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Preprints
https://doi.org/10.5194/acp-2020-360
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-360
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

  11 May 2020

11 May 2020

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A revised version of this preprint was accepted for the journal ACP and is expected to appear here in due course.

Evolution of NO3 reactivity during the oxidation of isoprene

Patrick Dewald1, Jonathan M. Liebmann1, Nils Friedrich1, Justin Shenolikar1, Jan Schuladen1, Franz Rohrer2, David Reimer2, Ralf Tillmann2, Anna Novelli2, Changmin Cho2, Kangming Xu3, Rupert Holzinger3, François Bernard4,a, Li Zhou4, Wahid Mellouki4, Steven S. Brown5,6, Hendrik Fuchs2, Jos Lelieveld1, and John N. Crowley1 Patrick Dewald et al.
  • 1Atmospheric Chemistry Department, Max Planck Institut für Chemie, 55128 Mainz, Germany
  • 2Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, 52428 Jülich, Germany
  • 3Institute for Marine and Atmospheric Research, IMAU, Utrecht University, Utrecht, Netherlands
  • 4Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), CNRS (UPR 3021)/OSUC, 1C Avenue de la Recherche Scientifique, 45071 Orléans CEDEX 2, France
  • 5NOAA Chemical Sciences Laboratory, 325 Broadway, Boulder, CO 80305, USA
  • 6Department of Chemistry, University of Colorado, Boulder, CO 80209, USA
  • anow at: Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Centre National de la Recherche Scientifique (CNRS), Université d'Orléans, Observatoire des Sciences de l’Univers en région Centre – Val de Loire (OSUC), Orléans, France

Abstract. In a series of experiments in an atmospheric simulation chamber (SAPHIR, Forschungszentrum Jülich, Germany) NO3 reactivity (kNO3) resulting from the reaction of NO3 with isoprene and stable trace gases formed as products was measured directly using a flow-tube reactor coupled to a cavity-ring-down spectrometer (FT-CRDS). The experiments were carried out in both dry and humid air with variation of the initial mixing ratios of ozone (50–100 ppbv), isoprene (3–22 ppbv) and NO2 (5–30 ppbv). kNO3 was in excellent agreement with values calculated from the isoprene mixing ratio and the rate coefficient for the reaction of NO3 with isoprene. This result serves both to confirm that the FT-CRDS returns accurate values of kNO3 even at elevated NO2 concentrations and to show that reactions of NO3 with stable reaction products like non-radical organic nitrates do not contribute significantly to NO3 reactivity during the oxidation of isoprene. A comparison of kNO3 with NO3 reactivities calculated from NO3 mixing ratios and NO3 production rates suggests that organic peroxy radicals and HO2 account for ~ 50 % of NO3 losses. This contradicts predictions based on numerical simulations using the Master Chemical Mechanism (MCM version 3.3.1) unless the rate coefficient for reaction between NO3 and isoprene-derived RO2 is roughly doubled to ≈ 5 × 10−12 cm3 molecule−1 s−1.

Patrick Dewald et al.

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Patrick Dewald et al.

Patrick Dewald et al.

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Latest update: 07 Aug 2020
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Short summary
We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from unstationary-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account for ~ 50 % of overall NO3 losses.
We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3...
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