Nonequilibrium thermodynamics of nucleation

Area of Science:

• Thermodynamics
• Physical Chemistry
• Materials Science

Background:

• Nucleation is a critical phenomenon in phase transitions.
• Existing models struggle with non-isothermal conditions and complex phase dynamics.

Purpose of the Study:

• To develop a novel, thermodynamically consistent framework for nucleation processes.
• To accurately model non-isothermal nucleation, even without intensive thermodynamic properties for nuclei.
• To capture the dynamics of phase expulsion and volume corrections during nucleation.

Main Methods:

• Utilizing the general equation for nonequilibrium reversible-irreversible coupling (GENERIC) framework.
• Deriving fundamental nucleation dynamics using continuous Fokker-Planck equations.
• Applying thermodynamic consistency arguments for phase exchange processes.

Main Results:

• Successfully derived the fundamental dynamics for nucleation processes.
• Enabled treatment of non-isothermal nucleation where nuclei lack intensive thermodynamic properties.
• Captured dynamics of metastable phase expulsion and rigorous volume corrections.
• Manifested a clear definition of thermodynamic nuclei temperature.

Conclusions:

• The GENERIC-based approach provides a robust framework for nucleation studies.
• This method accurately reproduces literature results for non-isothermal gas-phase nucleation.
• The framework offers a powerful tool for understanding complex phase transitions.