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Abstract

We report a 2000-year Antarctic ice-core record of stable carbon isotope measurements in atmospheric methane (δ13CH4). Large δ13CH4 variations indicate that the methane budget varied unexpectedly during the late preindustrial Holocene (circa 0 to 1700 A.D.). During the first thousand years (0 to 1000 A.D.), δ13CH4 was at least 2 per mil enriched compared to expected values, and during the following 700 years, an about 2 per mil depletion occurred. Our modeled methane source partitioning implies that biomass burning emissions were high from 0 to 1000 A.D. but reduced by almost ∼40% over the next 700 years. We suggest that both human activities and natural climate change influenced preindustrial biomass burning emissions and that these emissions have been previously understated in late preindustrial Holocene methane budget research.

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References and Notes

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Even if LPIH variations in OH were as large as 10%, the weighted average fractionation of all sinks would only vary by ∼0.15‰, which is equivalent to δ13CH4 measurement uncertainty, and [CH4] would vary by ∼50 ppb, which is equivalent to observed [CH4] variability. The CO variations present in Fig. 4 over 0 to 1500 A.D. could cause OH abundance to vary by up to ∼10%. The 0.3°C temperature variations (Fig. 3) would cause a small change in the OH rate constant; however, δ13CH4 would vary by less than 0.01 and [CH4] would vary by ∼4 ppb.
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We thank the staff of the Australian Antarctic Program, especially Casey Station, for field support; A. Smith for firn-air sampling assistance; the Bureau of Meteorology (Australia) for Cape Grim archive-air collection assistance; R. Francey, P. Steele, C. Allison, and S. Coram at CSIRO for logistical and technical help; and especially B. Ruddiman and B. Allan for valuable discussions. Supported by NSF (grant no. OPP0087357); NOAA/Climate Modeling and Diagnostics Laboratory; NIWA, New Zealand (Foundation for Research Science and Technology grant no. C01X0204); and the Australian Government's Antarctic Climate and Ecosystems Cooperative Research Centre and CSIRO Atmospheric Research.

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Published In

Science
Volume 309 | Issue 5741
9 September 2005

Submission history

Received: 23 May 2005
Accepted: 28 July 2005
Published in print: 9 September 2005

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Notes

Supporting Online Material
www.sciencemag.org/cgi/content/full/309/5741/1714/DC1
Materials and Methods
References and Notes

Authors

Affiliations

D. F. Ferretti* [email protected]
Institute of Arctic and Alpine Research, University of Colorado, Boulder, CO 80309, USA.
National Institute of Water and Atmospheric Research Limited (NIWA), Post Office Box 14901, Wellington, New Zealand.
J. B. Miller
National Oceanic and Atmospheric Administration (NOAA), R/CMDL1, 325 Broadway, Boulder, CO 80305, USA.
J. W. C. White
Institute of Arctic and Alpine Research, University of Colorado, Boulder, CO 80309, USA.
D. M. Etheridge
Commonwealth Scientific and Industrial Research Organisation (CSIRO), Marine and Atmospheric Research, Private Bag 1, Aspendale, Victoria 3195, Australia.
K. R. Lassey
National Institute of Water and Atmospheric Research Limited (NIWA), Post Office Box 14901, Wellington, New Zealand.
D. C. Lowe
National Institute of Water and Atmospheric Research Limited (NIWA), Post Office Box 14901, Wellington, New Zealand.
C. M. MacFarling Meure
Commonwealth Scientific and Industrial Research Organisation (CSIRO), Marine and Atmospheric Research, Private Bag 1, Aspendale, Victoria 3195, Australia.
M. F. Dreier
Institute of Arctic and Alpine Research, University of Colorado, Boulder, CO 80309, USA.
C. M. Trudinger
Commonwealth Scientific and Industrial Research Organisation (CSIRO), Marine and Atmospheric Research, Private Bag 1, Aspendale, Victoria 3195, Australia.
T. D. van Ommen
Department of the Environment and Heritage, Australian Antarctic Division, and Antarctic Climate and Ecosystems CRC, Private Bag 80, Hobart, Tasmania 7001, Australia.
R. L. Langenfelds
Commonwealth Scientific and Industrial Research Organisation (CSIRO), Marine and Atmospheric Research, Private Bag 1, Aspendale, Victoria 3195, Australia.

Notes

*
To whom correspondence should be addressed. E-mail: [email protected]

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