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Laser-induced structural modification in calcium aluminosilicate glasses using molecular dynamic simulations.

Sean Locker1, Sushmit Goyal2, Matthew E McKenzie2

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Pulsed laser processing transforms aluminum structures in calcium aluminosilicate glasses, increasing density. Laser energy and glass composition significantly influence these laser-induced structural changes and densification.

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Area of Science:

  • Materials Science
  • Condensed Matter Physics
  • Computational Materials Science

Background:

  • Understanding the structural behavior of multicomponent oxide glasses under extreme conditions is crucial for materials development.
  • Calcium aluminosilicate glasses are widely used in various industrial applications, necessitating detailed studies of their response to external stimuli.
  • Pulsed laser interactions with materials offer unique pathways for modifying material properties at the atomic level.

Purpose of the Study:

  • To investigate the structural transformations in CaO-Al2O3-SiO2 glasses induced by simulated pulsed laser irradiation.
  • To correlate changes in aluminum coordination (Al(IV) to Al(V)) with macroscopic property changes like glass densification.
  • To determine the influence of laser pulse energy and glass composition on laser-induced structural modifications.

Main Methods:

  • Molecular dynamics simulations were employed to model the effects of pulsed laser irradiation on glass structures.
  • Simulations covered a range of laser pulse energies and calcium aluminosilicate glass compositions (50-80% SiO2).
  • Analysis focused on short- and intermediate-range order, coordination numbers, bond angles, and bond distances.

Main Results:

  • A direct correlation was observed between the transformation of aluminum from four-fold (Al(IV)) to five-fold (Al(V)) coordination and increased glass density.
  • Laser processing led to reduced average T-O-T (T=Al, Si) bond angles and increased T-O bond lengths.
  • Glass densification was found to be dependent on both the applied laser pulse energy and the specific glass chemistry.

Conclusions:

  • Pulsed laser irradiation induces significant structural changes in calcium aluminosilicate glasses, including aluminum coordination shifts and densification.
  • The degree of laser-induced densification is strongly dependent on laser pulse energy and the silica content of the glass.
  • Molecular dynamics simulations provide valuable insights into the mechanisms of laser-matter interaction and structural evolution in oxide glasses.