Aerosol Chemistry Resolved by Mass Spectrometry: Linking Field Measurements of Cloud Condensation Nuclei Activity to Organic Aerosol Composition

Hdl Handle:
http://hdl.handle.net/10034/620221
Title:
Aerosol Chemistry Resolved by Mass Spectrometry: Linking Field Measurements of Cloud Condensation Nuclei Activity to Organic Aerosol Composition
Authors:
Vogel, Alexander; Schneider, Johannes; Mueller-Tautges, Christina; Phillips, Gavin J. ( 0000-0003-4443-0822 ) ; Poehlker, Mira L.; Rose, Diana; Zuth, Christoph; Makkonen, Ulla; Hakola, Hannele; Crowley, John N.; Andreae, Meinrat O.; Poeschl, Ulrich; Hoffmann, Thorsten
Abstract:
Aerosol hygroscopic properties were linked to its chemical composition by using complementary online mass spectrometric techniques in a comprehensive chemical characterization study at a rural mountaintop station in central Germany in August 2012. In particular, atmospheric pressure chemical ionization mass spectrometry ((−)APCI-MS) provided measurements of organic acids, organosulfates, and nitrooxy-organosulfates in the particle phase at 1 min time resolution. Offline analysis of filter samples enabled us to determine the molecular composition of signals appearing in the online (−)APCI-MS spectra. Aerosol mass spectrometry (AMS) provided quantitative measurements of total submicrometer organics, nitrate, sulfate, and ammonium. Inorganic sulfate measurements were achieved by semionline ion chromatography and were compared to the AMS total sulfate mass. We found that up to 40% of the total sulfate mass fraction can be covalently bonded to organic molecules. This finding is supported by both on- and offline soft ionization techniques, which confirmed the presence of several organosulfates and nitrooxy-organosulfates in the particle phase. The chemical composition analysis was compared to hygroscopicity measurements derived from a cloud condensation nuclei counter. We observed that the hygroscopicity parameter (κ) that is derived from organic mass fractions determined by AMS measurements may overestimate the observed κ up to 0.2 if a high fraction of sulfate is bonded to organic molecules and little photochemical aging is exhibited.
Affiliation:
Johannes Gutenberg-University; Max Planck Institute for Chemistry; Finnish Meteorological Insititute; Paul Scherrer Institute; University of Chester; Goethe University
Citation:
Vogel, A., et. al. (2016). Aerosol Chemistry Resolved by Mass Spectrometry: Linking Field Measurements of Cloud Condensation Nuclei Activity to Organic Aerosol Composition. Environmental Science & Technology, 50(20), 10823-10832. DOI: 10.1021/acs.est.6b01675
Publisher:
American Chemical Society
Journal:
Environmental Science & Technology
Publication Date:
6-Oct-2016
URI:
http://hdl.handle.net/10034/620221
DOI:
10.1021/acs.est.6b01675
Additional Links:
http://pubs.acs.org/doi/abs/10.1021/acs.est.6b01675
Type:
Article
Language:
en
Description:
This document is the Accepted Manuscript version of a Published Work that appeared in final form in Environmental Science & Technology, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/acs.est.6b01675
EISSN:
1520-5851
Appears in Collections:
Natural Sciences

Full metadata record

DC FieldValue Language
dc.contributor.authorVogel, Alexanderen
dc.contributor.authorSchneider, Johannesen
dc.contributor.authorMueller-Tautges, Christinaen
dc.contributor.authorPhillips, Gavin J.en
dc.contributor.authorPoehlker, Mira L.en
dc.contributor.authorRose, Dianaen
dc.contributor.authorZuth, Christophen
dc.contributor.authorMakkonen, Ullaen
dc.contributor.authorHakola, Hanneleen
dc.contributor.authorCrowley, John N.en
dc.contributor.authorAndreae, Meinrat O.en
dc.contributor.authorPoeschl, Ulrichen
dc.contributor.authorHoffmann, Thorstenen
dc.date.accessioned2016-10-24T14:14:12Z-
dc.date.available2016-10-24T14:14:12Z-
dc.date.issued2016-10-06-
dc.identifier.citationVogel, A., et. al. (2016). Aerosol Chemistry Resolved by Mass Spectrometry: Linking Field Measurements of Cloud Condensation Nuclei Activity to Organic Aerosol Composition. Environmental Science & Technology, 50(20), 10823-10832. DOI: 10.1021/acs.est.6b01675en
dc.identifier.doi10.1021/acs.est.6b01675-
dc.identifier.urihttp://hdl.handle.net/10034/620221-
dc.descriptionThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Environmental Science & Technology, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/acs.est.6b01675-
dc.description.abstractAerosol hygroscopic properties were linked to its chemical composition by using complementary online mass spectrometric techniques in a comprehensive chemical characterization study at a rural mountaintop station in central Germany in August 2012. In particular, atmospheric pressure chemical ionization mass spectrometry ((−)APCI-MS) provided measurements of organic acids, organosulfates, and nitrooxy-organosulfates in the particle phase at 1 min time resolution. Offline analysis of filter samples enabled us to determine the molecular composition of signals appearing in the online (−)APCI-MS spectra. Aerosol mass spectrometry (AMS) provided quantitative measurements of total submicrometer organics, nitrate, sulfate, and ammonium. Inorganic sulfate measurements were achieved by semionline ion chromatography and were compared to the AMS total sulfate mass. We found that up to 40% of the total sulfate mass fraction can be covalently bonded to organic molecules. This finding is supported by both on- and offline soft ionization techniques, which confirmed the presence of several organosulfates and nitrooxy-organosulfates in the particle phase. The chemical composition analysis was compared to hygroscopicity measurements derived from a cloud condensation nuclei counter. We observed that the hygroscopicity parameter (κ) that is derived from organic mass fractions determined by AMS measurements may overestimate the observed κ up to 0.2 if a high fraction of sulfate is bonded to organic molecules and little photochemical aging is exhibited.en
dc.language.isoenen
dc.publisherAmerican Chemical Societyen
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/acs.est.6b01675en
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/en
dc.subjectAtmospheric aerosolen
dc.subjectAtmospheric chemistryen
dc.subjectMass spectrometryen
dc.subjectCloud condensation nucleien
dc.titleAerosol Chemistry Resolved by Mass Spectrometry: Linking Field Measurements of Cloud Condensation Nuclei Activity to Organic Aerosol Compositionen
dc.typeArticleen
dc.identifier.eissn1520-5851-
dc.contributor.departmentJohannes Gutenberg-University; Max Planck Institute for Chemistry; Finnish Meteorological Insititute; Paul Scherrer Institute; University of Chester; Goethe Universityen
dc.identifier.journalEnvironmental Science & Technologyen
dc.date.accepted2016-09-16-
or.grant.openaccessYesen
rioxxterms.funderDFGen
rioxxterms.identifier.projectUnfundeden
rioxxterms.versionAMen
rioxxterms.licenseref.startdate2017-10-06-
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