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Title: Enhanced SOA formation from mixed anthropogenic and biogenic emissions during the CARES campaign

Journal Article · · Atmospheric Chemistry and Physics, 13(4):2091-2113

The CARES campaign was conducted during June, 2010 in the vicinity of Sacramento, California to study aerosol formation and aging in a region where anthropogenic and biogenic emissions regularly mix. Here, we describe measurements from an Aerodyne High Resolution Aerosol Mass Spectrometer (AMS), an Ionicon Proton Transfer Reaction Mass Spectrometer (PTR-MS), and trace gas detectors (CO, NO, NOx) deployed on the G-1 research aircraft to investigate ambient gas- and particle-phase chemical composition. AMS measurements showed that the particle phase is dominated by organic aerosol (OA) (85% on average) with smaller concentrations of sulfate (5%), nitrate (6%) and ammonium (3%) observed. PTR-MS data showed that isoprene dominated the biogenic volatile organic compound concentrations (BVOCs), with monoterpene concentrations generally below the detection limit. Using two different metrics, median OA concentrations and the slope of plots of OA vs. CO concentrations (i.e., ΔOA/ΔCO), we contrast organic aerosol evolution on flight days with different prevailing meteorological conditions to elucidate the role of anthropogenic and biogenic emissions on OA formation. Airmasses influenced predominantly by biogenic emissions had median OA concentrations of 2.9 μg/m3 and near zero ΔOA/ΔCO. Those influenced predominantly by anthropogenic emissions had median OA concentrations of 4.7 μg/m3 and ΔOA/ΔCO ratios of 35 - 44 μg/m3ppmv. When biogenic and anthropogenic emissions mix, OA levels are dramatically enhanced with median OA concentrations of 11.4 μg/m3 and ΔOA/ΔCO ratios of 77 - 157 μg/m3ppmv. Taken together, our observations show that production of OA is enhanced when anthropogenic emissions from Sacramento mix with isoprene-rich air from the foothills. A strong, non-linear dependence of SOA yield from isoprene is the mechanistic explanation for this enhancement most consistent with both the gas- and particle-phase data. If these observations are found to be robust in other seasons and in areas outside of Sacramento, regional and global aerosol modules will need to incorporate NOx-dependent SOA yields into their algorithms. Regardless of the mechanism, accurately predicting OA mass concentrations and their effect on radiation balance will require an accurate accounting of the interactions of biogenic and anthropogenic emissions.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1072889
Report Number(s):
PNNL-SA-91032; 35605; KP1701000
Journal Information:
Atmospheric Chemistry and Physics, 13(4):2091-2113, Journal Name: Atmospheric Chemistry and Physics, 13(4):2091-2113
Country of Publication:
United States
Language:
English

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