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Mobility propagation and dynamic facilitation in superionic conductors.

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Dynamic facilitation (DF) drives heterogeneous dynamics in superionic conductors like CaF2 and UO2. This mechanism peaks near the superionic transition temperature, explaining clustered mobile and immobile regions.

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Area of Science:

  • Materials Science
  • Condensed Matter Physics
  • Physical Chemistry

Background:

  • Dynamical heterogeneity (DH) describes clustered mobile and immobile regions in materials.
  • Type II superionic conductors, such as UO2, exhibit complex dynamic behaviors.
  • Previous work identified DH in UO2, necessitating a mechanistic understanding.

Purpose of the Study:

  • To demonstrate the dynamic facilitation (DF) mechanism in superionic conductors CaF2 and UO2.
  • To investigate the temperature dependence of DF and its relationship with DH.
  • To elucidate the role of DF in underpinning heterogeneous dynamics.

Main Methods:

  • Atomistic simulations were employed to model CaF2 and UO2.
  • The mobility transfer function was utilized to quantify DF.
  • Metrics for both DH and DF were calculated and compared.

Main Results:

  • Dynamic facilitation (DF) was demonstrated in both CaF2 and UO2.
  • DF intensity exhibits non-monotonic temperature dependence, peaking near the superionic transition temperature (Tλ).
  • A strong correspondence was observed between metrics quantifying DH and DF.

Conclusions:

  • Dynamic facilitation (DF) is the underlying mechanism for heterogeneous dynamics in type II superionic conductors.
  • DF plays a crucial role in the emergence of clustered mobile and immobile regions.
  • The findings support the framework of kinematically constrained models for superionic conductors.