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Self-assembly in chains, rings, and branches: a single component system with two critical points

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We study the interplay between phase separation and self-assembly in chains, rings, and branched structures in a model of particles with dissimilar patches. We extend Wertheim's first order perturbation theory to include the effects of ring formation and to theoretically investigate the thermodynamics of the model. We find a peculiar shape for the vapor-liquid coexistence, featuring reentrant behavior in both phases and two critical points, despite the single-component nature of the system. The emergence of the lower critical point is caused by the self-assembly of rings taking place in the vapor, generating a phase with lower energy and lower entropy than the liquid. Monte Carlo simulations of the same model fully support these unconventional theoretical predictions.

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Agências financiadoras: FCT - PEstOE/FIS/UI0618/2011; PTDC/FIS/098254/2008 ERC-PATCHYCOLLOIDS e MIUR-PRIN

Keywords

Directional Attractive Forces Dipolar Hard-Spheres Monte-Carlo Associating Fluids Model Saft Particles Clusters Sites

Citation

ROVIGATTI, Lorenzo; TAVARES, José Maria; SCIORTINO, Francesco - Self-Assembly in Chains, Rings, and Branches: A Single Component System with Two Critical Points. Physical Review Letters. Vol. 111, nr. 16 (2013).

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Amer Physical SOC

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