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Titel |
Towards a better understanding of the origins, chemical composition and aging of oxygenated organic aerosols: case study of a Mediterranean industrialized environment, Marseille |
VerfasserIn |
I. Haddad, B. D'Anna, B. Temime-Roussel, M. Nicolas, A. Boréave, O. Favez, D. Voisin, J. Sciare, C. George, J.-L. Jaffrezo, H. Wortham, N. Marchand |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1680-7316
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Chemistry and Physics ; 13, no. 15 ; Nr. 13, no. 15 (2013-08-15), S.7875-7894 |
Datensatznummer |
250085629
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Publikation (Nr.) |
copernicus.org/acp-13-7875-2013.pdf |
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Zusammenfassung |
As part of the FORMES summer 2008 experiment, an Aerodyne compact
time-of-flight aerosol mass spectrometer (cToF-AMS) was deployed at an
urban background site in Marseille to investigate the sources and aging of
organic aerosols (OA). France's second largest city and the largest port in
the Mediterranean, Marseille, provides a locale that is influenced by
significant urban industrialized emissions and an active photochemistry with
very high ozone concentrations. Particle mass spectra were analyzed by
positive matrix factorization (PMF2) and the results were in very good
agreement with previous apportionments obtained using a chemical mass
balance (CMB) approach coupled to organic markers and metals (El Haddad et
al., 2011a). AMS/PMF2 was able to identify for the first time, to the best
of our knowledge, the organic aerosol emitted by industrial processes. Even
with significant industries in the region, industrial OA was estimated to
contribute only ~ 5% of the total OA mass. Both source
apportionment techniques suggest that oxygenated OA (OOA) constitutes the
major fraction, contributing ~ 80% of OA mass. A novel
approach combining AMS/PMF2 data with 14C measurements was applied to
identify and quantify the fossil and non-fossil precursors of this fraction
and to explicitly assess the related uncertainties. Results show with high
statistical confidence that, despite extensive urban and industrial
emissions, OOA is overwhelmingly non-fossil, formed via the oxidation of
biogenic precursors, including monoterpenes. AMS/PMF2 results strongly
suggest that the variability observed in the OOA chemical composition is
mainly driven in our case by the aerosol photochemical age. This paper
presents the impact of photochemistry on the increase of OOA oxygenation
levels, formation of humic-like substances (HULIS) and the evolution of
α-pinene SOA (secondary OA) components. |
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