Novelli, Anna and Hens, Korbinian and Ernest, Cheryl Tatum and Martinez, Monica and Nölscher, Anke C. and Sinha, Vinayak and Paasonen, Pauli and Petäjä, Tuukka and Sipilä, Mikko and Elste, Thomas and Plass-Dülmer, Christian and Phillips, Gavin J. and Kubistin, Dagmar and Williams, Jonathan and Vereecken, Luc and Lelieveld, Jos and Harder, Hartwig (2017) Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument. Atmospheric Chemistry and Physics, 17 (12). pp. 7807-7826. ISSN 1680-7324. doi:10.5194/acp-17-7807-2017. https://resolver.caltech.edu/CaltechAUTHORS:20170720-081829934
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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 ∼ 5.0 × 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 SO_2 into H_2SO_4. 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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| Additional Information: | © 2017 Author(s). This work is distributed under the Creative Commons Attribution 3.0 License. Published by Copernicus Publications on behalf of the European Geosciences Union. Received: 11 Oct 2016 – Discussion started: 24 Oct 2016. Revised: 02 May 2017 – Accepted: 19 May 2017 – Published: 29 Jun 2017. Luc Vereecken was supported by the Max Planck Graduate Centre (MPGC) with the Johannes Gutenberg-Universität Mainz. Work during HUMPPA-COPEC was supported by the Hyytiälä site engineers and staff. Support of the European Community Research Infrastructure Action under the FP6 ”Structuring the European Research Area” programme, EUSAAR contract no. RII3-CT-2006-026140, is gratefully acknowledged. The HUMPPACOPEC 2010 campaign measurements and analyses were supported by the ERC grant ATMNUCLE (project no. 227463), the Academy of Finland Centre of Excellence programme (project no. 1118615), the Academy of Finland Centre of Excellence in Atmospheric Science – From Molecular and Biological processes to The Global Climate (ATM, 272041), the European integrated project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI, project no. 036833-2), the EUSAAR TNA (project no. 400586), and the IMECC TA (project No. 4006261). The work during HOPE 2012 was supported by the scientists and staff of DWD Hohenpeißenberg, whom we would like to thank for providing the “platform” and opportunity to perform such a campaign. In particular, we thank Anja Werner, Jennifer Englert, and Katja Michl for the VOC measurements, Stephan Gilge for the trace gases measurements, and Georg Stange for running the CIMS. We also would like to thank Markus Rudolf for much technical support and guidance, Eric Regelin and Umar Javed for the numerous scientific discussions, Petri Keronen for providing meteorological and trace gas concentration data from Hyytiälä during the HUMPPA-COPEC 2010 and Thorsten Berndt for providing the data to re-evaluate the rate coefficient between SCIs and SO2. The article processing charges for this open-access publication were covered by the Max Planck Society. The authors declare that they have no conflict of interest. | ||||||||||||||||||
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| Issue or Number: | 12 | ||||||||||||||||||
| DOI: | 10.5194/acp-17-7807-2017 | ||||||||||||||||||
| Record Number: | CaltechAUTHORS:20170720-081829934 | ||||||||||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20170720-081829934 | ||||||||||||||||||
| Official Citation: | Novelli, A., Hens, K., Tatum Ernest, C., Martinez, M., Nölscher, A. C., Sinha, V., Paasonen, P., Petäjä, T., Sipilä, M., Elste, T., Plass-Dülmer, C., Phillips, G. J., Kubistin, D., Williams, J., Vereecken, L., Lelieveld, J., and Harder, H.: Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument, Atmos. Chem. Phys., 17, 7807-7826, https://doi.org/10.5194/acp-17-7807-2017, 2017 | ||||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||||
| ID Code: | 79235 | ||||||||||||||||||
| Collection: | CaltechAUTHORS | ||||||||||||||||||
| Deposited By: | Tony Diaz | ||||||||||||||||||
| Deposited On: | 20 Jul 2017 18:29 | ||||||||||||||||||
| Last Modified: | 15 Nov 2021 17:46 |
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