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Heterogeneous diffusion, viscosity, and the Stokes-Einstein relation in binary liquids.

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|June 15, 2016
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Summary
This summary is machine-generated.

The Stokes-Einstein relation breaks down in metallic melts due to dynamic heterogeneity. Slow-moving particles significantly impact viscosity, explaining the breakdown and recovering the relation when considering "slow" diffusion and viscosity separately.

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Area of Science:

  • Condensed matter physics
  • Materials science
  • Computational chemistry

Background:

  • The Stokes-Einstein relation (SER) connects diffusivity and viscosity in liquids.
  • Its breakdown in undercooled melts, particularly metallic melts, is a key phenomenon in materials science.
  • Understanding this breakdown is crucial for predicting material properties at low temperatures.

Purpose of the Study:

  • To investigate the origins of the Stokes-Einstein relation breakdown in undercooled melts.
  • To analyze the role of dynamic heterogeneity in this phenomenon.
  • To explore the relationship between particle dynamics and macroscopic transport properties.

Main Methods:

  • Molecular dynamics simulations of a binary Lennard-Jones system, modeling a metallic melt.
  • Analysis of the isotope effect to understand motion collectivization.
  • Utilizing the van Hove self-correlation function to identify and track particle dynamics.
  • Calculating self-diffusivity and viscosity contributions from different particle populations.

Main Results:

  • A weak breakdown of SER at high temperatures is linked to collective motion.
  • A strong breakdown at lower temperatures correlates with increased dynamic heterogeneity.
  • Identified distinct populations of 'fast' and 'slow' particles.
  • Slow particles exhibit lower diffusivity than SER predicts and contribute significantly to viscosity.
  • Both diffusion and viscosity exhibit heterogeneous dynamics.

Conclusions:

  • Dynamic heterogeneity is the primary driver for the breakdown of the Stokes-Einstein relation in undercooled metallic melts.
  • The concept of "slow" diffusivity and "slow" viscosity can recover the SER.
  • This work provides a microscopic explanation for deviations from the SER in complex liquid systems.