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Methods of Ex Situ and In Situ Investigations of Structural Transformations: The Case of Crystallization of Metallic Glasses
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"Inner clocks" of glass-forming liquids.

Ricardo Peredo-Ortiz1, Magdaleno Medina-Noyola1, Thomas Voigtmann2

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We explain the microscopic origins of material time in aging amorphous materials. This concept, crucial for understanding property changes, is linked to irreversible thermodynamics and offers new insights into complex material behavior.

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Area of Science:

  • Statistical thermodynamics
  • Materials science
  • Physical chemistry

Background:

  • Explaining aging in non-equilibrium amorphous materials is a key challenge.
  • The Tool-Narayanaswamy-Moynihan model empirically describes property evolution using material time.
  • The fundamental basis for the material time concept's success remains unclear.

Purpose of the Study:

  • To provide a physically sound, microscopic explanation for the material time concept in aging amorphous materials.
  • To connect the empirical material time model with fundamental principles of irreversible thermodynamics.
  • To extend the understanding of material time to complex systems with multiple relaxation modes.

Main Methods:

  • Applying linear laws of irreversible thermodynamics and their extensions.
  • Treating kinetic coefficients as state functions of the evolving material state.
  • Leveraging the mathematical structure shared between the Tool model and non-equilibrium Langevin equation theory.
  • Utilizing Onsager's theory of irreversible processes.

Main Results:

  • A microscopic rationale for the material time concept is established.
  • The mathematical equivalence between the Tool model and advanced Langevin equation theory is identified.
  • A framework for generalizing material time to systems with multiple relaxation modes is proposed.
  • Partial ergodicity breaking in partially frozen glasses is linked to multiple internal clocks.

Conclusions:

  • The study provides a fundamental understanding of material time in amorphous materials.
  • The findings bridge empirical models with fundamental thermodynamic principles.
  • The work paves the way for understanding complex aging phenomena and designing materials with tailored properties.