Atmos. Chem. Phys. Discuss., 12, 9035-9077, 2012
www.atmos-chem-phys-discuss.net/12/9035/2012/
doi:10.5194/acpd-12-9035-2012
© Author(s) 2012. This work is distributed
under the Creative Commons Attribution 3.0 License.
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Carbon and hydrogen isotopic ratios of atmospheric methane in the upper troposphere over the Western Pacific
T. Umezawa1,*, T. Machida2, K. Ishijima3, H. Matsueda4, Y. Sawa4, P. K. Patra3, S. Aoki1, and T. Nakazawa1
1Center for Atmospheric and Oceanic Studies, Graduate School of Science, Tohoku University, Sendai, Japan
2National Institute for Environmental Studies, Tsukuba, Japan
3Japan Agency for Marine-Earth Science and Technology, Yokohama, Japan
4Meteorological Research Institute, Tsukuba, Japan
*now at: Max Planck Institute for Chemistry, Mainz, Germany

Abstract. We present the mixing ratio, δ13C and δD of atmospheric CH4 using commercial aircraft in the upper troposphere (UT) over the Western Pacific for the period December 2005–September 2010. The observed results were compared with those obtained using commercial container ships in the lower troposphere (LT) over the same region. In the Northern Hemisphere (NH), the UT CH4 mixing ratio shows high values in the boreal summer–autumn, when the LT CH4 mixing ratio reaches a seasonal minimum. From tagged tracer experiments made using an atmospheric chemistry transport model, we found that such high CH4 values are due to rapid transport of air masses influenced by CH4 sources in South Asia and East Asia. The observed isotopic ratio data suggest that CH4 sources in these areas have relatively low δ13C and δD signatures, implying biogenic sources. Latitudinal distributions of the annual average UT and LT CH4 mixing ratio intersect each other in the tropics; the mixing ratio value is lower in the UT than in the LT in the NH and the situation is reversed in the Southern Hemisphere (SH), due mainly to the NH air intrusion into the SH through the UT. Such intersection of the latitudinal distributions is observable in δD but not in δ13C, implying additional contribution of a reaction of CH4 with active chlorine in the marine boundary layer. δ13C and δD show low values in the NH and high values in the SH both in the UT and in the LT. We also observed an increase in the CH4 mixing ratio and decreases in δ13C and δD during 2007–2008 in the UT and LT over the Western Pacific, possibly due to enhanced biogenic emissions in the tropics and NH.

Citation: Umezawa, T., Machida, T., Ishijima, K., Matsueda, H., Sawa, Y., Patra, P. K., Aoki, S., and Nakazawa, T.: Carbon and hydrogen isotopic ratios of atmospheric methane in the upper troposphere over the Western Pacific, Atmos. Chem. Phys. Discuss., 12, 9035-9077, doi:10.5194/acpd-12-9035-2012, 2012.
 
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