Single particle diversity and mixing state measurements

dc.contributor.authorHealy, Robert M.
dc.contributor.authorRiemer, Nicole
dc.contributor.authorWenger, John C.
dc.contributor.authorMurphy, Michael
dc.contributor.authorWest, M.
dc.contributor.authorPoulain, Laurent
dc.contributor.authorWiedensohler, Alfred
dc.contributor.authorO'Connor, Ian P.
dc.contributor.authorMcGillicuddy, Eoin
dc.contributor.authorSodeau, John R.
dc.contributor.authorEvans, Greg J.
dc.contributor.funderHigher Education Authorityen
dc.contributor.funderIrish Research Council for Science Engineering and Technologyen
dc.contributor.funderEuropean Commission
dc.contributor.funderU.S. Environmental Protection Agency, United States
dc.date.accessioned2016-07-27T14:57:13Z
dc.date.available2016-07-27T14:57:13Z
dc.date.issued2014-02-14
dc.date.updated2014-06-06T14:14:27Z
dc.description.abstractA newly developed framework for quantifying aerosol particle diversity and mixing state based on information-theoretic entropy is applied for the first time to single particle mass spectrometry field data. Single particle mass fraction estimates for black carbon, organic aerosol, ammonium, nitrate and sulfate, derived using single particle mass spectrometer, aerosol mass spectrometer and multi-angle absorption photometer measurements are used to calculate single particle species diversity (Di). The average single particle species diversity (Dα) is then related to the species diversity of the bulk population (Dγ) to derive a mixing state index value (χ) at hourly resolution. The mixing state index is a single parameter representation of how internally/externally mixed a particle population is at a given time. The index describes a continuum, with values of 0 and 100% representing fully external and internal mixing, respectively. This framework was applied to data collected as part of the MEGAPOLI winter campaign in Paris, France, 2010. Di values are low (∼ 2) for fresh traffic and wood-burning particles that contain high mass fractions of black carbon and organic aerosol but low mass fractions of inorganic ions. Conversely, Di values are higher (∼ 4) for aged carbonaceous particles containing similar mass fractions of black carbon, organic aerosol, ammonium, nitrate and sulfate. Aerosol in Paris is estimated to be 59% internally mixed in the size range 150-1067 nm, and mixing state is dependent both upon time of day and air mass origin. Daytime primary emissions associated with vehicular traffic and wood-burning result in low χ values, while enhanced condensation of ammonium nitrate on existing particles at night leads to higher χ values. Advection of particles from continental Europe containing ammonium, nitrate and sulfate leads to increases in Dα, Dγ and χ. The mixing state index represents a useful metric by which to compare and contrast ambient particle mixing state at other locations globally.en
dc.description.sponsorshipHigher Education Authority Ireland (PRTLI Cycle IV); European Commission (Seventh Framework Programme FP/2007–2011 MEGAPOLI; Marie Curie Action FP7-25 PEOPLE-IOF-2011, Project: CHEMBC, Number 299755); U.S. Environmental Protection Agency, United States (Grant Number 835042)en
dc.description.statusPeer revieweden
dc.description.versionAccepted Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationHealy, R.M., Riemer, N., Wenger, J.C., Murphy, M., West, M., Poulain, L., Wiedensohler, A., O'Connor, I.P., McGillicuddy, E., Sodeau, J.R. and Evans, G. J. (2014) 'Single particle diversity and mixing state measurements', Atmospheric Chemistry and Physics Discussions, 14, pp. 3973–4005. doi:10.5194/acpd-14-3973-2014en
dc.identifier.doi10.5194/acpd-14-3973-2014
dc.identifier.endpage4005en
dc.identifier.issn1680-7367
dc.identifier.journaltitleAtmospheric Chemistry and Physics Discussionsen
dc.identifier.startpage3973en
dc.identifier.urihttps://hdl.handle.net/10468/2945
dc.identifier.volume14en
dc.language.isoenen
dc.publisherCopernicus Publications on behalf of the European Geosciences Union (EGU)en
dc.rights© 2014, 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.subjectAmmoniumen
dc.subjectBlack carbonen
dc.subjectMeasurement methoden
dc.subjectMixingen
dc.subjectNitrateen
dc.subjectSulfateen
dc.titleSingle particle diversity and mixing state measurementsen
dc.typeArticle (peer-reviewed)en
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