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

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

Research output: Contribution to journalArticleScientificpeer-review

9 Citations (Scopus)

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 3.5-6.52-320-50 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.
Original languageEnglish
Pages (from-to)2363-2380
Number of pages18
JournalAtmospheric Chemistry and Physics
Volume18
Issue number4
DOIs
Publication statusPublished - 1 Feb 2018
Externally publishedYes
Publication typeA1 Journal article-refereed

Keywords

  • 114 Physical sciences
  • GAS-PHASE OZONOLYSIS
  • VOLATILE ORGANIC-COMPOUNDS
  • OXIDATION-PRODUCTS
  • PARTICLE FORMATION
  • CHEMICAL-IONIZATION
  • AEROSOL FORMATION
  • GROWTH-RATES
  • ATMOSPHERIC SULFURIC-ACID
  • IONIZATION MASS-SPECTROMETRY
  • WATER-VAPOR

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