Hydration of Clays at the Molecular Scale: The Promising Perspective of Classical Density Functional Theory
arXiv:1402.2581 · doi:10.1080/00268976.2014.899647
Abstract
We report here how the hydration of complex surfaces can be efficiently studied thanks to recent advances in classical molecular density functional theory. This is illustrated on the example of the pyrophylite clay. After presenting the most recent advances, we show that the strength of this implicit method is that (i) it is in quantitative or semi-quantitative agreement with reference all-atoms simulations (molecular dynamics here) for both the solvation structure and energetics, and that (ii) the computational cost is two to three orders of magnitude less than in explicit methods. The method remains imperfect, in that it locally overestimates the polarization of water close to hydrophylic sites of the clay. The high numerical efficiency of the method is illustrated and exploited to carry a systematic study of the electrostatic and van der Waals components of the surface-solvant interactions within the most popular force field for clays, CLAYFF. Hydration structure and energetics are found to weakly depend upon the electrostatics. We conclude on the consequences of such findings in future force-field development.
24 pages, 8 figures. Molecular Physics (2014)
References in corpus (4)
- Molecular Density Functional Theory of Water
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Cited by in corpus (4)
- Molecular density functional theory of water including density-polarization coupling
- Solvation in atomic liquids: connection between Gaussian field theory and density functional theory
- A molecular density functional theory to study solvation in water
- Solvatation de systèmes d'intérêt pharmaceutique : apports de la théorie de la fonctionnelle de la densité moléculaire