References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-12-8095-2012

Carbon and hydrogen isotopic ratios of atmospheric methane in the upper troposphere over the Western Pacific

Umezawa

¹ ⁵ Machida

² Ishijima

³ Matsueda

⁴ Sawa

⁴ Patra

P. K.

³ Aoki

¹ Nakazawa

Center for Atmospheric and Oceanic Studies, Graduate School of Science, Tohoku University, Sendai, Japan

National Institute for Environmental Studies, Tsukuba, Japan

Research Institute for Global Change, JAMSTEC, Yokohama, Japan

Meteorological Research Institute, Tsukuba, Japan

now at: Max Planck Institute for Chemistry, Mainz, Germany

10 09 2012

12 17 8095 8113

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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 imply that these areas have CH4 sources with relatively low δ13C and δD signatures such as 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 an additional contribution from 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 δ<D during 2007–2008 in the UT and LT over the Western Pacific, possibly due to enhanced biogenic emissions in the tropics and NH.

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