Measurement–model comparison of stabilized Criegee intermediate and highly oxygenated molecule production in the CLOUD chamber

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dc.contributor.author Sarnela, Nina
dc.contributor.author Jokinen, Tuija
dc.contributor.author Duplissy, Jonathan
dc.contributor.author Yan, Chao
dc.contributor.author Nieminen, Tuomo
dc.contributor.author Ehn, Mikael
dc.contributor.author Schobesberger, Siegfried
dc.contributor.author Heinritzi, Martin
dc.contributor.author Ehrhart, Sebastian
dc.contributor.author Lehtipalo, Katrianne
dc.contributor.author Tröstl, Jasmin
dc.contributor.author Simon, Mario
dc.contributor.author Kürten, Andreas
dc.contributor.author Leiminger, Markus
dc.contributor.author Lawler, Michael J.
dc.contributor.author Rissanen, Matti P.
dc.contributor.author Bianchi, Federico
dc.contributor.author Praplan, Arnaud P.
dc.contributor.author Hakala, Jani
dc.contributor.author Amorim, Antonio
dc.contributor.author Gonin, Marc
dc.contributor.author Hansel, Armin
dc.contributor.author Kirkby, Jasper
dc.contributor.author Dommen, Josef
dc.contributor.author Curtius, Joachim
dc.contributor.author Smith, James N.
dc.contributor.author Petäjä, Tuukka
dc.contributor.author Worsnop, Douglas R.
dc.contributor.author Kulmala, Markku
dc.contributor.author Donahue, Neil M.
dc.contributor.author Sipilä, Mikko
dc.date.accessioned 2018-07-04T13:07:01Z
dc.date.available 2018-07-04T13:07:01Z
dc.date.issued 2018-02-19
dc.identifier.citation Sarnela , N , Jokinen , T , Duplissy , J , Yan , C , Nieminen , T , Ehn , M , Schobesberger , S , Heinritzi , M , Ehrhart , S , Lehtipalo , K , Tröstl , J , Simon , M , Kürten , A , Leiminger , M , Lawler , M J , Rissanen , M P , Bianchi , F , Praplan , A P , Hakala , J , Amorim , A , Gonin , M , Hansel , A , Kirkby , J , Dommen , J , Curtius , J , Smith , J N , Petäjä , T , Worsnop , D R , Kulmala , M , Donahue , N M & Sipilä , M 2018 , ' Measurement–model comparison of stabilized Criegee intermediate and highly oxygenated molecule production in the CLOUD chamber ' , Atmospheric Chemistry and Physics , vol. 18 , no. 4 , pp. 2363-2380 . https://doi.org/10.5194/acp-18-2363-2018
dc.identifier.other PURE: 99572713
dc.identifier.other PURE UUID: 2bbad543-d596-4f79-8a10-88fe193fe987
dc.identifier.other Scopus: 85042451097
dc.identifier.other ORCID: /0000-0002-1660-2706/work/46452828
dc.identifier.other ORCID: /0000-0002-8594-7003/work/46454494
dc.identifier.other ORCID: /0000-0003-0463-8098/work/46454868
dc.identifier.other ORCID: /0000-0003-2996-3604/work/46470119
dc.identifier.other WOS: 000425505500001
dc.identifier.other ORCID: /0000-0003-1874-3235/work/64324426
dc.identifier.other ORCID: /0000-0002-1881-9044/work/102822727
dc.identifier.uri http://hdl.handle.net/10138/236944
dc.description.abstract Atmospheric oxidation is an important phenomenon which produces large quantities of low-volatility compounds such as sulfuric acid and oxidized organic compounds. Such species may be involved in the nucleation of particles and enhance their subsequent growth to reach the size of cloud condensation nuclei (CCN). In this study, we investigate alpha-pinene, the most abundant monoterpene globally, and its oxidation products formed through ozonolysis in the Cosmic Leaving OUtdoor Droplets (CLOUD) chamber at CERN (the European Organization for Nuclear Research). By scavenging hydroxyl radicals (OH) with hydrogen (H-2), we were able to investigate the formation of highly oxygenated molecules (HOMs) purely driven by ozonolysis and study the oxidation of sulfur dioxide (SO2) driven by stabilized Criegee intermediates (sCIs). We measured the concentrations of HOM and sulfuric acid with a chemical ionization atmospheric-pressure interface time-of-flight (CI-APi-TOF) mass spectrometer and compared the measured concentrations with simulated concentrations calculated with a kinetic model. We found molar yields in the range of 3.5-6.5% for HOM formation and 22-32% for the formation of stabilized Criegee intermediates by fitting our model to the measured sulfuric acid concentrations. The simulated time evolution of the ozonolysis products was in good agreement with measured concentrations except that in some of the experiments sulfuric acid formation was faster than simulated. In those experiments the simulated and measured concentrations met when the concentration reached a plateau but the plateau was reached 20-50 min later in the simulations. The results shown here are consistent with the recently published yields for HOM formation from different laboratory experiments. Together with the sCI yields, these results help us to understand atmospheric oxidation processes better and make the reaction parameters more comprehensive for broader use. en
dc.format.extent 18
dc.language.iso eng
dc.relation.ispartof Atmospheric Chemistry and Physics
dc.rights cc_by
dc.rights.uri info:eu-repo/semantics/openAccess
dc.subject 114 Physical sciences
dc.subject VOLATILE ORGANIC-COMPOUNDS
dc.subject IONIZATION MASS-SPECTROMETRY
dc.subject ATMOSPHERIC SULFURIC-ACID
dc.subject GAS-PHASE OZONOLYSIS
dc.subject PARTICLE FORMATION
dc.subject AEROSOL FORMATION
dc.subject CHEMICAL-IONIZATION
dc.subject OXIDATION-PRODUCTS
dc.subject GROWTH-RATES
dc.subject WATER-VAPOR
dc.title Measurement–model comparison of stabilized Criegee intermediate and highly oxygenated molecule production in the CLOUD chamber en
dc.type Article
dc.contributor.organization INAR Physics
dc.contributor.organization Institute for Atmospheric and Earth System Research (INAR)
dc.contributor.organization Polar and arctic atmospheric research (PANDA)
dc.description.reviewstatus Peer reviewed
dc.relation.doi https://doi.org/10.5194/acp-18-2363-2018
dc.relation.issn 1680-7316
dc.rights.accesslevel openAccess
dc.type.version publishedVersion

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