Thermodynamically Consistent Phase-Field Theory Including Nearest-Neighbor Pair Correlations Explains Failure of Mean-Field Reasoning

Fuente: arXiv
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Autores principales: Blom, Kristian, Ziethen, Noah, Zwicker, David, Godec, Aljaž
Formato: Preprint
Publicado: 2022
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author Blom, Kristian
Ziethen, Noah
Zwicker, David
Godec, Aljaž
author_facet Blom, Kristian
Ziethen, Noah
Zwicker, David
Godec, Aljaž
contents Most of our current understanding of phase separation is based on ideas that disregard correlaions. Here we illuminate unexpected effects of correlations on the structure and thermodynamics of interfaces and in turn phase separation, which are decisive in systems with strong interactions. Evaluating the continuum limit of the Ising model on the Bethe-Guggenheim level, we derive a Cahn-Hilliard free energy that takes into account pair correlations. For a one-dimensional interface in a strip geometry these are shown to give rise to an effective interface broadening at interaction strengths near and above the thermal energy, which is verified in the Ising model. Interface broadening is the result of an entropy-driven interface delocalization, which is not accounted for in the widely adopted mean field theory. Pair correlations are required for thermodynamic consistency as they enforce a thermodynamically optimal local configuration of defects and profoundly affect nucleation and spinodal decomposition at strong coupling.
format Preprint
id arxiv_https___arxiv_org_abs_2204_02962
institution arXiv
publishDate 2022
record_format arxiv
spellingShingle Thermodynamically Consistent Phase-Field Theory Including Nearest-Neighbor Pair Correlations Explains Failure of Mean-Field Reasoning
Blom, Kristian
Ziethen, Noah
Zwicker, David
Godec, Aljaž
Statistical Mechanics
Soft Condensed Matter
Biological Physics
Chemical Physics
Most of our current understanding of phase separation is based on ideas that disregard correlaions. Here we illuminate unexpected effects of correlations on the structure and thermodynamics of interfaces and in turn phase separation, which are decisive in systems with strong interactions. Evaluating the continuum limit of the Ising model on the Bethe-Guggenheim level, we derive a Cahn-Hilliard free energy that takes into account pair correlations. For a one-dimensional interface in a strip geometry these are shown to give rise to an effective interface broadening at interaction strengths near and above the thermal energy, which is verified in the Ising model. Interface broadening is the result of an entropy-driven interface delocalization, which is not accounted for in the widely adopted mean field theory. Pair correlations are required for thermodynamic consistency as they enforce a thermodynamically optimal local configuration of defects and profoundly affect nucleation and spinodal decomposition at strong coupling.
title Thermodynamically Consistent Phase-Field Theory Including Nearest-Neighbor Pair Correlations Explains Failure of Mean-Field Reasoning
topic Statistical Mechanics
Soft Condensed Matter
Biological Physics
Chemical Physics
url https://arxiv.org/abs/2204.02962