Optimization of crystal nucleation close to a metastable fluid-fluid phase transition

The presence of a metastable fluid-fluid critical point is thought to dramatically influence the crystallization pathway, increasing the nucleation rate by many orders of magnitude over the predictions of classical nucleation theory. We use molecular dynamics simulations to study the kinetics of cry...

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Main Authors:	Wedekind, Jan, Xu, Limei, Buldyrev, Sergey V., Stanley, H. Eugene, Reguera, David, Franzese, Giancarlo
Format:	Online
Language:	English
Published:	Nature Publishing Group 2015
Online Access:	https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4476038/

id	pubmed-4476038
recordtype	oai_dc
spelling	pubmed-44760382015-06-24 Optimization of crystal nucleation close to a metastable fluid-fluid phase transition Wedekind, Jan Xu, Limei Buldyrev, Sergey V. Stanley, H. Eugene Reguera, David Franzese, Giancarlo Article The presence of a metastable fluid-fluid critical point is thought to dramatically influence the crystallization pathway, increasing the nucleation rate by many orders of magnitude over the predictions of classical nucleation theory. We use molecular dynamics simulations to study the kinetics of crystallization in the vicinity of this metastable critical point and throughout the metastable fluid-fluid phase diagram. To quantitatively understand how the fluid-fluid phase separation affects the crystal nucleation, we evaluate accurately the kinetics and reconstruct the thermodynamic free-energy landscape of crystal formation. Contrary to expectations, we find no special advantage of the proximity of the metastable critical point on the crystallization rates. However, we find that the ultrafast formation of a dense liquid phase causes the crystallization to accelerate both near the metastable critical point and almost everywhere below the fluid-fluid spinodal line. These results unveil three different scenarios for crystallization that could guide the optimization of the process in experiments Nature Publishing Group 2015-06-22 /pmc/articles/PMC4476038/ /pubmed/26095898 http://dx.doi.org/10.1038/srep11260 Text en Copyright © 2015, Macmillan Publishers Limited http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
repository_type	Open Access Journal
institution_category	Foreign Institution
institution	US National Center for Biotechnology Information
building	NCBI PubMed
collection	Online Access
language	English
format	Online
author	Wedekind, Jan Xu, Limei Buldyrev, Sergey V. Stanley, H. Eugene Reguera, David Franzese, Giancarlo
spellingShingle	Wedekind, Jan Xu, Limei Buldyrev, Sergey V. Stanley, H. Eugene Reguera, David Franzese, Giancarlo Optimization of crystal nucleation close to a metastable fluid-fluid phase transition
author_facet	Wedekind, Jan Xu, Limei Buldyrev, Sergey V. Stanley, H. Eugene Reguera, David Franzese, Giancarlo
author_sort	Wedekind, Jan
title	Optimization of crystal nucleation close to a metastable fluid-fluid phase transition
title_short	Optimization of crystal nucleation close to a metastable fluid-fluid phase transition
title_full	Optimization of crystal nucleation close to a metastable fluid-fluid phase transition
title_fullStr	Optimization of crystal nucleation close to a metastable fluid-fluid phase transition
title_full_unstemmed	Optimization of crystal nucleation close to a metastable fluid-fluid phase transition
title_sort	optimization of crystal nucleation close to a metastable fluid-fluid phase transition
description	The presence of a metastable fluid-fluid critical point is thought to dramatically influence the crystallization pathway, increasing the nucleation rate by many orders of magnitude over the predictions of classical nucleation theory. We use molecular dynamics simulations to study the kinetics of crystallization in the vicinity of this metastable critical point and throughout the metastable fluid-fluid phase diagram. To quantitatively understand how the fluid-fluid phase separation affects the crystal nucleation, we evaluate accurately the kinetics and reconstruct the thermodynamic free-energy landscape of crystal formation. Contrary to expectations, we find no special advantage of the proximity of the metastable critical point on the crystallization rates. However, we find that the ultrafast formation of a dense liquid phase causes the crystallization to accelerate both near the metastable critical point and almost everywhere below the fluid-fluid spinodal line. These results unveil three different scenarios for crystallization that could guide the optimization of the process in experiments
publisher	Nature Publishing Group
publishDate	2015
url	https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4476038/
_version_	1613238573461405696

Optimization of crystal nucleation close to a metastable fluid-fluid phase transition

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