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Diffusivity anomaly in modified Stillinger-Weber liquids.

Shiladitya Sengupta1, Vishwas V Vasisht2, Srikanth Sastry1

  • 1TIFR Centre for Interdisciplinary Sciences, 21 Brundavan Colony, Narsingi, Hyderabad 500089, India.

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Researchers studied how changing tetrahedrality affects liquid silicon

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Area of Science:

  • Condensed Matter Physics
  • Computational Materials Science
  • Physical Chemistry

Background:

  • The Stillinger-Weber model describes silicon's properties.
  • A diffusivity anomaly, similar to water's, is observed in some liquids.
  • Understanding liquid dynamics requires linking structure and thermodynamics.

Purpose of the Study:

  • To investigate the diffusivity anomaly in modified Stillinger-Weber silicon liquids.
  • To explore the relationship between tetrahedrality, temperature, and liquid dynamics.
  • To rationalize the diffusivity anomaly using structural and thermodynamic properties.

Main Methods:

  • Modified the tetrahedrality in the Stillinger-Weber potential.
  • Simulated a series of model silicon liquids at fixed pressure.
  • Analyzed diffusivity, excess entropy, and pair correlation entropy.
  • Applied the Rosenfeld relation to connect dynamics and thermodynamics.

Main Results:

  • Diffusivity shows a maximum with changing tetrahedrality (diffusivity anomaly).
  • The Rosenfeld relation accurately predicts diffusivity above melting temperatures.
  • Deviations from the Rosenfeld relation occur below melting temperatures, decreasing with lower tetrahedrality.
  • Excess entropy and pair correlation entropy also exhibit maxima with tetrahedrality.

Conclusions:

  • Structural and thermodynamic changes correlate with dynamical anomalies in these silicon liquids.
  • The Rosenfeld relation's validity is temperature-dependent.
  • Tetrahedrality is a key parameter influencing both structure and dynamics in model silicon liquids.