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Discussion papers | Copyright
https://doi.org/10.5194/acp-2018-324
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 05 Apr 2018

Research article | 05 Apr 2018

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

Direct measurements of NO3-reactivity in and above the boundary layer of a mountain-top site: Identification of reactive trace gases and comparison with OH-reactivity

Jonathan M. Liebmann1, Jennifer B. A. Muller2, Dagmar Kubistin2, Anja Claude2, Robert Holla2, Christian Plaß-Dülmer2, Jos Lelieveld1, and John N. Crowley1 Jonathan M. Liebmann et al.
  • 1Atmospheric Chemistry Department, Max Planck Institut für Chemie, 55128, Mainz, Germany
  • 2Meteorologisches Observatorium Hohenpeissenberg, Deutscher Wetterdienst, 82383, Hohenpeissenberg, Germany

Abstract. We present direct measurements of the summertime, total reactivity of NO3 towards organic trace gases, kOTGNO3, at a rural mountain site (988ma.s.l.) in southern Germany in 2017. The diel cycle of kOTGNO3 was strongly influenced by local meteorology with reactivity high during the day (values of up to 0.3s-1) but usually close to the detection limit (0.005s-1) at night when the measurement site was in the residual layer/free troposphere. Daytime values of kOTGNO3 were sufficiently large that the loss of NO3 due to reaction with organic trace gases competed with its photolysis and reaction with NO. Within experimental uncertainty, monoterpenes and isoprene accounted for all of the measured NO3-reactivity. Averaged over the daylight hours, more than 25% of NO3 was removed via reaction with biogenic volatile organic compounds (BVOCs), implying a significant daytime loss of NOx and formation of organic nitrates due to NO3 chemistry. Ambient NO3 concentrations were measured on one night and were comparable to those derived from a stationary state calculation using measured values of kOTGNO3. We present and compare the first simultaneous, direct-reactivity measurements for the NO3 and OH radicals. The decoupling of the measurement site from ground level emissions resulted in lower reactivity at night for both radicals, though the correlation between OH- and NO3-reactivity was weak as would be anticipated given their divergent trends in rate constants with many organic trace gases.

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We present direct measurements of the summertime, total reactivity (inverse lifetime) of NO3 towards organic trace gases, at a rural mountain site. High day-time and low night-time values were found. The reactivity was dominated by reaction with monoterpenes and sufficiently high to compete with photolysis and reaction with NO during day-time. NO3 radical measurements from one night are presented. For the first time direct measurements of OH- and NO3-reactivity are compared.
We present direct measurements of the summertime, total reactivity (inverse lifetime) of NO3...
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