Non-equilibrium Thermodynamics for Nucleation Kinetics
The kinetics of nucleation processes is analyzed in the framework of mesoscopic non-equilibrium thermodynamics (MNET). This scheme facilitates a flexible description of nucleation in terms of the number of atoms in the clusters of the new phase, their structure, or their dynamic state. By assuming that the evolution of the probability distribution function of those parameters is governed by the second law, an expression of the entropy production is obtained and used to characterize the irreversible nature of nucleation and to derive the corresponding kinetic equation. The MNET method is thus applied to study non-isothermal nucleation, the effects of the pressure, and nucleation in the presence of velocity and temperature gradients. Our study shows how non-equilibrium thermodynamics can be extended deep into mesoscopic and irreversible regimes, providing invaluable information on nucleation phenomena.