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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
© Author(s) 2017. This work is distributed under
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Research article
13 Sep 2017
Review status
This discussion paper is a preprint. A revision of this manuscript was accepted for the journal Atmospheric Chemistry and Physics (ACP) and is expected to appear here in due course.
Measurement-model comparison of stabilized Criegee Intermediate and Highly Oxygenated Molecule production in the CLOUD chamber
Nina Sarnela1, Tuija Jokinen1, Jonathan Duplissy1, Chao Yan1, Tuomo Nieminen2, Mikael Ehn1, Siegfried Schobesberger1,3, Martin Heinritzi4, Sebastian Ehrhart4, Katrianne Lehtipalo1,5, Jasmin Tröstl5, Mario Simon4, Andreas Kürten4, Markus Leiminger6, Michael Joseph Lawler7, Matti P. Rissanen1, Federico Bianchi1, Arnaud P. Praplan8, Jani Hakala1, Antonio Amorim9, Marc Gonin10, Armin Hansel6, Jasper Kirkby4,11, Josef Dommen5, Joachim Curtius4, James Smith7, Tuukka Petäjä1, Douglas R. Worsnop1,12, Markku Kulmala1, Neil M. Donahue13, and Mikko Sipilä1 1Department of Physics, University of Helsinki, Box 64, 00014 Helsinki, Finland
2University of Eastern Finland, Department of Applied Physics, PO Box 1627, FI-70211 Kuopio, Finland
3Department of Atmospheric Sciences, University of Washington, 408 ATG Bldg, Box 351640, Seattle, WA 98195, USA
4Institute for Atmospheric and Environmental Sciences, Goethe University of Frankfurt, Frankfurt am Main, Germany
5Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
6University of Innsbruck, Institute for Ion Physics and Applied Physics, Technikerstraße 25, 6020 Innsbruck, Austria
7University of California, Irvine, Department of Chemistry, Irvine, CA 92697, USA
8Finnish Meteorological Institute, P.O. Box 503, 00101 Helsinki, Finland
9CENTRA, Faculdade de Ciencias da Universidade de Lisboa
10Tofwerk AG, 3600 Thun, Switzerland
11CERN, CH-1211 Geneva, Switzerland
12Aerodyne Research, Inc., Billerica, MA 01821, USA
13Carnegie Mellon University Center for Atmospheric Particle Studies, 5000 Forbes Ave, Pittsburgh Pennsylvania, 15213, USA
Abstract. Atmospheric oxidation is an important phenomenon, which produces large quantities of low-volatile compounds such as sulphuric acid and oxidised organic compounds. Such species may be involved in 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 the ozonolysis in the Cosmic Leaving OUtdoors 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 (HOM) purely driven by ozonolysis, and study the oxidation of sulphur dioxide (SO2) driven by stabilized Criegee Intermediates (sCI). We measured the concentrations of HOM and sulphuric 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 dynamic model. We found molar yields in the range of 3.5–6.5 % for the HOM formation and 22–32 % for the formation of stabilized Criegee Intermediates by fitting our model to the measured concentrations. The simulated time evolution of the ozonolysis products was in good agreement with measured concentrations except that in some of the experiments sulphuric acid formation was faster than simulated. 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 to understand atmospheric oxidation processes better and make the reaction parameters more comprehensive for broader use.

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., Petäjä, T., Worsnop, D. R., Kulmala, M., Donahue, N. M., and Sipilä, M.: Measurement-model comparison of stabilized Criegee Intermediate and Highly Oxygenated Molecule production in the CLOUD chamber, Atmos. Chem. Phys. Discuss.,, in review, 2017.
Nina Sarnela et al.
Nina Sarnela et al.


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Short summary
Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes through the condensation of vapours. This process is called the new particle formation. In this paper we studied the formation of sulphuric acid and highly oxygenated molecules, the key compounds in atmospheric new particle formation, in chamber experiments and introduced a way to simulate these ozonolysis products of α-pinene in a simple manner.
Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes...