Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures
Abstract
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. Finally, 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.
- Authors:
-
- Chemical Sciences Division, Lawrence Berkeley National Laboratory, University of California, Berkeley, USA
- Department of Chemistry, University of California, Berkeley, USA
- Earth and Environmental Science Area, Lawrence Berkeley National Laboratory, University of California, Berkeley, USA
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1416403
- Alternate Identifier(s):
- OSTI ID: 1434007
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Name: Chemical Science Journal Volume: 9 Journal Issue: 6; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry (RSC)
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Pestana, Luis Ruiz, Minnetian, Natalie, Lammers, Laura Nielsen, and Head-Gordon, Teresa. Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures. United Kingdom: N. p., 2018.
Web. doi:10.1039/C7SC03524A.
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. United Kingdom. https://doi.org/10.1039/C7SC03524A
Pestana, Luis Ruiz, Minnetian, Natalie, Lammers, Laura Nielsen, and Head-Gordon, Teresa. Mon .
"Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures". United Kingdom. https://doi.org/10.1039/C7SC03524A.
@article{osti_1416403,
title = {Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures},
author = {Pestana, Luis Ruiz and Minnetian, Natalie and Lammers, Laura Nielsen and Head-Gordon, Teresa},
abstractNote = {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. Finally, 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.},
doi = {10.1039/C7SC03524A},
journal = {Chemical Science},
number = 6,
volume = 9,
place = {United Kingdom},
year = {Mon Jan 01 00:00:00 EST 2018},
month = {Mon Jan 01 00:00:00 EST 2018}
}
https://doi.org/10.1039/C7SC03524A
Web of Science
Figures / Tables:
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