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Structure and Dynamics of Liquid Water from ab Initio Molecular DynamicsComparison of BLYP, PBE, and revPBE Density Functionals with and without van der Waals Corrections
Ist Teil von
Journal of chemical theory and computation, 2012-10, Vol.8 (10), p.3902-3910
Ort / Verlag
United States: American Chemical Society
Erscheinungsjahr
2012
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
We investigate the accuracy provided by different treatments of the exchange and correlation effects, in particular the London dispersion forces, on the properties of liquid water using ab initio molecular dynamics simulations with density functional theory. The lack of London dispersion forces in generalized gradient approximations (GGAs) is remedied by means of dispersion-corrected atom-centered potentials (DCACPs) or damped atom-pairwise dispersion corrections of the C 6 R –6 form. We compare results from simulations using GGA density functionals (BLYP, PBE, and revPBE) with data from their van der Waals (vdW) corrected counterparts. As pointed out previously, all vdW-corrected BLYP simulations give rise to highly mobile water whose softened structure is closer to experimental data than the one predicted by the bare BLYP functional. Including vdW interactions in the PBE functional, on the other hand, has little influence on both structural and dynamical properties of water. Augmenting the revPBE functional with either damped atom-pairwise dispersion corrections or DCACP evokes opposite behaviors. The former further softens the already under-structured revPBE water, whereas the latter makes it more glassy. These results demonstrate the delicacy needed in describing weak interactions in molecular liquids.
Sprache
Englisch
Identifikatoren
ISSN: 1549-9618
eISSN: 1549-9626
DOI: 10.1021/ct3001848
Titel-ID: cdi_proquest_miscellaneous_1735908942
Format
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