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Register a new userDesigning morphology of separated phases in multicomponent liquid mixtures
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Added by
Andrej Ko\\v{s}mrlj
Publication date
2020
fields
Physics
and research's language is
English
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Phase separation of multicomponent liquid mixtures plays an integral part in many processes ranging from industry to cellular biology. In many cases the morphology of coexisting phases is crucially linked to the function of the separated mixture, yet it is unclear what determines morphology when multiple phases are present. We developed a graph theory approach to predict the topology of coexisting phases from a given set of surface energies (forward problem), enumerate all topologically distinct morphologies, and reverse engineer conditions for surface energies that produce the target morphology (inverse problem).
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Multicomponent systems are ubiquitous in nature and industry. While the physics of few-component liquid mixtures (i.e., binary and ternary ones) is well-understood and routinely taught in undergraduate courses, the thermodynamic and kinetic properties of $N$-component mixtures with $N>3$ have remained relatively unexplored. An example of such a mixture is provided by the intracellular fluid, in which protein-rich droplets phase separate into distinct membraneless organelles. In this work, we investigate equilibrium phase behavior and morphology of $N$-component liquid mixtures within the Flory-Huggins theory of regular solutions. In order to determine the number of coexisting phases and their compositions, we developed a new algorithm for constructing complete phase diagrams, based on numerical convexification of the discretized free energy landscape. Together with a Cahn-Hilliard approach for kinetics, we employ this method to study mixtures with $N=4$ and $5$ components. We report on both the coarsening behavior of such systems, as well as the resulting morphologies in three spatial dimensions. We discuss how the number of coexisting phases and their compositions can be extracted with Principal Component Analysis (PCA) and K-Means clustering algorithms. Finally, we discuss how one can reverse engineer the interaction parameters and volume fractions of components in order to achieve a range of desired packing structures, such as nested `Russian dolls and encapsulated Janus droplets.
Spontaneous liquid-liquid phase separation is commonly understood in terms of phenomenological mean-field theories. These theories correctly predict the structural features of the fluid at sufficiently long time scales and wavelengths. However, these conditions are not met in various examples in biology and materials science where the mixture is slowly destabilised, and phase separation takes place close to the critical point. Using kinetic Monte Carlo and molecular dynamics simulations of a binary surface fluid under these conditions, we show that the characteristic length scale of the emerging structure decreases, in 2D, with the 4/15 dynamic critical exponent of the quench rate rather than the mean-field 1/6th power. Hence, the dynamics of cluster formation governed by thermodynamically undriven Brownian motion is much more sensitive on the rate of destabilisation than expected from mean-field theory. We discuss the expected implications of this finding to 3D systems with ordering liquid crystals, as well as phase-separating passive or active particles.
Recently the supercooled Wahnstrom binary Lennard-Jones mixture was partially crystallized into ${rm MgZn_2}$ phase crystals in lengthy Molecular Dynamics simulations. We present Molecular Dynamics simulations of a modified Kob-Andersen binary Lennard-Jones mixture that also crystallizes in lengthy simulations, here however by forming pure fcc crystals of the majority component. The two findings motivate this paper that gives a general thermodynamic and kinetic treatment of the stability of supercooled binary mixtures, emphasizing the importance of negative mixing enthalpy whenever present. The theory is used to estimate the crystallization time in a Kob-Andersen mixture from the crystallization time in a series of relared systems. At T=0.40 we estimate this time to be 5$times 10^{7}$ time units ($approx 1. ms$). A new binary Lennard-Jones mixture is proposed that is not prone to crystallization and faster to simulate than the two standard binary Lennard-Jones mixtures; this is obtained by removing the like-particle attractions by switching to Weeks-Chandler-Andersen type potentials, while maintaining the unlike-particle attraction.
Lattice Boltzmann simulations of liquid-gas systems are believed to be restricted to modest density ratios of less than 10. In this article we show that reducing the speed of sound and, just as importantly, the interfacial contributions to the pressure allows lattice Boltzmann simulations to achieve high density ratios of 1000 or more. We also present explicit expressions for the limits of the parameter region in which the method gives accurate results. There are two separate limiting phenomena. The first is the stability of the bulk liquid phase. This consideration is specific to lattice Boltzmann methods. The second is a general argument for the interface discretization that applies to any diffuse interface method.
If a fluctuating medium is confined, the ensuing perturbation of its fluctuation spectrum generates Casimir-like effective forces acting on its confining surfaces. Near a continuous phase transition of such a medium the corresponding order parameter fluctuations occur on all length scales and therefore close to the critical point this effect acquires a universal character, i.e., to a large extent it is independent of the microscopic details of the actual system. Accordingly it can be calculated theoretically by studying suitable representative model systems. We report on the direct measurement of critical Casimir forces by total internal reflection microscopy (TIRM), with femto-Newton resolution. The corresponding potentials are determined for individual colloidal particles floating above a substrate under the action of the critical thermal noise in the solvent medium, constituted by a binary liquid mixture of water and 2,6-lutidine near its lower consolute point. Depending on the relative adsorption preferences of the colloid and substrate surfaces with respect to the two components of the binary liquid mixture, we observe that, upon approaching the critical point of the solvent, attractive or repulsive forces emerge and supersede those prevailing away from it. Based on the knowledge of the critical Casimir forces acting in film geometries within the Ising universality class and with equal or opposing boundary conditions, we provide the corresponding theoretical predictions for the sphere-planar wall geometry of the experiment. The experimental data for the effective potential can be interpreted consistently in terms of these predictions and a remarkable quantitative agreement is observed.
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