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Shape and area fluctuation effects on nucleation theory.

Santi Prestipino1, Alessandro Laio2, Erio Tosatti2

  • 1Università degli Studi di Messina, Dipartimento di Fisica e di Scienze della Terra, Contrada Papardo, I-98166 Messina, Italy.

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This study introduces a new nucleation theory considering fluctuating surface area, revealing higher nucleation barriers and non-spherical nucleus shapes. These findings refine understanding of phase transitions and material formation.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Thermodynamics

Background:

  • Standard nucleation theory relies on cluster volume (V) to calculate free energy barriers.
  • The role of other cluster properties, like surface area, in nucleation is often simplified or ignored.

Purpose of the Study:

  • To develop and apply a mesoscopic nucleation theory that incorporates fluctuating surface area (A) alongside volume (V).
  • To investigate the impact of surface area fluctuations on nucleation barriers and nucleus shape.

Main Methods:

  • Utilized a recently developed mesoscopic theory of nucleation.
  • Computed the free energy cost (ΔΩ) for clusters with both volume (V) and fluctuating surface area (A).
  • Analyzed the transition state where the free energy maximum is replaced by a saddle point in ΔΩ(V, A).

Main Results:

  • The nucleation barrier height is systematically higher by a few kBT compared to volume-only theories.
  • Nucleus shapes can be highly non-spherical, even with isotropic surface tension and stiffness.
  • Shape fluctuations do not alter the standard method for extracting interface tension from nucleation rates near coexistence.

Conclusions:

  • Incorporating surface area fluctuations provides a more accurate description of the nucleation process.
  • The theory predicts significant deviations from spherical shapes in nucleus formation.
  • Classical Nucleation Theory's approach to interface tension measurement remains valid despite these new insights.