Twenty-four hour integrated filter samples of fine particulate matter (PM2.5) were collected from May 2004 to April 2005 at one rural site and three urban sites located in the southeastern United States. Filters were extracted and analyzed for both biogenic secondary organic aerosol (SOA) tracers via gas chromatography-mass spectrometry (GC-MS), and water-soluble organic carbon (WSOC) concentrations. The tracers reported in this study include isoprene-derived 2-methylthreitol and 2-methylerythritol, as well as pinene-derived cis-pinonic acid. The mean ambient concentrations ranged from 21.7 to 94.3 ng/m3, 5.31 to 17.9 ng/m3, and 1.87 to 3.18 microgC/m3 for 2-methyltetrols (sum of 2-methylerythritol and 2-methylthreitol), cispinonic acid and WSOC, respectively. Distinct spatial distributions were observed for all tracers with the highest concentration at the rural site and the lowest level at a coastal site. Although 2-methyltetrols were small fractions of WSOC, varying from 0.35% at an urban site to highest fractions of 1.09% at the rural site, WSOC exhibited significant correlation with 2-methyltetrols during summer, suggesting isoprene SOA makes an important contribution to WSOC. 2-Methyltetrols had the highest concentrations during the summer,when high temperature, intense solar radiation, and high ozone level occurred. However, no obvious seasonal variation was found for cispinonic acid. Between inland sites WSOC was more spatially homogeneous than the 2-methyltetrols, suggesting that WSOC was produced from a variety of mechanisms.

Radiocarbon ( 14 C) analysis is a unique tool to distinguish fossil/nonfossil sources of carbonaceous aerosols. We present 14 C measurements of organic carbon (OC) and total carbon (TC) on highly time resolved filters (3-4 h, typically 12 h or longer have been reported) from 7 days collected during California Research at the Nexus of Air Quality and Climate Change (CalNex) 2010 in Pasadena. Average nonfossil contributions of 58% ± 15% and 51% ± 15% were found for OC and TC, respectively. Results indicate that nonfossil carbon is a major constituent of the background aerosol, evidenced by its nearly constant concentration (2-3 μgC m À3). Cooking is estimated to contribute at least 25% to nonfossil OC, underlining the importance of urban nonfossil OC sources. In contrast, fossil OC concentrations have prominent and consistent diurnal profiles, with significant afternoon enhancements (~3 μgC m À3 ), following the arrival of the western Los Angeles (LA) basin plume with the sea breeze. A corresponding increase in semivolatile oxygenated OC and organic vehicular emission markers and their photochemical reaction products occurs. This suggests that the increasing OC is mostly from fresh anthropogenic secondary OC (SOC) from mainly fossil precursors formed in the western LA basin plume. We note that in several European cities where the diesel passenger car fraction is higher, SOC is 20% less fossil, despite 2-3 times higher elemental carbon concentrations, suggesting that SOC formation from gasoline emissions most likely dominates over diesel in the LA basin. This would have significant implications for our understanding of the on-road vehicle contribution to ambient aerosols and merits further study.