Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument

Hdl Handle:
http://hdl.handle.net/10034/620571
Title:
Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument
Authors:
Novelli, Anna; Hens, Korbinian; Ernest, Cheryl Tatum; Martinez, Monica; Noelscher, Anke C.; Sinha, Vinayak; Paasonen, Pauli; Petaja, Tuukka; Sipila, Mikko; Elste, Thomas; Plass-Dulmer, Christian; Phillips, Gavin J. ( 0000-0003-4443-0822 ) ; Kubistin, Dagmar; Williams, Jonathan; Vereecken, Luc; Lelieveld, Jos; Harder, Hartwig
Abstract:
We analysed the extensive dataset from the HUMPPA-COPEC 2010 and the HOPE 2012 field campaigns in the boreal forest and rural environments of Finland and Germany, respectively, and estimated the abundance of stabilised Criegee intermediates (SCI) in the lower troposphere. Based on laboratory tests, we propose that the background OH signal observed in our IPI-LIF-FAGE instrument during the afore-mentioned campaigns is caused at least partially by SCI. This hypothesis is based on observed correlations with temperature and with concentrations of unsaturated volatile organic compounds and ozone. Just like SCI, the background OH concentration can be removed through the addition of sulfur dioxide. SCI also adds to the previously underestimated production rate of sulfuric acid. An average estimate of the SCI concentration of ~ 5.0 x 104 molecules cm-3 (with an order of magnitude uncertainty) is calculated for the two environments. This implies a very low ambient concentration of SCI, though, over the boreal forest, significant for the conversion of SO2 into H2SO4. The large uncertainties in these calculations, owing to the many unknowns in the chemistry of Criegee intermediates, emphasise the need to better understand these processes and their potential effect on the self-cleaning capacity of the atmosphere.
Affiliation:
Max Planck Institute for Chemistry; Indian Institute of Science Education and Research Mohali; University of Helsinki;German Meteorological Service; University of Chester; University of Wollongong
Citation:
Novelli, A., et. al. (2017). Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument. Atmospheric Chemistry and Physics, 17, 7807-7826. DOI: 10.5194/acp-17-7807-2017.
Publisher:
Copernicus Publications
Journal:
Atmospheric Chemistry and Physics
Publication Date:
29-Jun-2017
URI:
http://hdl.handle.net/10034/620571
DOI:
10.5194/acp-17-7807-2017
Additional Links:
http://www.atmos-chem-phys.net/17/7807/2017/acp-17-7807-2017.html
Type:
Article
Language:
en
EISSN:
1680-7324
Appears in Collections:
Natural Sciences

Full metadata record

DC FieldValue Language
dc.contributor.authorNovelli, Annaen
dc.contributor.authorHens, Korbinianen
dc.contributor.authorErnest, Cheryl Tatumen
dc.contributor.authorMartinez, Monicaen
dc.contributor.authorNoelscher, Anke C.en
dc.contributor.authorSinha, Vinayaken
dc.contributor.authorPaasonen, Paulien
dc.contributor.authorPetaja, Tuukkaen
dc.contributor.authorSipila, Mikkoen
dc.contributor.authorElste, Thomasen
dc.contributor.authorPlass-Dulmer, Christianen
dc.contributor.authorPhillips, Gavin J.en
dc.contributor.authorKubistin, Dagmaren
dc.contributor.authorWilliams, Jonathanen
dc.contributor.authorVereecken, Lucen
dc.contributor.authorLelieveld, Josen
dc.contributor.authorHarder, Hartwigen
dc.date.accessioned2017-07-20T14:27:26Z-
dc.date.available2017-07-20T14:27:26Z-
dc.date.issued2017-06-29-
dc.identifier.citationNovelli, A., et. al. (2017). Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument. Atmospheric Chemistry and Physics, 17, 7807-7826. DOI: 10.5194/acp-17-7807-2017.en
dc.identifier.doi10.5194/acp-17-7807-2017-
dc.identifier.urihttp://hdl.handle.net/10034/620571-
dc.description.abstractWe analysed the extensive dataset from the HUMPPA-COPEC 2010 and the HOPE 2012 field campaigns in the boreal forest and rural environments of Finland and Germany, respectively, and estimated the abundance of stabilised Criegee intermediates (SCI) in the lower troposphere. Based on laboratory tests, we propose that the background OH signal observed in our IPI-LIF-FAGE instrument during the afore-mentioned campaigns is caused at least partially by SCI. This hypothesis is based on observed correlations with temperature and with concentrations of unsaturated volatile organic compounds and ozone. Just like SCI, the background OH concentration can be removed through the addition of sulfur dioxide. SCI also adds to the previously underestimated production rate of sulfuric acid. An average estimate of the SCI concentration of ~ 5.0 x 104 molecules cm-3 (with an order of magnitude uncertainty) is calculated for the two environments. This implies a very low ambient concentration of SCI, though, over the boreal forest, significant for the conversion of SO2 into H2SO4. The large uncertainties in these calculations, owing to the many unknowns in the chemistry of Criegee intermediates, emphasise the need to better understand these processes and their potential effect on the self-cleaning capacity of the atmosphere.en
dc.language.isoenen
dc.publisherCopernicus Publicationsen
dc.relation.urlhttp://www.atmos-chem-phys.net/17/7807/2017/acp-17-7807-2017.htmlen
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/en
dc.subjectAtmospheric chemistryen
dc.subjectLaser induced fluorescenceen
dc.subjectCriegee intermediatesen
dc.titleEstimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrumenten
dc.typeArticleen
dc.identifier.eissn1680-7324-
dc.contributor.departmentMax Planck Institute for Chemistry; Indian Institute of Science Education and Research Mohali; University of Helsinki;German Meteorological Service; University of Chester; University of Wollongongen
dc.identifier.journalAtmospheric Chemistry and Physicsen
dc.date.accepted2017-05-19-
or.grant.openaccessYesen
rioxxterms.funderUnfundeden
rioxxterms.identifier.projectUnfundeden
rioxxterms.versionAMen
rioxxterms.licenseref.startdate2017-06-29-
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