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First-principles string molecular dynamics: An efficient approach for finding chemical reaction pathways

J. Chem. Phys. 121, 3359 (2004); doi:10.1063/1.1773159

Issue Date: 22 August 2004

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Y. Kanai, A. Tilocca, and A. Selloni
Department of Chemistry, Princeton University, Princeton, New Jersey 08544

R. Car
Department of Chemistry, Princeton University, Princeton, New Jersey 08544
Princeton Institute for the Science and Technology of Materials (PRISM), Princeton, New Jersey 08544
A recently proposed approach, called "string method," allows us to find minimum energy pathways connecting two metastable states of a system [W. E et al., Phys. Rev. B 66, 052301 (2002)]. So far this approach has been only used with empirical force field parametrizations of the atomic potential energy surface or in the context of macroscopic continuum models. Here we show that the string method can be efficiently combined with first-principles molecular dynamics to provide an accurate description of chemical reaction pathways and barriers. We illustrate the first-principles string molecular dynamics by applying it to the study of a surface chemical reaction, for which extensive experimental and theoretical works are available, namely, the adsorption of H2 on the reconstructed Si(100) surface. ©2004 American Institute of Physics.
History: Received 9 April 2004; accepted 24 May 2004
Permalink: http://link.aip.org/link/?JCPSA6/121/3359/1
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KEYWORDS and PACS

Keywords
PACS
  • 68.43.Mn
    Adsorption/desorption kinetics
  • 68.35.Bs
    Structure of clean solid surfaces (reconstruction)
  • 82.65.+r
    Surface and interface chemistry; heterogeneous catalysis at surfaces
  • YEAR: 2004

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ISSN:
0021-9606 (print)   1089-7690 (online)
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