We present the first systematic application of the integral equation implementation of the replica method to the study of arrested states in fluids with microscopic competing interactions (short-range attractive and long-range repulsive, SALR), as exemplified by the prototype Lennard-Jones-Yukawa model. Using a wide set of potential parameters, we provide as many as 11 different phase diagrams on the density (ρ)-temperature (T) plane, embodying both the cluster-phase boundary, TC(ρ), and the locus below which arrest takes place, TD(ρ). We describe how the interplay between TC and TD-with the former falling on top of the other, or the other way around, depending on thermodynamic conditions and potential parameters-gives rise to a rich variety of non-ergodic states interspersed with ergodic ones, of which both the building blocks are clusters or single particles. In a few cases, we find that the TD locus does not extend all over the density range subtended by the TC envelope; under these conditions, the λ-line is within reach of the cluster fluid, with the ensuing possibility to develop ordered microphases. Whenever a comparison is possible, our predictions favorably agree with previous numerical results. Thereby, we demonstrate the reliability and effectiveness of our scheme to provide a unified theoretical framework for the study of arrested states in SALR fluids, irrespective of their nature.
Arrested states in colloidal fluids with competing interactions: A static replica study
Costa, Dino;Munao', Gianmarco;Malescio, GianpietroPenultimo
;Prestipino, SantiUltimo
2024-01-01
Abstract
We present the first systematic application of the integral equation implementation of the replica method to the study of arrested states in fluids with microscopic competing interactions (short-range attractive and long-range repulsive, SALR), as exemplified by the prototype Lennard-Jones-Yukawa model. Using a wide set of potential parameters, we provide as many as 11 different phase diagrams on the density (ρ)-temperature (T) plane, embodying both the cluster-phase boundary, TC(ρ), and the locus below which arrest takes place, TD(ρ). We describe how the interplay between TC and TD-with the former falling on top of the other, or the other way around, depending on thermodynamic conditions and potential parameters-gives rise to a rich variety of non-ergodic states interspersed with ergodic ones, of which both the building blocks are clusters or single particles. In a few cases, we find that the TD locus does not extend all over the density range subtended by the TC envelope; under these conditions, the λ-line is within reach of the cluster fluid, with the ensuing possibility to develop ordered microphases. Whenever a comparison is possible, our predictions favorably agree with previous numerical results. Thereby, we demonstrate the reliability and effectiveness of our scheme to provide a unified theoretical framework for the study of arrested states in SALR fluids, irrespective of their nature.Pubblicazioni consigliate
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