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Science 24 December 2004:
Vol. 306. no. 5705, pp. 2227 - 2229
DOI: 10.1126/science.1104085
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Reports

First-Principles Theory for the H + CH4 -> H2 + CH3 Reaction

Tao Wu,1* Hans-Joachim Werner,2 Uwe Manthe3,1{dagger}

A full-dimensional quantum dynamics simulation of a hydrogen atom reacting with methane on an accurate ab initio potential energy surface is reported. Based on first-principles theory, thermal rate constants are predicted with an accuracy comparable to (or even exceeding) experimental precision. The theoretical prediction is within the range of the significantly varied experimental rate constants reported by different groups. This level of accuracy has previously been achieved only for smaller, three-or four-atom reactive systems. Comparison with classical transition state theory confirms the importance of quantum mechanical tunneling for the rate constant below 400 kelvin.

1 Theoretische Chemie, Technische Universität München, Lichtenbergstrasse 4, 85747 Garching, Germany.
2 Institut für Theoretische Chemie, Universität Stuttgart, Pfaffenwaldring 55, 70569 Stuttgart, Germany.
3 Theoretische Chemie, Fakultät für Chemie, Universität Bielefeld, Postfach 100131, 33501 Bielefeld, Germany.



* Present address: Department of Chemistry, Zhejiang University, Hangzhou, 310027, China.

{dagger} To whom correspondence should be addressed. E-mail: uwe.manthe{at}uni-bielefeld.de

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