Journal Article PreJuSER-15262

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SOA from limonene: role of NO3 in its generation and degradation

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2011
EGU Katlenburg-Lindau

Atmospheric chemistry and physics 11, 3879 - 3894 () [10.5194/acp-11-3879-2011]

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Abstract: The formation of organic nitrates and secondary organic aerosol (SOA) were monitored during the NO3 + limonene reaction in the atmosphere simulation chamber SAPHIR at Research Center Julich. The 24-h run began in a purged, dry, particle-free chamber and comprised two injections of limonene and oxidants, such that the first experiment measured SOA yield in the absence of seed aerosol, and the second experiment yields in the presence of 10 mu g m(-3) seed organic aerosol. After each injection, two separate increases in aerosol mass were observed, corresponding to sequential oxidation of the two limonene double bonds. Analysis of the measured NO3, limonene, product nitrate concentrations, and aerosol properties provides mechanistic insight and constrains rate constants, branching ratios and vapor pressures of the products. The organic nitrate yield from NO3 + limonene is approximate to 30%. The SOA mass yield was observed to be 25-40%. The first injection is reproduced by a kinetic model. PMF analysis of the aerosol composition suggests that much of the aerosol mass results from combined oxidation by both O-3 and NO3, e. g., oxidation of NO3 + limonene products by O-3. Further, later aerosol nitrate mass seems to derive from heterogeneous uptake of NO3 onto unreacted aerosol alkene.

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Note: The Berkeley authors were supported by NSF ATM-0639847 and NSF ATM-0511829. The authors thank the entire SAPHIR NO<INF>3</INF> intercomparison campaign team, June 2007 at Forschungszentrum Julich, for their support of these experiments. This work was a joint activity of the European Network of Excellence ACCENT (contract no: GOCE CT-2004-505337) and EUROCHAMP.

Contributing Institute(s):
  1. Troposphäre (IEK-8)
Research Program(s):
  1. Atmosphäre und Klima (P23)

Appears in the scientific report 2011
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