Identifying Criegee intermediates as potential oxidants in the troposphere
Authors
Novelli, AnnaHens, Korbinian
Tatum-Ernest, Cheryl
Martinez, Monica
Noelscher, Anke C.
Sinha, Vinayak
Paasonen, Pauli
Petaja, Tuukka
Sipila, Mikko
Elste, Thomas
Plass-Dulmer, Christian
Phillips, Gavin J.
Kubistin, Dagmar
Williams, Jonathan
Vereecken, Luc
Lelieveld, Jos
Harder, Hartwig
Affiliation
Max Planck Institute for Chemistry; Indian Institute of Science Education and Research Mohali; University of Helsinki; German Weather Service, Meteorological Observatory Hohenpeissenberg; University of Chester; University of WollongongPublication Date
2017-06-29
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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 (SCI) in the lower troposphere. Based on laboratory tests, we propose that the background OH signal observed in our IPI-LIF-FAGE instrument during the afore-mentioned campaigns is caused at least partially by SCI. This hypothesis is based on observed correlations with temperature and with concentrations of unsaturated volatile organic compounds and ozone. The background OH concentration also complements the previously underestimated production rate of sulfuric acid and is consistent with its scavenging through the addition of sulphur dioxide. A central estimate of the SCI concentration of ~ 5 × 104 molecules cm−3 (with an order of magnitude uncertainty) is calculated for the two environments. This implies a very low ambient concentration of SCI, 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.Citation
Novelli, A., et. al. (2017). Identifying Criegee intermediates as potential oxidants in the troposphere. Atmospheric Chemistry and Physics Discussions, 17, 7807-7826. DOI:10.5194/acp-2016-919Publisher
Copernicus PublicationsAdditional Links
http://www.atmos-chem-phys-discuss.net/acp-2016-919/Type
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enDescription
Discussion started 24/10/16EISSN
1680-7375ae974a485f413a2113503eed53cd6c53
10.5194/acp-2016-919
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