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Journal of Chemical Physics / Volume 122 / Issue 1 / ARTICLES / Condensed Phase Dynamics, Structure, and Thermodynamics: Spectroscopy, Reactions, and Relaxation

J. Chem. Phys. 122, 014515 (2005); http://dx.doi.org/10.1063/1.1828433 (6 pages)

The influence of temperature and density functional models in ab initio molecular dynamics simulation of liquid water

Joost VandeVondele1, Fawzi Mohamed2, Matthias Krack2, Jürg Hutter3, Michiel Sprik1, and Michele Parrinello2

1Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom
2Laboratory of Physical Chemistry, ETH Zurich, USI-Campus, Via Giuseppe Buffi 13, CH-6904 Lugano, Switzerland
3Physical Chemistry Institute, University of Zurich, Winterthurerstrasse 190, CH-8057 Zurich, Switzerland

(Received 29 July 2004; accepted 12 October 2004; published online 15 December 2004)

The performance of density functional theory methods for the modeling of condensed aqueous systems is hard to predict and validation by ab initio molecular simulation of liquid water is absolutely necessary. In order to assess the reliability of these tests, the effect of temperature on the structure and dynamics of liquid water has been characterized with 16 simulations of 20 ps in the temperature range of 280–380 K. We find a pronounced influence of temperature on the pair correlation functions and on the diffusion constant including nonergodic behavior on the time scale of the simulation in the lower temperature range (which includes ambient temperature). These observations were taken into account in a consistent comparison of a series of density functionals (BLYP, PBE, TPSS, OLYP, HCTH120, HCTH407). All simulations were carried out using an ab initio molecular dynamics approach in which wave functions are represented using Gaussians and the density is expanded in an auxiliary basis of plane waves. Whereas the first three functionals show similar behavior, it is found that the latter three functionals yield more diffusive dynamics and less structure.© 2005 American Institute of Physics.

© 2005 American Institute of Physics

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KEYWORDS and PACS

Keywords

liquid theory, diffusion, water, ab initio calculations, molecular dynamics method, density functional theory, wave functions

PACS

  • 61.20.Ja

    Computer simulation of liquid structure

  • 66.10.C-

    Diffusion and thermal diffusion

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.1828433

PUBLICATION DATA

ISSN

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

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

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