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

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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. 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.

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

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Publication details

The article was received on 11 Aug 2017, accepted on 26 Dec 2017 and first published on 02 Jan 2018


Article type: Edge Article
DOI: 10.1039/C7SC03524A
Citation: Chem. Sci., 2018, Advance Article
  • Open access: Creative Commons BY-NC license
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    Dynamical inversion of the energy landscape promotes non-equilibrium self-assembly of binary mixtures

    L. R. Pestana, N. Minnetian, L. N. Lammers and T. Head-Gordon, Chem. Sci., 2018, Advance Article , DOI: 10.1039/C7SC03524A

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