Abstract
Abstract. Long-term (1999 to 2013) data from the Southeastern Aerosol Research and Characterization (SEARCH) network are used to show that anthropogenic emission reductions led to important decreases in fine-particle organic aerosol (OA) concentrations in the southeastern US On average, 45 % (range 25 to 63 %) of the 1999 to 2013 mean organic carbon (OC) concentrations are attributed to combustion processes, including fossil fuel use and biomass burning, through associations of measured OC with combustion products such as elemental carbon (EC), carbon monoxide (CO), and nitrogen oxides (NOx). The 2013 mean combustion-derived OC concentrations were 0.5 to 1.4 µg m−3 at the five sites operating in that year. Mean annual combustion-derived OC concentrations declined from 3.8 ± 0.2 µg m−3 (68 % of total OC) to 1.4 ± 0.1 µg m−3 (60 % of total OC) between 1999 and 2013 at the urban Atlanta, Georgia, site (JST) and from 2.9 ± 0.4 µg m−3 (39 % of total OC) to 0.7 ± 0.1 µg m−3 (30 % of total OC) between 2001 and 2013 at the urban Birmingham, Alabama (BHM), site. The urban OC declines coincide with reductions of motor vehicle emissions between 2006 and 2010, which may have decreased mean OC concentrations at the urban SEARCH sites by > 2 µg m−3. BHM additionally exhibits a decline in OC associated with SO2 from 0.4 ± 0.04 µg m−3 in 2001 to 0.2 ± 0.03 µg m−3 in 2013, interpreted as the result of reduced emissions from industrial sources within the city. Analyses using non-soil potassium as a biomass burning tracer indicate that biomass burning OC occurs throughout the year at all sites. All eight SEARCH sites show an association of OC with sulfate (SO4) ranging from 0.3 to 1.0 µg m−3 on average, representing ∼ 25 % of the 1999 to 2013 mean OC concentrations. Because the mass of OC identified with SO4 averages 20 to 30 % of the SO4 concentrations, the mean SO4-associated OC declined by ∼ 0.5 to 1 µg m−3 as SO4 concentrations decreased throughout the SEARCH region. The 2013 mean SO4 concentrations of 1.7 to 2.0 µg m−3 imply that future decreases in mean SO4-associated OC concentrations would not exceed ∼ 0.3 to 0.5 µg m−3. Seasonal OC concentrations, largely identified with ozone (O3), vary from 0.3 to 1.4 µg m−3 ( ∼ 20 % of the total OC concentrations).
Highlights
In much of North America, organic aerosol (OA) represents approximately half of average PM2.5 mass concentrations in ambient air (Kanakidou et al, 2005)
Corresponding declines occurred in on-road and non-road motor vehicle PM2.5 organic carbon (OC) emissions, but total PM2.5 OC emissions showed little trend due to the dominance of relatively constant biomass burning emissions (Hidy et al, 2014)
Five analytical methods indicate that a major component (∼ 45 % on average, 1999 to 2013, all sites; intersite range 25 to 63 %) of OA derives from combustion sources, including motor vehicles and biomass burning, at all urban and rural sites and throughout the year
Summary
In much of North America, organic aerosol (OA) represents approximately half of average PM2.5 mass concentrations in ambient air (Kanakidou et al, 2005). OA derives from primary source emissions and secondary atmospheric processes involving reactions of volatile organic compounds (VOCs) of anthropogenic and natural origins (see Appendix). The latter is widely recognized in the southeastern US with its potential source of VOCs from dense vegetation (Hand et al, 2012). Initial speculation about secondary organic aerosol (SOA) in the southeast from natural terpenoid compounds dates back to 1991 (e.g., Pandis et al, 1991). The early 2000s investigations involving isoprene and terpenoids identified chemical mechanisms hypothetically applicable in the ambient atmo-
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