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Interlaboratory comparison of δ13C and δd measurements of atmospheric CH4 for combined use of data sets from different laboratories

  • Taku Umezawa*
  • , Carl A.M. Brenninkmeijer
  • , Thomas Röckmann
  • , Carina van der Veen
  • , Stanley C. Tyler
  • , Ryo Fujita
  • , Shinji Morimoto
  • , Shuji Aoki
  • , Todd Sowers
  • , Jochen Schmitt
  • , Michael Bock
  • , Jonas Beck
  • , Hubertus Fischer
  • , Sylvia E. Michel
  • , Bruce H. Vaughn
  • , John B. Miller
  • , James W.C. White
  • , Gordon Brailsford
  • , Hinrich Schaefer
  • , Peter Sperlich
  • Willi A. Brand, Michael Rothe, Thomas Blunier, David Lowry, Rebecca E. Fisher, Euan G. Nisbet, Andrew L. Rice, Peter Bergamaschi, Cordelia Veidt, Ingeborg Levin
*Corresponding author for this work
  • Max Planck Institute for Chemistry
  • National Institute for Environmental Studies of Japan
  • University of California at Irvine
  • Norco College
  • Tohoku University
  • National Institute of Polar Research
  • Pennsylvania State University
  • University of Bern
  • University of Colorado Boulder
  • NIWA
  • Max Planck Institute for Biogeochemistry
  • University of Copenhagen
  • Royal Holloway University of London
  • Portland State University
  • European Commission Joint Research Centre Institute
  • Heidelberg University 

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

We report results from a worldwide interlaboratory comparison of samples among laboratories that measure (or measured) stable carbon and hydrogen isotope ratios of atmospheric CH4 (δ13C-CH4 and δD-CH4). The offsets among the laboratories are larger than the measurement reproducibility of individual laboratories. To disentangle plausible measurement offsets, we evaluated and critically assessed a large number of intercomparison results, some of which have been documented previously in the literature. The results indicate significant offsets of δ13C-CH4 and δD-CH4 measurements among data sets reported from different laboratories; the differences among laboratories at modern atmospheric CH4 level spread over ranges of 0.5 % for δ13C-CH4 and 13 % for δD-CH4. The intercomparison results summarized in this study may be of help in future attempts to harmonize δ13C-CH4 and δD-CH4 data sets from different laboratories in order to jointly incorporate them into modelling studies. However, establishing a merged data set, which includes δ13C-CH4 and δD-CH4 data from multiple laboratories with desirable compatibility, is still challenging due to differences among laboratories in instrument settings, correction methods, traceability to reference materials and long-term data management. Further efforts are needed to identify causes of the interlaboratory measurement offsets and to decrease those to move towards the best use of available δ13C-CH4 and δD-CH4 data sets.

Original languageEnglish
Pages (from-to)1207-1231
Number of pages25
JournalAtmospheric Measurement Techniques
Volume11
Issue number2
DOIs
Publication statusPublished - 2 Mar 2018

Funding

1Max Planck Institute for Chemistry, Atmospheric Chemistry Department, 55128 Mainz, Germany 2Center for Environmental Measurement and Analysis, National Institute for Environmental Studies, Tsukuba 305-8506, Japan 3Institute for Marine and Atmospheric research Utrecht, Utrecht University, Utrecht, the Netherlands 4Earth System Science Department, University of California, Irvine, USA 5Chemistry Department, Norco College, Norco, CA 92860, USA 6Center for Atmospheric and Oceanic Studies, Graduate School of Science, Tohoku University, Sendai, Japan 7National Institute of Polar Research, Tokyo, Japan 8The Earth and Environmental Systems Institute, Pennsylvania State University, University Park, Pennsylvania 16802, USA 9Climate and Environmental Physics, Physics Institute and Oeschger Center for Climate Change Research, University of Bern, 3012 Bern, Switzerland 10Institute of Arctic and Alpine Research, University of Colorado Boulder, Boulder, Colorado, USA 11National Institute of Water and Atmospheric Research, Wellington 6021, New Zealand 12Max Planck Institute for Biogeochemistry, 07745 Jena, Germany 13Centre for Ice and Climate, University of Copenhagen, Copenhagen, Denmark 14Department of Earth Sciences, Royal Holloway, University of London, Egham, UK 15Department of Physics, Portland State University, Portland, OR 97207, USA 16European Commission Joint Research Centre, Institute for Environment and Sustainability, Ispra (Va), Italy 17Institute for Environmental Physics, Heidelberg University, 69120 Heidelberg, Germany Acknowledgements. We thank Morimasa Sato for measurements at TU. We thank Owen Sherwood for his contribution in setting up the INSTAAR measurement system and Ken Masarie and John Mund, who developed software enabling data comparisons from co-located samples measured by INSTAAR, RHUL and NIWA. We thank Paul Quay (UW) for isotopic CH4 data and intercalibration information and Doaa Teama for isotopic measurements at PDX. We thank Célia Sapart for helpful information about the past intercomparison. Part of this work at NIES was supported by the Environment Research and Technology Development Fund (2-1710) of the Ministry of the Environment, Japan and Environmental Restoration and Conservation Agency. Funding for work at PDX was provided by the US National Science Foundation (Atmospheric and Geospace Sciences Grant 0952307). CH4 isotope ice core work at UB received funding from the European Research Council under the European Union’s Seventh Framework Programme (FP7/2007-2013) ERC grant agreement no. 226172 and the Swiss National Science Foundation (grant no. 200020_159563 & 20020_172506). NIWA’s isotope measurements are funded under the Climate and Atmosphere Research Programme CAAC1804 (2017/18 SCI). We are grateful to the referee Sergey Assonov and one anonymous referee for their insightful and constructive comments for improving this paper.

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