相关论文: Predicting Solvation Free Energies and Thermodynam…
The structure of polar liquids and electrolytic solutions, such as water and aqueous electrolytes, at interfaces underlies numerous phenomena in physics, chemistry, biology, and engineering. In this work, we develop a continuum theory that…
Aqueous solid-liquid interfaces (SLI) are ubiquitous in nature and technology, often hosting molecular-level processes with macroscopic consequences. Molecular dynamics (MD) simulations offer a tool of choice to investigate interfacial…
The predictive electrolyte model COSMO-RS-ES is refined to improve the description of systems at 25{\deg}C in which strong ion pairing is expected due to a low static permittivity of the liquid phase. Furthermore, the short-range ion energy…
Treating water as a linearly responding dielectric continuum on molecular length scales allows very simple estimates of solvation structure and thermodynamics for charged and polar solutes. While this approach can successfully account for…
Recent molecular simulation and integral equation results alkali-halide ion pair potentials-of-mean-force in water are discussed. Dielectric model calculations are implemented to check that these models produce that characteristic structure…
Solvation free energy is an important design parameter in reaction kinetics and separation processes, making it a critical property to predict during process development. In previous research, directed message passing neural networks…
The dielectric properties of molecules or nanostructures are usually modified in a complex manner, when assembled into a condensed phase. We propose a first-principles method to compute polarizabilities of sub-entities of solids and…
We construct a mean-field formulation of the thermodynamics of ion solvation in immiscible polar binary mixtures. Assuming an equilibrium planar interface separating two semi-infinite regions of different constant dielectric medium, we…
Dipolar susceptibility of interfacial water and the corresponding interface dielectric constant were calculated from numerical molecular dynamics simulations for neutral and charged states of buckminsterfullerene C$_{60}$. Dielectric…
We define the dielectric constant (susceptibility) that should enter the Maxwell boundary value problem when applied to microscopic dielectric interfaces. The dielectric constant (susceptibility) of the interface is defined by exact…
Using molecular dynamics simulations and methods of importance sampling, we study the thermodynamics and dynamics of sodium chloride in the aqueous premelting layer formed spontaneously at the interface between ice and its vapor. We uncover…
The accurate prediction of solvation free energies is critical for understanding various phenomena in the liquid phase, including reaction rates, equilibrium constants, activity coefficients, and partition coefficients. Despite extensive…
This paper tests a dielectric model for variation of hydration free energy with geometry of complex solutes in water. It works out some basic aspects of the theory of boundary integral methods for these problems. One aspect of the…
Inferring properties of macroscopic solutions from molecular simulations is complicated by the limited size of systems that can be feasibly examined with a computer. When long-ranged electrostatic interactions are involved, the resulting…
Continuum solvation models enable electronic structure calculations of systems in liquid environments, but because of the large number of empirical parameters, they are limited to the class of systems in their fit set (typically organic…
Implicit solvation is an effective, highly coarse-grained approach in atomic-scale simulations to account for a surrounding liquid electrolyte on the level of a continuous polarizable medium. Originating in molecular chemistry with finite…
The interface between the vapor and liquid phase of quadrupolar-dipolar fluids is the seat of an electric interfacial potential whose influence on ion solvation and distribution is not yet fully understood. To obtain further microscopic…
A dielectric model of electrostatic solvation is applied to describe potentials of mean force in water along reaction paths for: a) formation of a sodium chloride ion pair; b) the symmetric SN2 exchange of chloride in methylchloride; and c)…
The thesis focuses on the prediction of solvation thermodynamics using integral equation theories. Our main goal is to improve the approach using a rational correction. We achieve it by extending recently introduced pressure correction, and…
In this thesis, we develop a simple model potential for polar molecules that effectively and accurately represents the thermodynamics of dilute gases. This potential models dipolar interactions, with a nonpolar spherical component, as seen…