Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements

dc.contributor.authorHealy, Robert M.
dc.contributor.authorSciare, J.
dc.contributor.authorPoulain, Laurent
dc.contributor.authorCrippa, M.
dc.contributor.authorWiedensohler, Alfred
dc.contributor.authorPrévôt, A. S. H.
dc.contributor.authorBaltensperger, U.
dc.contributor.authorSarda-Estève, R.
dc.contributor.authorMcGuire, Maygan L.
dc.contributor.authorJeong, Cheol-Heon
dc.contributor.authorMcGillicuddy, Eoin
dc.contributor.authorO'Connor, Ian P.
dc.contributor.authorSodeau, John R.
dc.contributor.authorEvans, Greg J.
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.accessioned2016-07-28T13:03:45Z
dc.date.available2016-07-28T13:03:45Z
dc.date.issued2013-09-26
dc.date.updated2014-06-06T14:19:03Z
dc.description.abstractSingle-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 (R-2 = 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 (OOA(2)-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. 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 (R-2 = 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 (OOA(2)-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.en
dc.description.sponsorshipHigher Education Authority (PRTLI Cycle IV); European Commission (Seventh Framework Programme FP/2007–2011 MEGAPOLI; Marie Curie Action FP7-25 PEOPLE-IOF-2011, Project: CHEMBC, No. 299755)en
dc.description.statusPeer revieweden
dc.description.versionPublished Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationHealy, R.M., Sciare, J., Poulain, L., Crippa, M., Wiedensohler, A., Prévôt, A.S.H., Baltensperger, U., Sarda-Estève, R., McGuire, M.L., Jeong, C.-H., McGillicuddy, E., O'Connor, I P., Sodeau, J.R., Evans, G.J. and Wenger, J.C. (2013) 'Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements', Atmospheric Chemistry and Physics, 13, pp. 9479–9496. doi:10.5194/acp-13-9479-2013en
dc.identifier.doi10.5194/acp-13-9479-2013
dc.identifier.endpage9496en
dc.identifier.issn1680-73161680-7316
dc.identifier.journaltitleAtmospheric Chemistry and Physicsen
dc.identifier.startpage9479en
dc.identifier.urihttps://hdl.handle.net/10468/2947
dc.identifier.volume13en
dc.language.isoenen
dc.publisherCopernicus Publications on behalf of the European Geosciences Union (EGU)en
dc.rights© 2013, 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.subjectAerosolen
dc.subjectChemical compositionen
dc.subjectMass spectrometryen
dc.subjectMixingen
dc.subjectParticle sizeen
dc.subjectQuantitative analysisen
dc.subjectUrban atmosphereen
dc.subjectParisen
dc.subjectFranceen
dc.titleQuantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurementsen
dc.typeArticle (peer-reviewed)en
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