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Discussion papers | Copyright
https://doi.org/10.5194/acp-2017-1233
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 08 Feb 2018

Research article | 08 Feb 2018

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This discussion paper is a preprint. A revision of this manuscript was accepted for the journal Atmospheric Chemistry and Physics (ACP) and is expected to appear here in due course.

Mercury distribution in the upper troposphere and lower most stratosphere according to measurements by the IAGOS-CARIBIC observatory, 2014–2016

Franz Slemr1, Andreas Weigelt2,a, Ralf Ebinghaus2, Johannes Bieser2, Carl A. M. Brenninkmeijer1, Armin Rauthe-Schöch1,b, Markus Hermann3, Bengt G. Martinsson4, Peter van Velthoven5, Harald Bönisch6, Marco Neumaier6, Andreas Zahn6, and Helmut Ziereis7 Franz Slemr et al.
  • 1Max-Planck-Institut für Chemie (MPI), Air Chemistry Division, Hahn-Meitner-Weg 1, D-55128 Mainz, Germany
  • 2Helmholtz-Zentrum Geesthacht (HZG), Institute of Coastal Research, Max-Planck-Str. 1, D-21502 Geesthacht, Germany
  • 3Leibniz-Institut für Troposphärenforschung (Tropos), Permoserstr. 15, D-04318 Leipzig, Germany
  • 4University of Lund, Division of Nuclear Physics, P.O. Box 118, S-22100 Lund, Sweden
  • 5Royal Netherlands Meteorological Institute (KNMI), P.O. Box 201, NL-3730 AE, de Bilt, the Netherlands
  • 6Institute of Meteorology and Climate Research (IMK), Karlsruhe Institute of Technology, Hermann-von-Helmholtz-Platz, D-76344 Eggenstein-Leopoldshafen
  • 7Deutsches Zentrum für Luft- und Raumfahrt (DLR), Institut für Physik der Atmosphäre, D-82230 Wessling, Germany
  • anow at: Bundesamt für Seeschifffahrt und Hydrographie (BSH), Wüstland 2, D-22589 Hamburg, Germany
  • bnow at: Deutscher Wetterdienst, Global Precipitation Climatology Centre, Frankfurter Straße 135, 63067 Offenbach/Main, Germany

Abstract. Mercury was measured onboard the IAGOS-CARIBIC passenger aircraft since May 2005 until February 2016 during nearly monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa, and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data.

Elevated upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Using speciation experiments, we show that nearly identical TM and gaseous elementary mercury (GEM) concentrations exist at and below the tropopause. Above the thermal tropopause GEM concentrations are almost always smaller than those of TM and the TMGEM (i.e. Hg2+) difference increases up to ~40% of TM at ~2km and more above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72±37 and 74±27yr for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation, and cloud scavenging processes.

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Franz Slemr et al.
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Short summary
Total and elemental mercury were measured in the upper troposphere and lower stratosphere onboard a passenger aircraft. Their concentrations in the upper troposphere were comparable implying low concentrations of oxidized mercury in this region. Large scale seasonally dependent influence of emissions from biomass burning was also observed. Their distributions in the lower stratosphere implies a long stratospheric lifetime which precludes significant mercury oxidation by ozone.
Total and elemental mercury were measured in the upper troposphere and lower stratosphere...
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