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Using swapping layers in molecular dynamics simulations to drive structural equilibration far below T_{g}.

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This study introduces a novel "swept swapping" simulation technique to improve structural annealing in molecular solids. This method enhances density and order at lower temperatures, surpassing previous limitations.

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Area of Science:

  • Materials Science
  • Computational Physics
  • Chemical Engineering

Background:

  • Vapor-deposited molecular solids exhibit anomalous surface mobility, enabling structural annealing and density increases down to approximately 0.85 times the glass transition temperature (Tg).
  • Extending structural annealing to lower temperatures has been a significant challenge in materials simulation.

Purpose of the Study:

  • To design and characterize a novel simulation technique, "swept swapping," to facilitate structural annealing at lower temperatures.
  • To investigate the impact of sphere size dispersion and a surface-following Monte Carlo swap region on structural relaxation.

Main Methods:

  • Simulation of films grown using size-dispersed attractive Lennard-Jones (L-J) potential spheres deposited onto a free surface.
  • Equilibration using a surface-following Monte Carlo swap region, where motion and sphere size dispersion accelerate structural relaxation.
  • Utilized a sphere size span of 25% and a size step of ~2.5% to suppress crystallization and maintain high swap acceptance.

Main Results:

  • The "swept swapping" technique achieves structural relaxation orders of magnitude faster than bulk swapping.
  • The simulation attains a high packing fraction, comparable to hexagonal-close-packed L-J crystals without size dispersion.
  • Further swapping refines the structure, maximizing short-range icosahedral order to unprecedented levels.

Conclusions:

  • The "swept swapping" method effectively extends structural annealing to lower temperatures, significantly enhancing molecular solid simulation.
  • This technique allows for the creation of highly ordered amorphous solids with packing fractions near crystalline limits.
  • The observed levels of icosahedral order are primarily limited by computational resources.