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This study directly computes the Tolman length (δ) for solid-liquid interfaces using atomistic simulations. The findings validate the approach and improve predictions of nucleation free energy using classical nucleation theory.

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Area of Science:

  • Materials Science
  • Chemical Physics
  • Thermodynamics

Background:

  • Interfacial free energy curvature is key for nucleation kinetics and phase stability.
  • The Tolman length (δ) quantifies this curvature dependence.
  • Direct computation of δ for solid-liquid interfaces is challenging.

Purpose of the Study:

  • To directly evaluate the Tolman length (δ) for solid-liquid interfaces.
  • To validate a novel computational approach for determining δ.
  • To assess the impact of δ on classical nucleation theory predictions.

Main Methods:

  • Atomistic simulations of a solid-liquid planar interface under non-equilibrium conditions.
  • Calculating surface tension via thermal capillary fluctuations of a localized Gibbs dividing surface.
  • Determining δ by analyzing changes in surface energy relative to the equimolar dividing surface.

Main Results:

  • Successful direct computation of the Tolman length (δ) for a model solid-liquid interface.
  • Good agreement between directly computed δ and values inferred from nucleation simulations.
  • Validation of the computational methodology for determining δ.

Conclusions:

  • The direct computation method for Tolman length (δ) is validated.
  • Accurate incorporation of Tolman length improves classical nucleation theory predictions.
  • This work provides a pathway for more precise modeling of nucleation phenomena.