Comprehensive modeling study of ozonolysis of oleic acid aerosol based on real-time, online measurements of aerosol composition

Gallimore, P. J. and Griffiths, P. T. and Pope, F. D. and Reid, J. P. and Kalberer, M.. (2017) Comprehensive modeling study of ozonolysis of oleic acid aerosol based on real-time, online measurements of aerosol composition. Journal of Geophysical Research: Atmospheres, 122 (8). pp. 4364-4377.

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Official URL: https://edoc.unibas.ch/81345/

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The chemical composition of organic aerosols profoundly influences their atmospheric properties, but a detailed understanding of heterogeneous and in-particle reactivity is lacking. We present here a combined experimental and modeling study of the ozonolysis of oleic acid particles. An online mass spectrometry (MS) method, Extractive Electrospray Ionization (EESI), is used to follow the composition of the aerosol at a molecular level in real time; relative changes in the concentrations of both reactants and products are determined during aerosol aging. The results show evidence for multiple non-first-order reactions involving stabilized Criegee intermediates, including the formation of secondary ozonides and other oligomers. Offline liquid chromatography MS is used to confirm the online MS assignment of the monomeric and dimeric products. We explain the observed EESI-MS chemical composition changes, and chemical and physical data from previous studies, using a process-based aerosol chemistry simulation, the Pretty Good Aerosol Model (PG-AM). In particular, we extend previous studies of reactant loss by demonstrating success in reproducing the time dependence of product formation and the evolving particle size. This advance requires a comprehensive chemical scheme coupled to the partitioning of semivolatile products; relevant reaction and evaporation parameters have been refined using our new measurements in combination with PG-AM.
Faculties and Departments:05 Faculty of Science > Departement Umweltwissenschaften > Geowissenschaften > Atmospheric Sciences (Kalberer)
UniBasel Contributors:Kalberer, Markus
Item Type:Article, refereed
Article Subtype:Research Article
Publisher:American Geophysical Union
Note:Publication type according to Uni Basel Research Database: Journal article
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Last Modified:13 Apr 2021 09:04
Deposited On:13 Apr 2021 09:04

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