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Analyzing Melts and Fluids from Ab Initio Molecular Dynamics Simulations with the UMD Package

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Molecular correlations and solvation in simple fluids.

Marco A A Barbosa¹, B Widom

¹Department of Chemistry, Baker Laboratory, Cornell University, Ithaca, New York 14853-1301, USA.

The Journal of Chemical Physics

|June 10, 2010

Summary

This summary is machine-generated.

This study models low-solubility solutions, revealing that solute-solute attraction, driven by solvent interactions, explains low solubility and negative osmotic virial coefficients. Molecular correlations dictate solution thermodynamics.

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Area of Science:

Physical Chemistry
Statistical Mechanics
Solution Theory

Background:

Understanding molecular correlations is key to explaining solution thermodynamics, especially for low-solubility solutes.
Thermodynamic properties like osmotic virial coefficients are influenced by solute-solvent and solute-solute interactions.
Lattice models provide a framework for studying these interactions at a molecular level.

Purpose of the Study:

To investigate the molecular correlations in a lattice model of a low-solubility solute solution.
To elucidate how thermodynamic properties, such as the second osmotic virial coefficient, are reflected in correlation functions.
To analyze the relationship between solvation free energy and the potential of mean force between solute molecules.

Main Methods:

Utilized a lattice model for a solution of a low-solubility solute.
Employed the Bethe-Guggenheim approximation, exact on a Bethe lattice (Cayley tree).
Analyzed three pair correlation functions: h(11)(r), h(12)(r), and h(22)(r), in the limit of infinite dilution.

Main Results:

Identified a common exponential decay length for all three pair correlation functions.
Observed that for low solubility, the amplitude of h(22)(r) is significantly larger than h(12)(r) and h(11)(r).
Found a large, negative second osmotic virial coefficient, directly linked to a strong effective solute-solute attraction at contact.

Conclusions:

Low solute solubility is driven by a large, positive Gibbs free energy of solvation, resulting in strong solute-solute attraction.
The solvent-mediated part of the potential of mean force at contact is strongly negative, contributing to the negative second osmotic virial coefficient.
Unfavorable solvation enthalpy and entropy contribute to low solubility, distinct from the mechanism of the hydrophobic effect.