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Related Experiment Videos

Crystal nucleation in simple and complex fluids.

David W Oxtoby1

  • 1The James Franck Institute, University of Chicago, 5640 South Ellis Avenue, Chicago, IL 60637, USA.

Philosophical Transactions. Series A, Mathematical, Physical, and Engineering Sciences
|March 29, 2003
PubMed
Summary

Density-functional methods reveal distinct crystal nucleation mechanisms in simple and complex fluids. For complex fluids like protein solutions, density changes precede crystalline order, explaining the observed

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Area of Science:

  • Statistical mechanics
  • Materials science
  • Biophysics

Background:

  • Crystal nucleation from melts is crucial in materials science and biophysics.
  • Existing models often assume uniform density changes during nucleation.
  • Protein crystallization exhibits empirical 'crystallization windows' lacking theoretical basis.

Purpose of the Study:

  • To apply density-functional theory to understand crystal nucleation mechanisms.
  • To compare nucleation in simple fluids (metals) versus complex fluids (protein solutions).
  • To provide a theoretical framework for protein crystallization phenomena.

Main Methods:

  • Utilized density-functional methods derived from statistical mechanics.
  • Compared theoretical predictions with molecular dynamics simulations.

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  • Analyzed fluid behavior, including density and crystalline order.

    • Main Results:

    • Identified size-dependent nucleation mechanisms based on fluid complexity.
    • Proposed a novel nucleation pathway for complex fluids involving pre-ordering density changes.
    • Demonstrated consistency between theoretical models and simulation data.

    Conclusions:

    • Density-functional theory offers a unified approach to crystal nucleation.
    • A distinct nucleation mechanism involving density fluctuations is key for complex fluids.
    • This provides a theoretical foundation for the 'crystallization window' in protein crystallization.