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Time-dependent distributions in self-quenching nucleation.

Vitaly A Shneidman1

  • 1Department of Physics, New Jersey Institute of Technology, Newark, New Jersey 07102, USA.

Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics
|November 9, 2011
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Nonadiabatic effects significantly alter nucleation rates and nucleus distribution in closed systems, deviating from quasi-steady-state predictions. This study reveals a continuous, double-exponential nucleus distribution, offering insights into early-stage phase transitions.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Thermodynamics

Background:

  • The Becker-Döring (BD) model describes nucleation kinetics, but often relies on quasi-steady-state (QSS) approximations.
  • Nonadiabatic effects, particularly for low nucleation barriers (<20-25k(B)T), can significantly impact nucleation dynamics.
  • Understanding these deviations is crucial for accurately modeling phase transitions and material formation.

Purpose of the Study:

  • To investigate diffusion- and interface-limited nucleation within a closed system considering supersaturation depletion.
  • To analyze the impact of nonadiabatic effects on nucleation rates and nucleus size distribution.
  • To compare the findings with QSS approximations and established theoretical models.

Main Methods:

  • Theoretical analysis of Becker-Döring type nucleation equations.
  • Inclusion of nonadiabatic effects and supersaturation depletion.
  • Comparison with numerical solutions of the BD equations and prior asymptotic solutions.

Main Results:

  • Nucleation rates deviate significantly from QSS predictions due to nonadiabatic effects.
  • The nucleus distribution exhibits a continuous, double-exponential shape, not a sharp front.
  • The total number of nuclei formed is greater than predicted by the QSS approximation.

Conclusions:

  • Nonadiabatic effects are critical for accurate nucleation modeling, especially with low energy barriers.
  • The derived nucleus distributions provide improved initial conditions for subsequent Ostwald Ripening stages.
  • This work refines the understanding of nucleation kinetics in closed systems beyond QSS assumptions.