Sources and mixing state of size-resolved elemental carbon particles in a European megacity: Paris

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dc.contributor.authorHealy, Robert M.
dc.contributor.authorSciare, J.
dc.contributor.authorPoulain, Laurent
dc.contributor.authorKamili, K.
dc.contributor.authorMerkel, M.
dc.contributor.authorMüller, T.
dc.contributor.authorWiedensohler, Alfred
dc.contributor.authorEckhardt, S.
dc.contributor.authorStohl, A.
dc.contributor.authorSarda-Estève, R.
dc.contributor.authorMcGillicuddy, Eoin
dc.contributor.authorO'Connor, Ian P.
dc.contributor.authorSodeau, John R.
dc.contributor.authorWenger, John C.
dc.contributor.funderHigher Education Authorityen
dc.contributor.funderIrish Research Council for Science Engineering and Technologyen
dc.contributor.funderEuropean Commission
dc.date.accessioned2016-07-28T15:12:41Z
dc.date.available2016-07-28T15:12:41Z
dc.date.issued2012-02-15
dc.date.updated2014-06-06T14:20:42Z
dc.description.abstractAn Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS) was deployed to investigate the size-resolved chemical composition of single particles at an urban background site in Paris, France, as part of the MEGAPOLI winter campaign in January/February 2010. ATOFMS particle counts were scaled to match coincident Twin Differential Mobility Particle Sizer (TDMPS) data in order to generate hourly size-resolved mass concentrations for the single particle classes observed. The total scaled ATOFMS particle mass concentration in the size range 150–1067 nm was found to agree very well with the sum of concurrent High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and Multi-Angle Absorption Photometer (MAAP) mass concentration measurements of organic carbon (OC), inorganic ions and black carbon (BC) (R2 = 0.91). Clustering analysis of the ATOFMS single particle mass spectra allowed the separation of elemental carbon (EC) particles into four classes: (i) EC attributed to biomass burning (ECbiomass), (ii) EC attributed to traffic (ECtraffic), (iii) EC internally mixed with OC and ammonium sulfate (ECOCSOx), and (iv) EC internally mixed with OC and ammonium nitrate (ECOCNOx). Average hourly mass concentrations for EC-containing particles detected by the ATOFMS were found to agree reasonably well with semi-continuous quantitative thermal/optical EC and optical BC measurements (r2 = 0.61 and 0.65–0.68 respectively, n = 552). The EC particle mass assigned to fossil fuel and biomass burning sources also agreed reasonably well with BC mass fractions assigned to the same sources using seven-wavelength aethalometer data (r2 = 0.60 and 0.48, respectively, n = 568). Agreement between the ATOFMS and other instrumentation improved noticeably when a period influenced by significantly aged, internally mixed EC particles was removed from the intercomparison. 88% and 12% of EC particle mass was apportioned to fossil fuel and biomass burning respectively using the ATOFMS data compared with 85% and 15% respectively for BC estimated from the aethalometer model. On average, the mass size distribution for EC particles is bimodal; the smaller mode is attributed to locally emitted, mostly externally mixed EC particles, while the larger mode is dominated by aged, internally mixed ECOCNOx particles associated with continental transport events. Periods of continental influence were identified using the Lagrangian Particle Dispersion Model (LPDM) "FLEXPART". A consistent minimum between the two EC mass size modes was observed at approximately 400 nm for the measurement period. EC particles below this size are attributed to local emissions using chemical mixing state information and contribute 79% of the scaled ATOFMS EC particle mass, while particles above this size are attributed to continental transport events and contribute 21% of the EC particle mass. These results clearly demonstrate the potential benefit of monitoring size-resolved mass concentrations for the separation of local and continental EC emissions. Knowledge of the relative input of these emissions is essential for assessing the effectiveness of local abatement strategies.en
dc.description.sponsorshipHigher Education Authority, Ireland (PRTLI cycle IV); European Commission (Seventh Framework Programme FP/2007-2011 MEGAPOLI Project, Grant Agreement No. 212520)en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationHealy, R. M., Sciare, J., Poulain, L., Kamili, K., Merkel, M., Müller, T., Wiedensohler, A., Eckhardt, S., Stohl, A., Sarda-Estève, R., McGillicuddy, E., O'Connor, I.P., Sodeau, J.R., and Wenger, J.C. (2012) ‘Sources and mixing state of size-resolved elemental carbon particles in a European megacity: Paris’, Atmospheric Chemistry and Physics, 12, 1681-1700. doi:10.5194/acp-12-1681-2012en
dc.identifier.doi10.5194/acp-12-1681-2012
dc.identifier.endpage1700en
dc.identifier.issn1680-7316
dc.identifier.journaltitleAtmospheric Chemistry and Physicsen
dc.identifier.startpage1681en
dc.identifier.urihttps://hdl.handle.net/10468/2949
dc.identifier.volume12en
dc.language.isoenen
dc.publisherCopernicus Publications on behalf of the European Geosciences Union (EGU)en
dc.rights© 2012, the Authors. This work is distributed under the Creative Commons Attribution 3.0 License.en
dc.rights.urihttps://creativecommons.org/licenses/by/3.0/en
dc.subjectBiomass burningen
dc.subjectBlack carbonen
dc.subjectConcentrationen
dc.subjectCompositionen
dc.subjectFossil fuelen
dc.subjectMegacityen
dc.subjectMixingen
dc.subjectOrganic carbonen
dc.subjectParticle sizeen
dc.subjectParisen
dc.subjectFranceen
dc.titleSources and mixing state of size-resolved elemental carbon particles in a European megacity: Parisen
dc.typeArticle (peer-reviewed)en
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