Chemical tracer methods for determining contributions to primary organic aerosol (POA) are fairly well established, whereas similar techniques for secondary organic aerosol (SOA), inherently complicated by time-dependent atmospheric processes, are only beginning to be studied. Laboratory chamber experiments provide insights into the precursors of SOA, but field data must be used to test the approaches. This study investigates primary and secondary sources of organic carbon (OC) and determines their mass contribution to particulate matter 2.5 m or less in aerodynamic diameter (PM 2.5 ) in Southeastern Aerosol Research and Characterization (SEARCH) network samples. Filter samples were taken during 20 24-hr periods between May and August 2005 at SEARCH sites in Atlanta, GA (JST); Birmingham, AL (BHM); Centerville, AL (CTR); and Pensacola, FL (PNS) and analyzed for organic tracers by gas chromatography-mass spectrometry. Contribution to primary OC was made using a chemical mass balance method and to secondary OC using a mass fraction method. Aerosol masses were reconstructed from the contributions of POA, SOA, elemental carbon, inorganicmetals, and metal oxides and compared with the measured PM 2.5 . From the analysis, OC contributions from seven primary sources and four secondary sources were determined. The major primary sources of carbon were from wood combustion, diesel and gasoline exhaust, and meat cooking; major secondary sources were from isoprene and monoterpenes with minor contributions from toluene and -caryophyllene SOA. Mass concentrations at the four sites were determined using source-specific organic mass (OM)-to-OC ratios and gave values in the range of 12-42 g m Ϫ3 . Reconstructed masses at three of the sites (JST, CTR, PNS) ranged from 87 to 91% of the measured PM 2.5 mass. The reconstructed mass at the BHM site exceeded the measured mass by approximately 25%. The difference between the reconstructed and measured PM 2.5 mass for nonindustrial areas is consistent with not including aerosol liquid water or other sources of organic aerosol.
INTRODUCTIONPM 2.5 is composed of a wide variety of organic and inorganic components of primary and secondary origin. This size range of particulate matter (PM) leads to physiochemical changes in the atmosphere, such as visibility degradation, 1 radiative forcing, 2,3 and cloud formation. 4 In addition, several studies have indicated that PM 2.5 (PM Յ 2.5 m in aerodynamic diameter) exposure may be related to adverse health effects. 5 Moreover, recent studies have indicated that decreasing PM 2.5 levels can lead to longer life expectancies. 6 The regulation of PM 2.5 in the United States is based on aerosol mass. To formulate control strategies, particularly those based on air quality models, information is required for the mass-based composition of PM 2.5 from primary and secondary sources. Organic aerosol, which is a mixture of organic compounds from primary emissions and secondary formation, typically comprises a substantial fraction of the PM 2.5 mass. ...