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Theoretical evidence for a dense fluid precursor to crystallization.

James F Lutsko1, Grégoire Nicolis

  • 1Center for Nonlinear Phenomena and Complex Systems, Université Libre de Bruxelles, C.P. 231, Boulevard du Triomphe, 1050 Brussels, Belgium.

Physical Review Letters
|February 21, 2006
PubMed
Summary

Crystallization of fluids, including proteins, often proceeds via a dense fluid intermediate, following the Ostwald rule. This contrasts with the classical view of simultaneous ordering and densification during crystal formation.

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Area of Science:

  • Physical Chemistry
  • Soft Matter Physics
  • Biophysics

Background:

  • Understanding fluid crystallization is crucial for materials science and protein crystallization.
  • Classical crystallization models often assume direct ordering and densification.
  • The Ostwald rule of stages describes stepwise phase transitions, but its applicability to fluid crystallization is debated.

Purpose of the Study:

  • To investigate the free-energy landscape of fluid crystallization below the triple point.
  • To determine the preferred pathway for crystallization in simple atomic fluids and model proteins.
  • To compare computational findings with classical crystallization theories.

Main Methods:

  • Classical density functional theory (DFT) calculations were employed.

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  • The free-energy landscape was analyzed as a function of density and crystallinity.
  • Simulations were performed for a model globular protein and a Lennard-Jones atomic fluid.

    • Main Results:

    • A metastable dense fluid intermediate was identified as a key feature in the crystallization pathway.
    • The calculated crystallization process aligns with the Ostwald rule of stages for both model systems.
    • The findings contradict the classical assumption of simultaneous ordering and densification.

    Conclusions:

    • Fluid crystallization, even for complex systems like proteins, favors a stepwise process through a metastable dense fluid.
    • Classical density functional theory provides valuable insights into the mechanisms of phase transitions.
    • The Ostwald rule of stages is a relevant framework for understanding fluid-to-crystal transitions.