Extreme deuterium enrichment in stratospheric hydrogen and the global atmospheric budget of H2

Thom Rahn (), John M. Eiler, Kristie A. Boering, Paul O. Wennberg, Michael C. McCarthy, Stanley Tyler, Sue Schauffler, Stephen Donnelly and Elliot Atlas
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Thom Rahn: California Institute of Technology
John M. Eiler: California Institute of Technology
Kristie A. Boering: University of California at Berkeley
Paul O. Wennberg: California Institute of Technology
Michael C. McCarthy: University of California at Berkeley
Stanley Tyler: University of California, Irvine
Sue Schauffler: National Center for Atmospheric Research
Stephen Donnelly: National Center for Atmospheric Research
Elliot Atlas: National Center for Atmospheric Research

Nature, 2003, vol. 424, issue 6951, 918-921

Abstract: Abstract Molecular hydrogen (H2) is the second most abundant trace gas in the atmosphere after methane1 (CH4). In the troposphere, the D/H ratio of H2 is enriched by 120‰ relative to the world's oceans2,3,4. This cannot be explained by the sources of H2 for which the D/H ratio has been measured to date (for example, fossil fuels and biomass burning)5,6. But the isotopic composition of H2 from its single largest source—the photochemical oxidation of methane—has yet to be determined. Here we show that the D/H ratio of stratospheric H2 develops enrichments greater than 440‰, the most extreme D/H enrichment observed in a terrestrial material. We estimate the D/H ratio of H2 produced from CH4 in the stratosphere, where production is isolated from the influences of non-photochemical sources and sinks, showing that the chain of reactions producing H2 from CH4 concentrates D in the product H2. This enrichment, which we estimate is similar on a global average in the troposphere, contributes substantially to the D/H ratio of tropospheric H2.

Date: 2003
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DOI: 10.1038/nature01917

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