Molecular composition of biogenic secondary organic aerosols using ultrahigh resolution mass spectrometry: comparing laboratory and field studies

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Date
2013-11
Authors
Kourtchev, Ivan
Fuller, S. J.
Giorio, Chiara
Healy, Robert M.
Wilson, Eoin
O'Connor, Ian P.
Wenger, John C.
McLeod, M.
Aalto, Juho
Ruuskanen, T. M.
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Copernicus Publications
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Abstract
Numerous laboratory experiments have been performed in an attempt to mimic atmospheric secondary organic aerosol (SOA) formation. However, it is still unclear how close the aerosol particles generated in laboratory experiments resemble atmospheric SOA with respect to their detailed chemical composition. In this study, we generated SOA in a simulation chamber from the ozonolysis of α-pinene and a biogenic volatile organic compound (BVOC) mixture containing α- and β-pinene, Δ3-carene, and isoprene. The detailed molecular composition of laboratory-generated SOA was compared with that of background ambient aerosol collected at a boreal forest site (Hyytiälä, Finland) and an urban location (Cork, Ireland) using direct infusion nanoelectrospray ultrahigh resolution mass spectrometry. Kendrick Mass Defect and Van Krevelen approaches were used to identify and compare compound classes and distributions of the detected species. The laboratory-generated SOA contained a distinguishable group of dimers that was not observed in the ambient samples. The presence of dimers was found to be less pronounced in the SOA from the VOC mixtures when compared to the one component precursor system. The elemental composition of the compounds identified in the monomeric region from the ozonolysis of both α-pinene and VOC mixtures represented the ambient organic composition of particles collected at the boreal forest site reasonably well, with about 70% of common molecular formulae. In contrast, large differences were found between the laboratory-generated BVOC samples and the ambient urban sample. To our knowledge this is the first direct comparison of molecular composition of laboratory-generated SOA from BVOC mixtures and ambient samples.
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Keywords
Atmospheric secondary organic aerosol , Biogenic volatile organic compound
Citation
KOURTCHEV, I., FULLER, S. J., GIORIO, C., HEALY, R. M., WILSON, E., O'CONNOR, I. P., WENGER, J. C., MCLEOD, M., AALTO, J., RUUSKANEN, T. M., MAENHAUT, W., JONES, R., VENABLES, D. S., SODEAU, J. R., KULMALA, M. & KALBERER, M. 2013. Molecular composition of biogenic secondary organic aerosols using ultrahigh resolution mass spectrometry: comparing laboratory and field studies. Atmospheric Chemistry and Physics Discussions. 13, 29593-29627.