NMOC, ozone, and organic aerosol in the southeastern United States, 1999-2007: 3. Origins of organic aerosol in Atlanta, Georgia, and surrounding areas

Carbonaceous compounds constitute a major fraction of the fine particle mass at locations throughout North America: much of the condensed-phase organic carbon (OC) is produced in the atmosphere from NMOC reactions as "secondary" OC (SOC). Ten years of particulate carbon and speciated non-methane organic compound (NMOC) data combined with other measurements from Southeastern Aerosol Research and Characterization (SEARCH) and other sites provide insight into the association between elemental carbon (EC), OC and NMOCs. Data are analyzed to characterize the OC and SOC contrasts between urban Atlanta, Georgia, and nearby non-urban conditions in the Southeast. Analysis of the monitoring record indicates that the mean Atlanta urban excess of total carbon (TC) is 2.1-2.8 mu g m(-3). The OC/EC ratio of the Atlanta urban excess is in the range 1.3 to 1.8, consistent with OC/EC ratios observed in motor vehicle emissions and a fossil carbon source of urban excess TC. Carbon isotope analysis of a subset of particle samples demonstrates that the urban excess is mainly fossil in origin, even though the majority of the TC is modern at both urban and non-urban sites. Temperature-dependent partitioning of OC between gas and condensed phases cannot explain the observed diurnal and seasonal variations of OC/CO, EC/CO, and OC/EC ratios. Alternatively, a hypothesis involving vertical mixing of OC-enriched air from aloft is supported by the seasonal and diurnal OC, isopentane, aromatic and isoprene observations at the ground. A statistical model is applied to indicate the relative significance of aerometric factors affecting OC and EC concentrations, including meteorological and pollutant associations. The model results demonstrate strong linkages between fine particle carbon and pollutant indicators of source emissions compared with meteorological factors: the model results show weaker dependence of OC on meteorological factors than is the case for ozone (O(3)) concentrations. (C) 2010 Elsevier Ltd. All rights reserved.