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Heating a crystalline solid increases the average energy of its atoms, molecules, or ions, and the solid gets hotter. At some point, the added energy becomes large enough to partially overcome the forces holding the molecules or ions of the solid in their fixed positions, and the solid begins the process of transitioning to the liquid state or melting. At this point, the temperature of the solid stops rising, despite the continual input of heat, and it remains constant until all of the solid is...
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Fragility and correlated dynamics in supercooled liquids.

Atreyee Banerjee1, David J Wales1

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Supercooled liquids exhibit super-Arrhenius behavior linked to correlated dynamics. Short-time dynamics reveal similar nonergodic behavior across different potentials, suggesting a strong connection between fragility and dynamical correlation.

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Computational Chemistry

Background:

  • Supercooled liquids exhibit complex dynamics deviating from simple Arrhenius behavior.
  • Understanding the relationship between dynamical properties and correlated motion is crucial for glass transition theories.

Purpose of the Study:

  • To investigate the connection between super-Arrhenius behavior and correlated dynamics in supercooled liquids.
  • To analyze dynamical properties using both Lennard-Jones and Weeks-Chandler-Andersen potentials across various densities.

Main Methods:

  • Examination of short-time nonergodic trajectory segments within longer ergodic trajectories.
  • Analysis of apparent diffusivity and its behavior at low temperatures.
  • Introduction of a correlation factor to rescale nonergodic diffusivity.

Main Results:

  • Apparent diffusivity follows Arrhenius behavior at short times, independent of potentials and densities.
  • Short-time nonergodic dynamics show similarity across different potentials, despite differing ergodic diffusivities.
  • A rescaled nonergodic diffusivity, incorporating a correlation factor, reasonably estimates the true ergodic diffusivity.

Conclusions:

  • Confirms a strong link between system fragility and dynamical correlation in supercooled liquids.
  • Short-time nonergodic dynamics provide insights into the collective behavior of supercooled liquids.
  • The developed rescaling method offers a way to estimate true ergodic diffusivity from nonergodic segments.