Identifying Criegee intermediates as potential oxidants in the troposphere

Hdl Handle:
http://hdl.handle.net/10034/620224
Title:
Identifying Criegee intermediates as potential oxidants in the troposphere
Authors:
Novelli, Anna; Hens, Korbinian; Tatum-Ernest, Cheryl; Martinez, Monica; Noelscher, Anke C.; Sinha, Vinayak; Paasonen, Paasonen; 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. The background OH concentration also complements the previously underestimated production rate of sulfuric acid and is consistent with its scavenging through the addition of sulphur dioxide. A central estimate of the SCI concentration of ~ 5 × 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 Weather Service, Meteorological Observatory Hohenpeissenberg; University of Chester; University of Wollongong
Citation:
Novelli, A., et. al. (2017). Identifying Criegee intermediates as potential oxidants in the troposphere. Atmospheric Chemistry and Physics Discussions, 17, 7807-7826. DOI:10.5194/acp-2016-919
Publisher:
Copernicus Publications
Journal:
Atmospheric Chemistry and Physics Discussions
Publication Date:
29-Jun-2017
URI:
http://hdl.handle.net/10034/620224
DOI:
10.5194/acp-2016-919
Additional Links:
http://www.atmos-chem-phys-discuss.net/acp-2016-919/
Type:
Article
Language:
en
Description:
Discussion started 24/10/16
EISSN:
1680-7375
Appears in Collections:
Natural Sciences

Full metadata record

DC FieldValue Language
dc.contributor.authorNovelli, Annaen
dc.contributor.authorHens, Korbinianen
dc.contributor.authorTatum-Ernest, Cherylen
dc.contributor.authorMartinez, Monicaen
dc.contributor.authorNoelscher, Anke C.en
dc.contributor.authorSinha, Vinayaken
dc.contributor.authorPaasonen, Paasonenen
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.accessioned2016-10-25T10:50:07Z-
dc.date.available2016-10-25T10:50:07Z-
dc.date.issued2017-06-29-
dc.identifier.citationNovelli, A., et. al. (2017). Identifying Criegee intermediates as potential oxidants in the troposphere. Atmospheric Chemistry and Physics Discussions, 17, 7807-7826. DOI:10.5194/acp-2016-919en
dc.identifier.doi10.5194/acp-2016-919-
dc.identifier.urihttp://hdl.handle.net/10034/620224-
dc.descriptionDiscussion started 24/10/16-
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. The background OH concentration also complements the previously underestimated production rate of sulfuric acid and is consistent with its scavenging through the addition of sulphur dioxide. A central estimate of the SCI concentration of ~ 5 × 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-discuss.net/acp-2016-919/en
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/en
dc.subjectCriegee intermediatesen
dc.subjectAtmospheric chemistryen
dc.subjectLaser induced fluorescenceen
dc.subjectSulfuric aciden
dc.titleIdentifying Criegee intermediates as potential oxidants in the troposphereen
dc.typeArticleen
dc.identifier.eissn1680-7375-
dc.contributor.departmentMax Planck Institute for Chemistry; Indian Institute of Science Education and Research Mohali; University of Helsinki; German Weather Service, Meteorological Observatory Hohenpeissenberg; University of Chester; University of Wollongongen
dc.identifier.journalAtmospheric Chemistry and Physics Discussionsen
dc.date.accepted2017-05-19-
or.grant.openaccessYesen
rioxxterms.funderUnfundeden
rioxxterms.identifier.projectUnfundeden
rioxxterms.versionAMen
rioxxterms.licenseref.startdate2016-10-24-
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