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Volume 18, issue 4
Atmos. Chem. Phys., 18, 2363-2380, 2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Special issue: The CERN CLOUD experiment (ACP/AMT inter-journal SI)

Atmos. Chem. Phys., 18, 2363-2380, 2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 19 Feb 2018

Research article | 19 Feb 2018

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 Schobesberger1,2,3, Martin Heinritzi4, Sebastian Ehrhart4,a, Katrianne Lehtipalo1,5, Jasmin Tröstl5, Mario Simon4, Andreas Kürten4, Markus Leiminger6, Michael J. 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 N. Smith7, Tuukka Petäjä1, Douglas R. Worsnop1,12, Markku Kulmala1, Neil M. Donahue13,1, and Mikko Sipilä1 Nina Sarnela et al.
  • 1Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, 00014 Helsinki, Finland
  • 2University of Eastern Finland, Department of Applied Physics, P.O. Box 1627, 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 Frankfurt, Altenhöferallee 1, 60438 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, Lisbon, Portugal
  • 10Tofwerk AG, 3600 Thun, Switzerland
  • 11CERN, 1211 Geneva, Switzerland
  • 12Aerodyne Research, Inc., Billerica, MA 01821, USA
  • 13Carnegie Mellon University Center for Atmospheric Particle Studies, 5000 Forbes Ave, Pittsburgh, PA 15213, USA
  • anow at: Max-Planck Institute of Chemistry, Atmospheric Chemistry Department, Hahn-Meitner-Weg 1, 55128 Mainz, Germany

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 the reaction parameters more comprehensive for broader use.

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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 new particle formation. In this paper we studied the formation of sulfuric 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...