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Discussion papers | Copyright
https://doi.org/10.5194/acp-2018-645
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 12 Jul 2018

Research article | 12 Jul 2018

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Reactive quenching of electronically excited NO2* and NO3* by H2O as potential sources of atmospheric HOx radical

Terry J. Dillon1,a and John N. Crowley1 Terry J. Dillon and John N. Crowley
  • 1Max Planck Institute for Chemistry, Division of Atmospheric Chemistry, Mainz, Germany
  • anow at: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, UK

Abstract. Pulsed laser excitation of NO2 (532–647nm) or NO3 (623–662nm) in the presence of H2O was used to initiate the gas-phase reactions NO2*+H2O → products (R5) and NO3*+H2O → products (R12). No evidence for OH production in (R5) or (R12) was observed and upper-limits for OH production of k5b/k5<1×10−5 and k12b/k12<0.03 were assigned. The upper limit for k5b/k5 renders this reaction insignificant as a source of OH in the atmosphere and extends the studies (Crowley and Carl, 1997; Carr et al., 2009; Amedro et al., 2011) which demonstrate that the previously reported large OH yield by (Li et al., 2008) was erroneous. The upper limit obtained for k12b/k12 indicates that non-reactive energy transfer is the dominant mechanism for (R12), though generation of small but significant amounts of atmospheric HOx and HONO cannot be ruled out. In the course of this work, rate coefficients for overall removal of NO3* by N2 (R10) and by H2O (R12) were determined: k10=(2.1±0.1)×10−11cm3molecule−1s−1 and k12=(1.6±0.3)×10−10cm3molecule−1s−1 which is more than a factor of three smaller than one previously reported value.

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Terry J. Dillon and John N. Crowley
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