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

Y Kanai; A Tilocca; A Selloni; R Car

doi:10.1063/1.1773159

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

J Chem Phys. 2004 Aug 22;121(8):3359-67. doi: 10.1063/1.1773159.

Authors

Y Kanai¹, A Tilocca, A Selloni, R Car

Affiliation

¹ Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA.

PMID: 15303898
DOI: 10.1063/1.1773159

Abstract

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 H(2) on the reconstructed Si(100) surface.