Publication

Soft-Sphere Continuum Solvation in Electronic-Structure Calculations

Résumé

We present an implicit solvation approach where the interface-between the quantum-mechanical solute and the surrounding environment is, described by a fully continuous permittivity built up with atomic-centered "soft" spheres. This approach combines many of-the advantages the self-consistent continuum solvation model, in-handling solutes and surfaces in contact with complex dielectric environments or electrolytes in electronic-structure calculations. In addition it is able to describe accurately both neutral and charged systems. The continuous function, describing the variation of the permittivity, allows, to compute analytically the nonelectrostatic contributions to the solvation free energy that are described in terms of the quantum surface. The whole methodology is computationally stable, provides consistent energies and forces, and keeps the computational efforts and runtimes comparable to those of standard vacuum calculations. The capability to treat arbitrary molecular or slab-like geometries as well as charged Molecules is key to tackle electrolytes within mixed frameworks. We show that, with given, fixed atomic radii, two parameters are sufficient to give a mean absolute error of only 1.12 kcal/mol with respect to the experimental aqueous solvation energies for a set of 274 neutral solutes. For charged systems, the same set of parameters provides solvation energies for a set of 60 anions and 52 cations with an error of 2.96 and 2.13 kcal/mol, respectively, improving upon previous literature values. To tackle elements not present in most solvation databases, a new benchmark scheme On wettability and contact angles is proposed for solid-liquid interfaces and applied to the investigation of the stable terminations of a CdS (11 (2) over bar0) surface in an electrochemical medium.

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Concepts associés (40)
Implicit solvation
Implicit solvation (sometimes termed continuum solvation) is a method to represent solvent as a continuous medium instead of individual “explicit” solvent molecules, most often used in molecular dynamics simulations and in other applications of molecular mechanics. The method is often applied to estimate free energy of solute-solvent interactions in structural and chemical processes, such as folding or conformational transitions of proteins, DNA, RNA, and polysaccharides, association of biological macromolecules with ligands, or transport of drugs across biological membranes.
Relative permittivity
The relative permittivity (in older texts, dielectric constant) is the permittivity of a material expressed as a ratio with the electric permittivity of a vacuum. A dielectric is an insulating material, and the dielectric constant of an insulator measures the ability of the insulator to store electric energy in an electrical field. Permittivity is a material's property that affects the Coulomb force between two point charges in the material. Relative permittivity is the factor by which the electric field between the charges is decreased relative to vacuum.
Solvatation
vignette|Un ion sodium solvaté par des molécules d'eau. La solvatation est le phénomène physico-chimique observé lors de la dissolution d'une substance chimique dans un solvant. Lors de l'introduction d'une espèce chimique initialement à l'état solide (sous forme de cristal ou amorphe), liquide ou gazeux dans un solvant, les atomes, ions ou molécules de l'espèce chimique se dispersent dans la solution et interagissent avec les molécules de solvant. Cette interaction s'appelle la solvatation.
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