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Atmospheric Measurement Techniques An interactive open-access journal of the European Geosciences Union
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Volume 9, issue 3
Atmos. Meas. Tech., 9, 1095–1111, 2016
https://doi.org/10.5194/amt-9-1095-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
Atmos. Meas. Tech., 9, 1095–1111, 2016
https://doi.org/10.5194/amt-9-1095-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 18 Mar 2016

Research article | 18 Mar 2016

Global stratospheric measurements of the isotopologues of methane from the Atmospheric Chemistry Experiment Fourier transform spectrometer

Eric M. Buzan1, Chris A. Beale2, Chris D. Boone3, and Peter F. Bernath1,3 Eric M. Buzan et al.
  • 1Department of Chemistry and Biochemistry, Old Dominion University, Norfolk, Virginia, USA
  • 2Department of Ocean, Earth, and Atmospheric Sciences, Old Dominion University, Norfolk, Virginia, USA
  • 3Department of Chemistry, University of Waterloo, Waterloo, Ontario, Canada

Abstract. This paper presents an analysis of observations of methane and its two major isotopologues, CH3D and 13CH4, from the Atmospheric Chemistry Experiment (ACE) satellite between 2004 and 2013. Additionally, atmospheric methane chemistry is modeled using the Whole Atmospheric Community Climate Model (WACCM). ACE retrievals of methane extend from 6 km for all isotopologues to 75 km for 12CH4, 35 km for CH3D, and 50 km for 13CH4. While total methane concentrations retrieved from ACE agree well with the model, values of δD–CH4 and δ13C–CH4 show a bias toward higher δ compared to the model and balloon-based measurements. Errors in spectroscopic constants used during the retrieval process are the primary source of this disagreement. Calibrating δD and δ13C from ACE using WACCM in the troposphere gives improved agreement in δD in the stratosphere with the balloon measurements, but values of δ13C still disagree. A model analysis of methane's atmospheric sinks is also performed.

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This paper presents the first global data set of atmospheric concentrations of the isotopologues of methane as measured by ACE-FTS. Both CH3D and 13CH4 show enrichment at higher altitudes and some seasonal variation at the poles. After applying a constant correction factor to the CH3D data set, good agreement with existing balloon measurements is achieved. However, 13CH4 still shows a large amount of error. Improved lab measurements of CH4 would help reduce errors in the ACE-FTS data.
This paper presents the first global data set of atmospheric concentrations of the isotopologues...
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