Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument

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http://hdl.handle.net/10138/211401

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Novelli , A , Hens , K , Ernest , C T , Martinez , M , Noelscher , A C , Sinha , V , Paasonen , P , Petäjä , T , Sipilä , M , Elste , T , Plass-Duelmer , C , Phillips , G J , Kubistin , D , Williams , J , Vereecken , L , Lelieveld , J & Harder , H 2017 , ' Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument ' , Atmospheric Chemistry and Physics , vol. 17 , no. 12 , pp. 7807-7826 . https://doi.org/10.5194/acp-17-7807-2017

Title: Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument
Author: Novelli, Anna; Hens, Korbinian; Ernest, Cheryl Tatum; Martinez, Monica; Noelscher, Anke C.; Sinha, Vinayak; Paasonen, Pauli; Petäjä, Tuukka; Sipilä, Mikko; Elste, Thomas; Plass-Duelmer, Christian; Phillips, Gavin J.; Kubistin, Dagmar; Williams, Jonathan; Vereecken, Luc; Lelieveld, Jos; Harder, Hartwig
Contributor: University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
University of Helsinki, Department of Physics
Date: 2017-06-29
Language: eng
Number of pages: 20
Belongs to series: Atmospheric Chemistry and Physics
ISSN: 1680-7316
URI: http://hdl.handle.net/10138/211401
Abstract: We analysed the extensive dataset from the HUMPPA-COPEC 2010 and the HOPE 2012 field campaigns in the boreal forest and rural environments of Finland and Germany, respectively, and estimated the abundance of stabilised Criegee intermediates (SCIs) in the lower troposphere. Based on laboratory tests, we propose that the background OH signal observed in our IPI-LIF-FAGE instrument during the aforementioned campaigns is caused at least partially by SCIs. This hypothesis is based on observed correlations with temperature and with concentrations of unsaturated volatile organic compounds and ozone. Just like SCIs, the background OH concentration can be removed through the addition of sulfur dioxide. SCIs also add to the previously underestimated production rate of sulfuric acid. An average estimate of the SCI concentration of similar to 5.0 x 10(4) molecules cm(-3) (with an order of magnitude uncertainty) is calculated for the two environments. This implies a very low ambient concentration of SCIs, though, over the boreal forest, significant for the conversion of SO2 into H2SO4. The large uncertainties in these calculations, owing to the many unknowns in the chemistry of Criegee intermediates, emphasise the need to better understand these processes and their potential effect on the self-cleaning capacity of the atmosphere.
Subject: GAS-PHASE OZONOLYSIS
CONFORMER-DEPENDENT REACTIVITY
SULFURIC-ACID CONCENTRATIONS
SUBSTITUTED CARBONYL OXIDES
DIRECT KINETIC MEASUREMENTS
LASER-INDUCED FLUORESCENCE
TOTAL OH REACTIVITY
BOREAL FOREST
WATER-VAPOR
HYDROXYL RADICALS
114 Physical sciences
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