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Title: 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:
 [1]
  1. 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}
}