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- Title
Measurement-model comparison of stabilized Criegee Intermediate and Highly Oxygenated Molecule production in the CLOUD chamber.
- Authors
Sarnela, Nina; Jokinen, Tuija; Duplissy, Jonathan; Chao Yan; Nieminen, Tuomo; Ehn, Mikael; Schobesberger, Siegfried; Heinritzi, Martin; Ehrhart, Sebastian; Lehtipalo, Katrianne; Tröstl, Jasmin; Simon, Mario; Kürten, Andreas; Leiminger, Markus; Lawler, Michael Joseph; Rissanen, Matti P.; Bianchi, Federico; Praplan, Arnaud P.; Hakala, Jani; Amorim, Antonio
- 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.
- Subjects
CLOUD chambers; CLOUD condensation nuclei; OZONOLYSIS
- Publication
Atmospheric Chemistry & Physics Discussions, 2017, p1
- ISSN
1680-7367
- Publication type
Abstract
- DOI
10.5194/acp-2017-780