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

Sarnela, Nina; Jokinen, Tuija; Duplissy, Jonathan; Yan, Chao; Nieminen, Tuomo; Ehn, Mikael; Schobesberger, Siegfried; Heinritzi, Martin; Ehrhart, Sebastian; Lehtipalo, Katrianne; Tröstl, Jasmin; Simon, Mario; Kürten, Andreas; Leiminger, Markus; Lawler, Michael J.; Rissanen, Matti P.; Bianchi, Federico; Praplan, Arnaud P.; Hakala, Jani; Amorim, Antonio; Gonin, Marc; Hansel, Armin; Kirkby, Jasper; Dommen, Josef; Curtius, Joachim; Smith, James N.; Petäjä, Tuukka; Worsnop, Douglas R.; Kulmala, Markku; Donahue, Neil M.; Sipilä, Mikko

doi:10.5194/acp-18-2363-2018

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

Journal Article · Mon Feb 19 00:00:00 EST 2018 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-18-2363-2018· OSTI ID:1505587

Sarnela, Nina ^[1];

^[1]; Duplissy, Jonathan ^[1];

^[1];

^[2];

^[1];

^[3]; Heinritzi, Martin ^[4]; Ehrhart, Sebastian ^[5];

^[6]; Tröstl, Jasmin ^[7]; Simon, Mario ^[4]; Kürten, Andreas ^[4]; Leiminger, Markus ^[8]; Lawler, Michael J. ^[9];

^[1];

^[1]; Praplan, Arnaud P. ^[10]; Hakala, Jani ^[1]; Amorim, Antonio ^[11] more »

Univ. of Helsinki, Helsinki (Finland)
Univ. of Eastern Finland, Kuopio (Finland)
Univ. of Helsinki, Helsinki (Finland); Univ. of Eastern Finland, Kuopio (Finland); Univ. of Washington, Seattle, WA (United States)
Goethe Univ. Frankfurt, Frankfurt am Main (Germany)
Goethe Univ. Frankfurt, Frankfurt am Main (Germany); Max-Planck Institute of Chemistry, Mainz (Germany)
Univ. of Helsinki, Helsinki (Finland); Paul Scherrer Inst. (PSI), Villigen (Switzerland)
Paul Scherrer Inst. (PSI), Villigen (Switzerland)
Univ. of Innsbruck, Innsbruck (Austria)
Univ. of California, Irvine, CA (United States)
Finnish Meteorological Institute, Helsinki (Finland)
CENTRA, Lisbon (Portugal)
Tofwerk AG, Thun (Switzerland)
Goethe Univ. Frankfurt, Frankfurt am Main (Germany); European Organization for Nuclear Research (CERN), Geneva (Switzerland)
Univ. of Helsinki, Helsinki (Finland); Aerodyne Research Inc., Billerica, MA (United States)
Univ. of Helsinki, Helsinki (Finland); Carnegie Mellon Univ., Pittsburgh, PA (United States)

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 α-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 (H₂), 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 20–50min 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 there action parameters more comprehensive for broader use.

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Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0014469

OSTI ID:: 1505587

Journal Information:: Atmospheric Chemistry and Physics (Online), Vol. 18, Issue 4; ISSN 1680-7324

Publisher:: European Geosciences UnionCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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Growth of Aitken mode ammonium sulfate particles by α-pinene ozonolysis Krasnomowitz, Justin M.; Apsokardu, Michael J.; Stangl, Christopher M. Taylor & Francis https://doi.org/10.6084/m9.figshare.7599686	text	January 2019
Growth of Aitken mode ammonium sulfate particles by α-pinene ozonolysis Krasnomowitz, Justin M.; Apsokardu, Michael J.; Stangl, Christopher M. Aerosol Science and Technology, Vol. 53, Issue 4 https://doi.org/10.1080/02786826.2019.1568381	journal	February 2019
Growth of Aitken Mode Ammonium Sulfate Particles by α-Pinene Ozonolysis Krasnomowitz, Justin M.; Apsokardu, Michael J.; Stangl, Christopher M. Figshare https://doi.org/10.6084/m9.figshare.7599686.v1	text	January 2019
Growth of Aitken mode ammonium sulfate particles by α-pinene ozonolysis Krasnomowitz, Justin M.; Apsokardu, Michael J.; Stangl, Christopher M. Figshare https://doi.org/10.6084/m9.figshare.7599686.v2	text	January 2019
High concentration of ultrafine particles in the Amazon free troposphere produced by organic new particle formation Zhao, Bin; Shrivastava, Manish; Donahue, Neil M. Proceedings of the National Academy of Sciences, Vol. 117, Issue 41 https://doi.org/10.1073/pnas.2006716117	journal	September 2020

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