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Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures

When driven out of equilibrium, many diverse systems can form complex spatial and dynamical patterns, even in the absence of attractive interactions. Using kinetic Monte Carlo simulations, we investigate the phase behavior of a binary system of particles of dissimilar size confined between semiflexi...

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Autores principales: Pestana, Luis Ruiz, Minnetian, Natalie, Lammers, Laura Nielsen, Head-Gordon, Teresa
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5887813/
https://www.ncbi.nlm.nih.gov/pubmed/29675210
http://dx.doi.org/10.1039/c7sc03524a
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author Pestana, Luis Ruiz
Minnetian, Natalie
Lammers, Laura Nielsen
Head-Gordon, Teresa
author_facet Pestana, Luis Ruiz
Minnetian, Natalie
Lammers, Laura Nielsen
Head-Gordon, Teresa
author_sort Pestana, Luis Ruiz
collection PubMed
description When driven out of equilibrium, many diverse systems can form complex spatial and dynamical patterns, even in the absence of attractive interactions. Using kinetic Monte Carlo simulations, we investigate the phase behavior of a binary system of particles of dissimilar size confined between semiflexible planar surfaces, in which the nanoconfinement introduces a non-local coupling between particles, which we model as an activation energy barrier to diffusion that decreases with the local fraction of the larger particle. The system autonomously reaches a cyclical non-equilibrium state characterized by the formation and dissolution of metastable micelle-like clusters with the small particles in the core and the large ones in the surrounding corona. The power spectrum of the fluctuations in the aggregation number exhibits 1/f noise reminiscent of self-organized critical systems. We suggest that the dynamical metastability of the micellar structures arises from an inversion of the energy landscape, in which the relaxation dynamics of one of the species induces a metastable phase for the other species.
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spelling pubmed-58878132018-04-19 Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures Pestana, Luis Ruiz Minnetian, Natalie Lammers, Laura Nielsen Head-Gordon, Teresa Chem Sci Chemistry When driven out of equilibrium, many diverse systems can form complex spatial and dynamical patterns, even in the absence of attractive interactions. Using kinetic Monte Carlo simulations, we investigate the phase behavior of a binary system of particles of dissimilar size confined between semiflexible planar surfaces, in which the nanoconfinement introduces a non-local coupling between particles, which we model as an activation energy barrier to diffusion that decreases with the local fraction of the larger particle. The system autonomously reaches a cyclical non-equilibrium state characterized by the formation and dissolution of metastable micelle-like clusters with the small particles in the core and the large ones in the surrounding corona. The power spectrum of the fluctuations in the aggregation number exhibits 1/f noise reminiscent of self-organized critical systems. We suggest that the dynamical metastability of the micellar structures arises from an inversion of the energy landscape, in which the relaxation dynamics of one of the species induces a metastable phase for the other species. Royal Society of Chemistry 2018-01-02 /pmc/articles/PMC5887813/ /pubmed/29675210 http://dx.doi.org/10.1039/c7sc03524a Text en This journal is © The Royal Society of Chemistry 2018 http://creativecommons.org/licenses/by-nc/3.0/ This article is freely available. This article is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported Licence (CC BY-NC 3.0)
spellingShingle Chemistry
Pestana, Luis Ruiz
Minnetian, Natalie
Lammers, Laura Nielsen
Head-Gordon, Teresa
Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures
title Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures
title_full Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures
title_fullStr Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures
title_full_unstemmed Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures
title_short Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures
title_sort dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5887813/
https://www.ncbi.nlm.nih.gov/pubmed/29675210
http://dx.doi.org/10.1039/c7sc03524a
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