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Correlation between Fast Relaxation, Shear Phonon Propagation, and Dynamic Heterogeneity in Glass-Forming Liquids.

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Fast relaxation dynamics in glass-formers are linked to local structure and shear phonon behavior. This study reveals fast relaxation as a key intermediate process in the emergence of glassy dynamics.

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Area of Science:

  • Condensed matter physics
  • Materials science
  • Chemical physics

Background:

  • Fast relaxation precedes α-relaxation in glass-forming liquids, but its origins are unclear.
  • Understanding fast relaxation is crucial for explaining glassy dynamics and dynamic heterogeneity.

Purpose of the Study:

  • To investigate the microscopic origin and dynamics of fast relaxation in fragile glass-formers.
  • To elucidate the role of fast relaxation in the emergence of glassy dynamics.

Main Methods:

  • Inelastic neutron scattering (INS) was employed to study the fragile glass-former Ca$_{0.4}$K$_{0.6}$(NO$_{3}$)$_{1.4}$.
  • Analysis focused on the temperature dependence of fast relaxation dynamics and its correlation with structural and elastic properties.

Main Results:

  • Fast relaxation dynamics are significantly influenced by local structural arrangements.
  • A distinct temperature dependence of fast relaxation was observed, correlating with shear phonon propagation.
  • This behavior links to the Arrhenius-to-super-Arrhenius crossover observed in α-relaxation.

Conclusions:

  • Fast relaxation originates from the interplay between shear phonon softening and local structural rearrangements.
  • Fast relaxation acts as an intermediate dynamical process connecting elastic interactions to kinetic facilitation.
  • This process is fundamental to the emergence of dynamic heterogeneity in supercooled liquids.