Aqueous-Phase Reactive Uptake of Dicarbonyls as a Source of Organic Aerosol Over Eastern North America

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Aqueous-Phase Reactive Uptake of Dicarbonyls as a Source of Organic Aerosol Over Eastern North America

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dc.contributor.author Fu, Tzung-May
dc.contributor.author Jacob, Daniel J.
dc.contributor.author Heald, Colette L.
dc.date.accessioned 2010-01-20T21:36:47Z
dc.date.issued 2009
dc.identifier.citation Fu, Tzung-May, Daniel J. Jacob, and Colette L. Heald. 2009. Aqueous-phase reactive uptake of dicarbonyls as a source of organic aerosol over eastern North America. Atmospheric Environment 43(10): 1814-1822. en_US
dc.identifier.issn 1352-2310 en_US
dc.identifier.uri http://nrs.harvard.edu/urn-3:HUL.InstRepos:3553958
dc.description.abstract We use a global 3-D atmospheric chemistry model (GEOS-Chem) to simulate surface and aircraft measurements of organic carbon (OC) aerosol over eastern North America during summer 2004 (ICARTT aircraft campaign), with the goal of evaluating the potential importance of a new secondary organic aerosol (SOA) formation pathway via irreversible uptake of dicarbonyl gases (glyoxal and methylglyoxal) by aqueous particles. Both dicarbonyls are predominantly produced in the atmosphere by isoprene, with minor contributions from other biogenic and anthropogenic precursors. Dicarbonyl SOA formation is represented by a reactive uptake coefficient γ = 2.9 × 10−3 and takes place mainly in clouds. Surface measurements of OC aerosol at the IMPROVE network in the eastern U.S. average 2.2 ± 0.7 μg C m−3 for July–August 2004 with little regional structure. The corresponding model concentration is 2.8 ± 0.8 μg C m−3, also with little regional structure due to compensating spatial patterns of biogenic, anthropogenic, and fire contributions. Aircraft measurements of water-soluble organic carbon (WSOC) aerosol average 2.2 ± 1.2 μg C m−3 in the boundary layer (<2 km) and 0.9 ± 0.8 μg C m−3 in the free troposphere (2–6 km), consistent with the model (2.0 ± 1.2 μg C m−3 in the boundary layer and 1.1 ± 1.0 μg C m−3 in the free troposphere). Source attribution for the WSOC aerosol in the model boundary layer is 27% anthropogenic, 18% fire, 28% semi-volatile SOA, and 27% dicarbonyl SOA. In the free troposphere it is 13% anthropogenic, 37% fire, 23% semi-volatile SOA, and 27% dicarbonyl SOA. Inclusion of dicarbonyl SOA doubles the SOA contribution to WSOC aerosol at all altitudes. Observed and simulated correlations of WSOC aerosol with other chemical variables measured aboard the aircraft suggest a major SOA source in the free troposphere compatible with the dicarbonyl mechanism. en_US
dc.description.sponsorship Earth and Planetary Sciences en_US
dc.description.sponsorship Engineering and Applied Sciences en_US
dc.language.iso en_US en_US
dc.publisher Elsevier en_US
dc.relation.isversionof doi:10.1016/j.atmosenv.2008.12.029 en_US
dc.relation.hasversion http://acmg.seas.harvard.edu/cvdj.html#P2009 en_US
dash.license LAA
dc.subject ICARTT en_US
dc.subject secondary organic aerosol en_US
dc.subject WSOC en_US
dc.subject organic carbon en_US
dc.subject methylglyoxal en_US
dc.subject glyoxal en_US
dc.title Aqueous-Phase Reactive Uptake of Dicarbonyls as a Source of Organic Aerosol Over Eastern North America en_US
dc.type Journal Article en_US
dc.description.version Version of Record en_US
dc.relation.journal Atmospheric Environment en_US
dash.depositing.author Jacob, Daniel J.
dc.date.available 2010-01-20T21:36:47Z

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  • FAS Scholarly Articles [7594]
    Peer reviewed scholarly articles from the Faculty of Arts and Sciences of Harvard University

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