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| Titel |
Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements |
| VerfasserIn |
R. M. Healy, J. Sciare, L. Poulain, M. Crippa, A. Wiedensohler, A. S. H. Prévôt, U. Baltensperger, R. Sarda-Estève, M. L. McGuire, C.-H. Jeong, E. McGillicuddy, I. P. O'Connor, J. R. Sodeau, G. J. Evans, J. C. Wenger |
| 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. 18 ; Nr. 13, no. 18 (2013-09-26), S.9479-9496 |
| Datensatznummer |
250085712
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| Publikation (Nr.) |
 copernicus.org/acp-13-9479-2013.pdf |
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| Zusammenfassung |
| Single-particle mixing state information can be a powerful tool for assessing
the relative impact of local and regional sources of ambient particulate
matter in urban environments. However, quantitative mixing state data are
challenging to obtain using single-particle mass spectrometers. In this
study, the quantitative chemical composition of carbonaceous single particles
has been determined using an aerosol time-of-flight mass spectrometer
(ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France.
Relative peak areas of marker ions for elemental carbon (EC), organic aerosol
(OA), ammonium, nitrate, sulfate and potassium were compared with concurrent
measurements from an Aerodyne high-resolution time-of-flight aerosol mass
spectrometer (HR-ToF-AMS), a thermal–optical OCEC analyser and a particle
into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived
estimated mass concentrations reproduced the variability of these species
well (R2 = 0.67–0.78), and 10 discrete mixing states for
carbonaceous particles were identified and quantified. The chemical mixing
state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix
factorisation, was also investigated through comparison with the ATOFMS
dataset. The results indicate that hydrocarbon-like OA (HOA) detected in
Paris is associated with two EC-rich mixing states which differ in their
relative sulfate content, while fresh biomass burning OA (BBOA) is
associated with two mixing states which differ significantly in their OA / EC
ratios. Aged biomass burning OA (OOA2-BBOA) was found to be
significantly internally mixed with nitrate, while secondary, oxidised OA
(OOA) was associated with five particle mixing states, each exhibiting
different relative secondary inorganic ion content. Externally mixed
secondary organic aerosol was not observed. These findings demonstrate the
range of primary and secondary organic aerosol mixing states in Paris.
Examination of the temporal behaviour and chemical composition of the ATOFMS
classes also enabled estimation of the relative contribution of transported
emissions of each chemical species and total particle mass in the size range
investigated. Only 22% of the total ATOFMS-derived particle mass was
apportioned to fresh, local emissions, with 78% apportioned to
regional/continental-scale emissions. |
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