Towards an assessment of the accuracy of density functional theory for first principles simulations of water. II
10.1063/1.1782074
Crossref journal-article
AIP Publishing
The Journal of Chemical Physics (317)
Abstract

A series of 20 ps ab initio molecular dynamics simulations of water at ambient density and temperatures ranging from 300 to 450 K are presented. Car-Parrinello (CP) and Born-Oppenheimer (BO) molecular dynamics techniques are compared for systems containing 54 and 64 water molecules. At 300 K, an excellent agreement is found between radial distribution functions (RDFs) obtained with BO and CP dynamics, provided an appropriately small value of the fictitious mass parameter is used in the CP simulation. However, we find that the diffusion coefficients computed from CP dynamics are approximately two times larger than those obtained with BO simulations for T>400 K, where statistically meaningful comparisons can be made. Overall, both BO and CP dynamics at 300 K yield overstructured RDFs and slow diffusion as compared to experiment. In order to understand these discrepancies, the effect of proton quantum motion is investigated with the use of empirical interaction potentials. We find that proton quantum effects may have a larger impact than previously thought on structure and diffusion of the liquid.

Bibliography

Schwegler, E., Grossman, J. C., Gygi, F., & Galli, G. (2004). Towards an assessment of the accuracy of density functional theory for first principles simulations of water. II. The Journal of Chemical Physics, 121(11), 5400–5409.

Authors 4
  1. Eric Schwegler (first)
  2. Jeffrey C. Grossman (additional)
  3. François Gygi (additional)
  4. Giulia Galli (additional)
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Dates
Type When
Created 20 years, 11 months ago (Sept. 8, 2004, 11:55 a.m.)
Deposited 1 year, 6 months ago (Feb. 6, 2024, 8:36 p.m.)
Indexed 1 month ago (Aug. 2, 2025, 12:24 a.m.)
Issued 20 years, 11 months ago (Sept. 15, 2004)
Published 20 years, 11 months ago (Sept. 15, 2004)
Published Print 20 years, 11 months ago (Sept. 15, 2004)
Funders 0

None

@article{Schwegler_2004, title={Towards an assessment of the accuracy of density functional theory for first principles simulations of water. II}, volume={121}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.1782074}, DOI={10.1063/1.1782074}, number={11}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Schwegler, Eric and Grossman, Jeffrey C. and Gygi, François and Galli, Giulia}, year={2004}, month=sep, pages={5400–5409} }