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Published March 20, 2017 | Supplemental Material
Journal Article Open

Criegee Chemistry on Aqueous Organic Surfaces


In the troposphere, the fate of gas-phase Criegee intermediates (CIs) is deemed to be determined by their reactions with water molecules. Here it is shown that CIs produced in situ on the surface of water/acetonitrile (W/AN) solutions react competitively with millimolar carboxylic acids. Present experiments probe, via online electrospray mass spectrometry, CIs' chemistry on the surface of α-humulene and β-caryophyllene in W/AN microjets exposed to O3(g) for <10 μs. Mass-specific identification lets us establish the progeny of products and intermediates generated in the early stages of CIs' reactions with H2O, D2O, H218O, and n-alkyl-COOH (n = 1–7). It is found that n-alkyl-COOH competes for CIs with interfacial water, their competitiveness being an increasing function of n. Present findings demonstrate that CIs can react with species other than H2O on the surface of aqueous organic aerosols due to the low water concentrations prevalent in the outermost interfacial layers.

Additional Information

© 2017 American Chemical Society. Received: February 22, 2017; Accepted: March 20, 2017; Published: March 20, 2017. We are grateful to Drs. Satoshi Inomata, Akihiro Fushimi, and Kei Sato of NIES, Prof. Yosuke Sakamoto of Kyoto University, and Prof. Jun Hirokawa of Hokkaido University for helpful discussion. S.E. is grateful to the Research Foundation for Opto-science and Technology, JSPS KAKENHI Grant Numbers 15H05328 and 15K12188.

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