1Department of Environmental Toxicology, University of California, 1 Shields Ave., Davis, California 95616, USA
2Atmospheric Sciences Research Center, State University of New York at Albany, Albany, New York, USA
3Research Center for Environmental Changes, Academia Sinica, Taipei, Taiwan
4Department of Atmospheric Sciences, National Taiwan University, Taipei, Taiwan
5Division of Air Resources, New York State Department of Environmental Conservation, Albany, New York, USA
*now at: Department of Atmospheric Science, Colorado State University, Fort Collins, CO, USA
**now at: Environmental Engineering Department, Mokpo National University, South of Korea
Received: 19 Sep 2010 – Published in Atmos. Chem. Phys. Discuss.: 04 Oct 2010
Abstract. Submicron aerosol particles (PM1) were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer during the summer 2009 Field Intensive Study at Queens College in New York, NY. Organic aerosol (OA) and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of the total PM1 mass. The average mass-based size distribution of OA presents a small mode peaking at ~150 nm (Dva) and an accumulation mode (~550 nm) that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of both sulfate and OA peak between 01:00–02:00 p.m. EST due to photochemical production. The average (±σ) oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of OA in NYC are 0.36 (±0.09), 1.49 (±0.08), and 0.012 (±0.005), respectively, corresponding to an average organic mass-to-carbon (OM/OC) ratio of 1.62 (±0.11). Positive matrix factorization (PMF) of the high resolution mass spectra identified two primary OA (POA) sources, traffic and cooking, and three secondary OA (SOA) components including a highly oxidized, regional low-volatility oxygenated OA (LV-OOA; O/C = 0.63), a less oxidized, semi-volatile SV-OOA (O/C = 0.38) and a unique nitrogen-enriched OA (NOA; N/C = 0.053) characterized with prominent CxH2x + 2N+ peaks likely from amino compounds. Our results indicate that cooking and traffic are two distinct and mass-equivalent POA sources in NYC, together contributing ~30% of the total OA mass during this study. The OA composition is dominated by secondary species, especially during high PM events. SV-OOA and LV-OOA on average account for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC appears to progress with a continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed analysis of NOA (5.8% of OA) presents evidence that organic nitrogen species such as amines might have played an important role in the atmospheric processing of OA in NYC, likely involving both acid-base chemistry and photochemistry. In addition, analysis of air mass trajectories and satellite imagery of aerosol optical depth (AOD) indicates that the high potential source regions of secondary sulfate and aged OA are mainly located in regions to the west and southwest of the city.
Revised: 11 Jan 2011 – Accepted: 12 Feb 2011 – Published: 18 Feb 2011
Sun, Y.-L., Zhang, Q., Schwab, J. J., Demerjian, K. L., Chen, W.-N., Bae, M.-S., Hung, H.-M., Hogrefe, O., Frank, B., Rattigan, O. V., and Lin, Y.-C.: Characterization of the sources and processes of organic and inorganic aerosols in New York city with a high-resolution time-of-flight aerosol mass apectrometer, Atmos. Chem. Phys., 11, 1581-1602, doi:10.5194/acp-11-1581-2011, 2011.