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

Novelli, A., Hens, K., Ernest, C. T., Martínez, M., Noelscher, A. C., Sinha, V., et al. (2017). Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument. Atmospheric Chemistry and Physics, 17(12), 7807-7826. doi:10.5194/acp-17-7807-2017.

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Novelli, A.1, Autor           
Hens, K.1, Autor           
Ernest, C. T.1, Autor           
Martínez, M.1, Autor           
Noelscher, Anke C.2, Autor
Sinha, Vinayak2, Autor
Paasonen, Pauli2, Autor
Petaja, Tuukka2, Autor
Sipila, Mikko2, Autor
Elste, Thomas2, Autor
Plass-Duelmer, Christian2, Autor
Phillips, G. J.1, Autor           
Kubistin, D.1, Autor           
Williams, J.1, Autor           
Vereecken, L.1, Autor           
Lelieveld, J.1, Autor           
Harder, H.1, Autor           
Affiliations:
1Atmospheric Chemistry, Max Planck Institute for Chemistry, Max Planck Society, ou_1826285              
2external, ou_persistent22              

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 Zusammenfassung: 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  ∼  5.0  ×  104 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.

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Sprache(n): eng - English
 Datum: 2017
 Publikationsstatus: Erschienen
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 Ort, Verlag, Ausgabe: -
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 Art der Begutachtung: -
 Identifikatoren: ISI: 000404653100001
DOI: 10.5194/acp-17-7807-2017
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Titel: Atmospheric Chemistry and Physics
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: Katlenburg-Lindau, Germany : European Geosciences Union
Seiten: - Band / Heft: 17 (12) Artikelnummer: - Start- / Endseite: 7807 - 7826 Identifikator: ISSN: 1680-7316
CoNE: https://pure.mpg.de/cone/journals/resource/111030403014016