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Nucleation and polymorph selection in a model colloidal fluid.

Andrea Robben Browning1, Michael F Doherty, Glenn H Fredrickson

  • 1Department of Chemical Engineering, University of California, Santa Barbara, California 93106, USA.

Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics
|June 4, 2008
PubMed
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Controlling crystal structure (polymorph selection) is key to material properties. Simulations show undercooling influences whether bcc seeds form bcc or fcc crystals in the hard-core repulsive Yukawa fluid.

Area of Science:

  • Materials Science
  • Chemical Physics
  • Crystallography

Background:

  • Crystal structure significantly impacts material properties.
  • Polymorph selection during nucleation is crucial for controlling these properties.
  • The hard-core repulsive Yukawa fluid model allows for tunable polymorph stability.

Purpose of the Study:

  • To investigate polymorph selection during nucleation in a hard-core repulsive Yukawa fluid.
  • To understand the influence of undercooling on the evolution of crystal seeds.
  • To compare simulation results with experimental observations of nucleation.

Main Methods:

  • Utilized seeded molecular-dynamics simulations to track the growth of metastable bcc seeds within the stable fcc region.
  • Varied the degree of undercooling to observe its effect on seed development.

Related Experiment Videos

  • Compared simulation outcomes of homogeneous nucleation with colloidal crystallization experiments.

    • Main Results:

    • The degree of undercooling dictates the fate of bcc seeds: low undercooling favors bcc crystal formation, while high undercooling leads to transformation into fcc crystals.
    • Simulations produced nuclei with shapes and minimum growth sizes comparable to experimental findings.
    • Simulated nuclei initially showed a stronger bcc signature than experimental ones, which diminished with further growth.

    Conclusions:

    • Undercooling is a critical factor in determining the final crystal structure during nucleation.
    • Simulation results align well with experimental observations, with discrepancies potentially explained by longer structural relaxation times in experiments.
    • This study provides insights into controlling polymorph selection through nucleation conditions.