O/C < 0.5). Our results also show that photochemical production of LV-OOA during this event is approximately 2–3 h behind of sulfate production, which might explain, sometimes, the lack of correlations between LV-OOA and sulfate, two secondary aerosol species which often exist in internal mixtures over regional scales.
Revised: 21 Nov 2011 – Accepted: 07 Dec 2011 – Published: 16 Dec 2011
Sun, Y. L., Zhang, Q., Schwab, J. J., Chen, W. N., Bae, M. S., Lin, Y. C., Hung, H. M., and Demerjian, K. L.: A case study of aerosol processing and evolution in summer in New York City, Atmos. Chem. Phys., 11, 12737-12750, doi:10.5194/acp-11-12737-2011, 2011.