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Phase Stability of Dynamically Disordered Solids from First Principles.

Johan Klarbring1, Sergei I Simak1

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This study introduces a new method to calculate the free energy of dynamically disordered solids, crucial for understanding superionic conductors. The approach accurately predicts phase transition properties, advancing solid-state electrolyte development.

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Area of Science:

  • Materials Science
  • Solid-State Physics
  • Computational Chemistry

Background:

  • Studying phase stability in dynamically disordered solids is challenging due to limitations in standard models.
  • Dynamically disordered materials, especially superionic conductors, offer potential for advanced applications like solid-state batteries.
  • Limited stability of disordered phases hinders the practical application of these promising materials.

Purpose of the Study:

  • To develop a theoretical method for calculating the free energy of dynamically disordered solids.
  • To investigate the phase stability of superionic conductors and other materials exhibiting dynamic disorder.
  • To accurately model the thermodynamic properties of phase transitions in these materials.

Main Methods:

  • Utilizing stress-strain thermodynamic integration along a deformation path.
  • Connecting a mechanically stable ordered phase to the dynamically disordered phase.
  • Analyzing the stress behavior along the deformation path to capture entropy contributions.

Main Results:

  • Successfully calculated the free energy of dynamically disordered solids.
  • Applied the method to Bi_{2}O_{3}, accurately reproducing experimental transition enthalpy and critical temperature for the superionic δ phase.
  • Demonstrated that entropy contributions from dynamic disorder are reflected in stress-strain behavior.

Conclusions:

  • The developed method provides a first-principles approach to describe phase stability in materials with dynamic disorder.
  • This technique is applicable to superionic conductors and other solids where the disordered phase can be continuously deformed from a stable phase.
  • The findings pave the way for designing more stable and efficient solid-state electrolytes.