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Modelling the structural evolution of ternary phosphate glasses from melts to solid amorphous materials.

Devis Di Tommaso1, Richard I Ainsworth, Emilia Tang

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Summary

This study characterizes phosphate-based melts and glasses using advanced simulations. Higher calcium content increases glass rigidity, validating a new shell-model forcefield for accurate structural analysis.

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Area of Science:

  • Materials Science
  • Computational Chemistry
  • Solid State Chemistry

Background:

  • Phosphate-based melts and glasses are crucial in various applications.
  • Understanding their local and medium-range structural properties is essential for material design.
  • Existing simulation methods may not fully capture the complexities of these amorphous systems.

Purpose of the Study:

  • To characterize the structural properties of phosphate-based melts and glasses.
  • To investigate the effect of calcium content on glass structure and rigidity.
  • To validate a new shell-model forcefield against first-principles simulations.

Main Methods:

  • First principles (density functional theory) molecular dynamics simulations.
  • Classical (shell-model) molecular dynamics simulations.
  • Melt-and-quench simulations for glass structure generation.

Main Results:

  • Melts exhibit transient threefold (P3c) and fivefold (P5c) phosphorus atoms, with defects decreasing upon cooling.
  • Glass structure is dominated by Q2 and Q1 species; Q3 units decrease with increasing calcium.
  • Higher calcium content enhances phosphate network rigidity due to calcium's higher field strength.
  • The validated shell-model forcefield accurately describes local and medium-range structures, outperforming rigid ion potentials.

Conclusions:

  • Calcium concentration significantly influences the structural rigidity of phosphate glasses.
  • The developed shell-model forcefield is a reliable tool for simulating phosphate-based materials.
  • First-principles simulations provide a benchmark for validating classical simulation models.