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Polymorph selection during the crystallization of Yukawa systems.

Caroline Desgranges1, Jerome Delhommelle

  • 1Department of Chemical Engineering, 301 South Main Street, University of South Carolina, Columbia South Carolina 29201, USA.

The Journal of Chemical Physics
|February 17, 2007
PubMed
Summary

Molecular-dynamics simulations reveal that colloidal crystal crystallization depends on the screening parameter. Body-centered cubic (bcc) crystallization is straightforward, while face-centered cubic (fcc) crystallization involves complex mechanisms and later polymorph selection.

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Computational Chemistry

Background:

  • Supercooled liquids of charge-stabilized colloidal suspensions are modeled using the Yukawa potential.
  • The screening parameter (lambda) influences the relative stability of body-centered cubic (bcc) and face-centered cubic (fcc) polymorphs.

Purpose of the Study:

  • To investigate the crystallization mechanisms of colloidal suspensions under varying stability conditions of bcc and fcc polymorphs.
  • To understand how the screening parameter affects crystal nucleation and growth.
  • To examine crystallization from a seeded stable polymorph.

Main Methods:

  • Molecular-dynamics simulations were employed.
  • The Yukawa potential was used to model charge-stabilized colloidal suspensions.
  • The screening parameter (lambda) was systematically varied to alter polymorph stability.

Main Results:

  • Crystallization mechanisms differ significantly with the screening parameter.
  • For lambda=3 (bcc stable), nucleation and polymorph selection are rapid and straightforward.
  • For lambda=10 (fcc stable), nucleation favors bcc, followed by complex growth involving cross-nucleation between fcc and hexagonal close-packed (hcp) polymorphs, leading to later polymorph selection.
  • Growth from a seeded fcc crystal face follows similar complex mechanisms.

Conclusions:

  • The crystallization pathway of colloidal suspensions is highly sensitive to the screening parameter.
  • Polymorph selection timing is dictated by the interplay between kinetics and thermodynamics during nucleation and growth.
  • Seeded growth recapitulates the complex polymorph selection mechanisms observed in homogeneous nucleation.