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Ligand-Mediated Nucleation and Growth of Palladium Metal Nanoparticles
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Classical nucleation theory from a dynamical approach to nucleation.

James F Lutsko1, Miguel A Durán-Olivencia

  • 1Center for Nonlinear Phenomena and Complex Systems, Code Postal 231, Université Libre de Bruxelles, Blvd. du Triomphe, 1050 Brussels, Belgium. jlutsko@ulb.ac.be

The Journal of Chemical Physics
|July 5, 2013
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Summary

A new dynamical theory of nucleation recovers classical nucleation theory (CNT) and refines it for systems like proteins. It corrects nucleation rates and reveals limitations of the monomer attachment model at high supersaturations.

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Area of Science:

  • Physical Chemistry
  • Chemical Physics
  • Materials Science

Background:

  • Classical nucleation theory (CNT) provides a foundational model for phase transitions.
  • Recent advancements include dynamical theories based on fluctuating hydrodynamics.
  • Understanding nucleation is critical for processes involving protein crystallization and solution behavior.

Purpose of the Study:

  • To demonstrate that classical nucleation theory (CNT) is a limit of a dynamical theory.
  • To develop a more realistic nucleation theory incorporating finite interfacial width.
  • To investigate nucleation in globular protein solutions.

Main Methods:

  • Derivation of a dynamical nucleation theory from fluctuating hydrodynamics.
  • Extension of the theory to include finite interfacial width effects.
  • Application to the dilute solution/dense solution transition in globular proteins.

Main Results:

  • Classical nucleation theory (CNT) is recovered as a limiting case of the dynamical theory.
  • The extended theory provides corrections to nucleation rates in protein solutions, even at low supersaturations.
  • The monomer attachment/detachment model fails for clusters smaller than approximately 100 molecules.
  • Improved free energy barrier estimates are crucial for accurate nucleation predictions.

Conclusions:

  • The dynamical theory offers a more comprehensive framework for nucleation phenomena.
  • Finite interfacial width and monomer distribution significantly impact nucleation rates.
  • The study highlights the importance of reaction coordinate choice and corrections to the capillary model in nucleation theory.