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Entropy and Solvation

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Solvent cavitation under solvophobic confinement.

Henry S Ashbaugh1

  • 1Department of Chemical and Biomolecular Engineering, Tulane University, New Orleans, Louisiana 70118, USA. hanka@tulane.edu

The Journal of Chemical Physics
|August 17, 2013
PubMed
Summary

Confinement-mediated evaporation stabilizes biomolecular assemblies. This study quantitatively validates thermodynamic theory for solvophobic confinement using 2D simulations, revealing length-dependent forces and evaporation critical separations.

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Area of Science:

  • Thermodynamics
  • Soft Matter Physics
  • Interfacial Science

Background:

  • Liquid stability can shift towards vapor phase under solvophobic confinement, inducing attractive forces between surfaces.
  • Confinement-mediated evaporation is crucial for stabilizing biomolecular and colloidal assemblies, particularly water near hydrophobic surfaces.
  • Macroscopic thermodynamic theory connects confining surface size, interfacial energies, and pressure to cavitation and forces.

Purpose of the Study:

  • To quantitatively validate macroscopic thermodynamic theory of cavitation under confinement.
  • To investigate the length dependence of solvation free energy and its impact on forces and evaporation.
  • To bridge the gap between molecular simulations and theoretical predictions for solvophobic confinement.

Main Methods:

  • Simulated a two-dimensional Lennard-Jones fluid confined between solvophobic plates.
  • Calculated forces and liquid-vapor coexistence properties across various plate sizes and pressures.
  • Accounted for the length dependence of solvation free energy for confining plates.

Main Results:

  • Simulations quantitatively agreed with theoretical predictions for solvent-mediated forces and critical evaporation separations.
  • The length dependence of effective solid-liquid line tension was identified, decaying to a macroscopic value for plates >150 solvent diameters.
  • Molecular scale correlations explain the effective line tension's length dependence.

Conclusions:

  • Macroscopic thermodynamic theory accurately describes 2D liquids under solvophobic confinement.
  • The findings support the application of this theory to surfactant monolayers for experimental validation.
  • Confinement-mediated cavitation is a key phenomenon in interfacial and soft matter systems.