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Frequency-dependent Stokes-Einstein relation in supercooled liquids.

Ronen Zangi1, Laura J Kaufman

  • 1Department of Chemistry, Columbia University, New York, NY 10027, USA.

Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics
|August 7, 2007
PubMed
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The frequency-dependent Stokes-Einstein relation is valid for supercooled liquids at intermediate frequencies but deviates at lower frequencies. This breakdown is linked to correlated motions and decreasing temperatures, impacting diffusion coefficient accuracy.

Area of Science:

  • Condensed matter physics
  • Chemical physics
  • Materials science

Background:

  • The Stokes-Einstein relation traditionally links diffusion and viscosity in liquids.
  • Supercooled liquids exhibit complex dynamics, challenging classical relations.
  • Understanding relaxation processes is key to characterizing supercooled liquid behavior.

Purpose of the Study:

  • To evaluate the frequency-dependent Stokes-Einstein relation in supercooled liquids.
  • To identify conditions under which the Stokes-Einstein relation deviates.
  • To elucidate the molecular origins of deviations in supercooled liquids.

Main Methods:

  • Molecular dynamics simulations were employed.
  • Simulations were conducted at various temperatures.

Related Experiment Videos

  • Analysis focused on frequency-dependent diffusion and relaxation regimes.

    • Main Results:

    • The Stokes-Einstein relation holds at intermediate frequencies (beta- and alpha-relaxation onset).
    • Significant deviations occur at lower frequencies, increasing with lower temperatures.
    • These deviations correlate with frequencies below the maximum of the non-Gaussian parameter (alpha2).

    Conclusions:

    • The frequency-dependent Stokes-Einstein relation is not universally valid in supercooled liquids.
    • Deviations arise from neglecting correlated motions in diffusion coefficient calculations.
    • Accurate modeling of supercooled liquid dynamics requires accounting for collective molecular movements.