Nonequilibrium thermodynamics of nucleation
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.
- Authors:
-
- ETH Zurich, Department of Materials, Polymer Physics, Vladimir-Prelog-Weg 2, 8093 Zurich (Switzerland)
- Publication Date:
- OSTI Identifier:
- 22413286
- Resource Type:
- Journal Article
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 141; Journal Issue: 22; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; FOKKER-PLANCK EQUATION; LIQUIDS; NUCLEATION; PARTICLE TRACKS; THERMODYNAMIC PROPERTIES; THERMODYNAMICS; TIME DEPENDENCE
Citation Formats
Schweizer, M., E-mail: marco.schweizer@math.ethz.ch, Sagis, L. M. C.,, and Food Physics Group, Wageningen University, Bornse Weilanden, 6708 WG Wageningen. Nonequilibrium thermodynamics of nucleation. United States: N. p., 2014.
Web. doi:10.1063/1.4902885.
Schweizer, M., E-mail: marco.schweizer@math.ethz.ch, Sagis, L. M. C.,, & Food Physics Group, Wageningen University, Bornse Weilanden, 6708 WG Wageningen. Nonequilibrium thermodynamics of nucleation. United States. https://doi.org/10.1063/1.4902885
Schweizer, M., E-mail: marco.schweizer@math.ethz.ch, Sagis, L. M. C.,, and Food Physics Group, Wageningen University, Bornse Weilanden, 6708 WG Wageningen. 2014.
"Nonequilibrium thermodynamics of nucleation". United States. https://doi.org/10.1063/1.4902885.
@article{osti_22413286,
title = {Nonequilibrium thermodynamics of nucleation},
author = {Schweizer, M., E-mail: marco.schweizer@math.ethz.ch and Sagis, L. M. C., and Food Physics Group, Wageningen University, Bornse Weilanden, 6708 WG Wageningen},
abstractNote = {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.},
doi = {10.1063/1.4902885},
url = {https://www.osti.gov/biblio/22413286},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 22,
volume = 141,
place = {United States},
year = {Sun Dec 14 00:00:00 EST 2014},
month = {Sun Dec 14 00:00:00 EST 2014}
}