Nonequilibrium thermodynamics of nucleation

M. Schweizer, L.M.C. Sagis

Research output: Contribution to journalArticleAcademicpeer-review

10 Citations (Scopus)

Abstract

We present a novel approach to nucleation processes based on the GENERIC framework (general equation for the nonequilibrium reversible-irreversible coupling). Solely based on the GENERIC structure of time-evolution equations and thermodynamic consistency arguments of exchange processes between a metastable phase and a nucleating phase, we derive the fundamental dynamics for this phenomenon, based on continuous Fokker-Planck equations. We are readily able to treat non-isothermal nucleation even when the nucleating cores cannot be attributed intensive thermodynamic properties. In addition, we capture the dynamics of the time-dependent metastable phase being continuously expelled from the nucleating phase, and keep rigorous track of the volume corrections to the dynamics. Within our framework the definition of a thermodynamic nuclei temperature is manifest. For the special case of nucleation of a gas phase towards its vapor-liquid coexistence, we illustrate that our approach is capable of reproducing recent literature results obtained by more microscopic considerations for the suppression of the nucleation rate due to nonisothermal effects.
Original languageEnglish
Article number224102
Number of pages13
JournalJournal of Chemical Physics
Volume141
DOIs
Publication statusPublished - 2014

Keywords

  • homogeneous nucleation
  • inhomogeneous-media
  • general formalism
  • complex fluids
  • systems
  • clusters
  • dynamics
  • temperature
  • interface
  • equations

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