Origin and detection of microstructural clustering in fluids with spatial-range competitive interactions

Jadrich, Ryan B.; Bollinger, Jonathan A.; Johnston, Keith P.; Truskett, Thomas M.

doi:10.1103/physreve.91.042312

Cited by 37 publications

(60 citation statements)

References 27 publications

(51 reference statements)

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“…31 It seems intuitive that this disparity between the IBI-optimized and SALR potentials is responsible for the former's enhanced cluster size-specificity (even under compression). This approach was successfully applied to discover a new class of pair potentials that stabilize ideal cluster (IC) fluids, comprised of long-lived, monodisperse, spherical fluid droplets with good center of mass mobility.…”

Section: Discussionmentioning

confidence: 99%

“…[30][31][32][33][34][35][36][37][38] Specifically, we compare IC results with those from a ternary mixture model developed in a previous study 31 that can generate both amorphous and microcrystalline clusters. [30][31][32][33][34][35][36][37][38] Specifically, we compare IC results with those from a ternary mixture model developed in a previous study 31 that can generate both amorphous and microcrystalline clusters.…”

Section: Salr Model Systemsmentioning

confidence: 99%

“…As is customary, [30][31][32][33][34][35][36][37][38] two particles are considered part of the same cluster if at least one of the following conditions are met: (1) their centers are within a pre-defined cutoff distance r cut , making them direct neighbors; and/or (2) their centers are both within r cut of one (or more) other particle(s), i.e., are connected via some percolating pathway. As is customary, [30][31][32][33][34][35][36][37][38] two particles are considered part of the same cluster if at least one of the following conditions are met: (1) their centers are within a pre-defined cutoff distance r cut , making them direct neighbors; and/or (2) their centers are both within r cut of one (or more) other particle(s), i.e., are connected via some percolating pathway.…”

Section: Cluster-size Distribution and Bond Order Analysismentioning

confidence: 99%

“…It comprises two steps: generation of a configurational ensemble of target microstructures via simulations using an artificially complex, many-body interaction chosen to guarantee assembly of the desired morphology, and then use of a tool from systematic coarse-graining [24][25][26][27][28][29] to reduce the many-body interaction to an effective pair potential. [30][31][32][33][34][35][36][37][38]44,45 Various functional forms for the attractions have been studied (modeling, e.g., polymer-mediated depletion forces between colloids), typically in combination with a repulsive Yukawa tail to model weakly screened Coulombic interactions. As a first application of this methodology, we attempt to inverse design a pairwise potential that forms a fluid of ''ideal'' amorphous equilibrium clusters of prescribed size.…”

Section: Introductionmentioning

confidence: 99%

“…In the present work, we adopt iterative Boltzmann inversion (IBI) for the latter step, which uniquely determines the pair potential that will generate the radial distribution function (RDF) of the target ensemble at equilibrium. 30,31,46 Although the SALR model qualitatively captures the effective pair potential and equilibrium cluster behavior seen in some types of experimental systems (e.g., mixtures of charged-stabilized colloids with weakly interacting polymers), it does not generate microstructures reflecting properties typically expected in the idealized picture 47 of such cluster phases [31][32][33][34][35][36][37][38]45,46 that are found in other experimental systems, 48,49 which we denote here as ideal cluster (IC) fluids: particle assemblies that are monodisperse, spherical, long-lived, and fluid-like in terms of inter-and intra-cluster structure and mobility. Clustered fluids of colloidal particles have attracted considerable interest due to their novel multiscale structure, their rich dynamic and rheological properties, and their potential functionality.…”

Section: Introductionmentioning

confidence: 99%

See 4 more Smart Citations

Equilibrium cluster fluids: pair interactions via inverse design

et al. 2015

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Inverse methods of statistical mechanics are becoming productive tools in the design of materials with specific microstructures or properties. While initial studies have focused on solid-state design targets (e.g., assembly of colloidal superlattices), one can alternatively design fluid states with desired morphologies. This work addresses the latter and demonstrates how a simple iterative Boltzmann inversion strategy can be used to determine the isotropic pair potential that reproduces the radial distribution function of a fluid of amorphous clusters with prescribed size. The inverse designed pair potential of this "ideal" cluster fluid, with its broad attractive well and narrow repulsive barrier at larger separations, is qualitatively different from the so-called SALR form most commonly associated with equilibrium cluster formation in colloids, which features short-range attractive (SA) and long-range repulsive (LR) contributions. These differences reflect alternative mechanisms for promoting cluster formation with an isotropic pair potential, and they in turn produce structured fluids with qualitatively different static and dynamic properties. Specifically, equilibrium simulations show that the amorphous clusters resulting from the inverse designed potentials display more uniformity in size and shape, and they also show greater spatial and temporal resolution than those resulting from SALR interactions.

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Section: Discussionmentioning

confidence: 99%

Section: Salr Model Systemsmentioning

confidence: 99%

Section: Cluster-size Distribution and Bond Order Analysismentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Equilibrium cluster fluids: pair interactions via inverse design

et al. 2015

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Aggregate formation in fluids with bounded repulsive core and competing interactions

Malescio

Sciortino

2020

Journal of Molecular Liquids

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Clustering in Mixtures of SALR Particles and Hard Spheres with Cross Attraction

et al. 2022

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Self-assembling complex fluids are often modeled as particles with effective competing isotropic interactions, combining a short-range attraction (SA) followed by a longer-range repulsion (LR). For moderately low temperatures and densities, SALR particles form clusters in equilibrium, at least provided that the potential parameters are appropriate. Here we inquire into the possibility that cluster formation in SALR fluids might be pushed by a foreign species even under thermodynamic conditions that would not allow for clusterization of the pure system. To this aim, we study by Monte Carlo simulations a mixture of hard-sphere two-Yukawa particles and hard spheres, with a cross interaction modeled by a square-well attraction, and we investigate the conditions of clustering in terms of strength of attraction and relative concentration of the two species. We find that clusters can occur in the mixture for the same temperature and density where the pure SALR fluid is almost structureless. In particular, we single out a cross attraction such that clusters are formed with a SALR concentration as low as 5%. We also find a situation where nearly pure droplets of hard spheres are held together by a shell of SALR particles. Conversely, we show that clustering can be undermined in the mixture under conditions for which this process takes place in the parent SALR fluid. Using a simple criterion, based on the second virial coefficients of the attractive part of interaction potentials (the so-called “reference attractive fluids”), we are able to predict accurately whether clustering is favored (or hindered) in the mixture, as compared to the pure SALR fluid.

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Origin and detection of microstructural clustering in fluids with spatial-range competitive interactions

Cited by 37 publications

References 27 publications

Equilibrium cluster fluids: pair interactions via inverse design

Equilibrium cluster fluids: pair interactions via inverse design

Aggregate formation in fluids with bounded repulsive core and competing interactions

Clustering in Mixtures of SALR Particles and Hard Spheres with Cross Attraction

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