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Stokes-Einstein relations for a square-well fluid.

P Nigra1, G T Evans

  • 1Department of Chemistry, Oregon State University, Corvallis, 97331, USA.

The Journal of Chemical Physics
|July 23, 2005
PubMed
Summary
This summary is machine-generated.

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The Stokes-Einstein relation for shear viscosity (eta) and self-diffusion (D) holds for simple fluid interactions. Deviations arise from complex three-body interactions, impacting diffusion more than viscosity.

Area of Science:

  • Physical Chemistry
  • Statistical Mechanics
  • Soft Matter Physics

Background:

  • The Stokes-Einstein relation connects shear viscosity (eta) and self-diffusion (D) in fluids.
  • Understanding deviations from this relation is crucial for complex fluids.

Purpose of the Study:

  • To construct and analyze a Stokes-Einstein relation for a classical fluid with square-well potentials.
  • To investigate the contributions of multi-body interactions to viscosity and diffusion.

Main Methods:

  • Utilized a Smoluchowski equation for pair diffusion dynamics.
  • Separated time correlation functions for eta and D into contributions from hard-sphere and square-well forces.
  • Analyzed two-, three-, and four-body correlation functions.

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Main Results:

  • Self-diffusion (D) exhibits activated, Arrhenius-like behavior.
  • The product of D and eta adheres to the Stokes-Einstein relation at the two-body level, with minor corrections for soft potentials.
  • Three-body correlations enhance D, while higher-order correlations in eta partially offset each other.
  • Deviations from the Stokes-Einstein law are primarily attributed to three-body correlation functions in D.

Conclusions:

  • The study provides a detailed molecular-level analysis of the Stokes-Einstein relation in a model fluid.
  • Three-body interactions are identified as the key source of deviation from the Stokes-Einstein law, particularly influencing self-diffusion.