Colloids immersed in a critical binary liquid mixture are subject to critical Casimir forces (CCFs) because they confine its concentration fluctuations and influence the latter via effective surface fields. To date, CCFs have only been studied in thermodynamic equilibrium. However, due to the critical slowing down, the order parameter around a particle can easily be perturbed by any motion of the colloid or by solvent flow. This leads to significant but largely unexplored changes in the CCF. Here we study the drag force on a single colloidal particle moving in a near-critical fluid mixture and the relative motion of two colloids due to the CCF acting on them. In order to account for the kinetic couplings among the order parameter field, the solvent velocity field, and the particle motion, we use a fluid particle dynamics method. These studies extend the understanding of CCFs from thermal equilibrium to non-equilibrium processes, which are relevant to current experiments, and show the emergence of significant effects near the critical point.
In net-neutral systems correlations between charge fluctuations generate strong attractive thermal Casimir forces and engineering these forces to optimize nanodevice performance is an important challenge. We show how the normal and lateral thermal Casimir forces between two plates containing Brownian charges can be modulated by decorrelating the system through the application of an electric field, which generates a nonequilibrium steady state with a constant current in one or both plates, reducing the ensuing fluctuation-generated normal force while at the same time generating a lateral drag f…
We show that critical Casimir effects can be accessed through direct simulation of a model binary fluid passing through the demixing transition. We work in the semi grand canonical ensemble, in slab geometry, in which the Casimir force appears as the excess of the generalized pressure, $P_{\bot}-nμ$. The excesses of the perpendicular pressure, $P_{\bot}$, and of $nμ$, are individually of much larger amplitude. A critical pressure anisotropy is observed between forces parallel and perpendicular to the confinement direction, which collapses onto a universal scaling function closely related to th…
A model for the pair distribution function of nonequilibrium hard-core fluids is proposed based on a model for the effect of velocity correlations on the structure. Good agreement is found with molecular dynamics simulations of granular fluids and of sheared elastic hard spheres. It is argued that the incorporation of velocity correlations are crucial to correctly modeling atomic scale structure in nonequilibrium fluids.
We study fluctuation-induced interaction in confined fluids above the isotropic-lamellar transition. At an ideal continuous transition, the disjoining pressure has the asymptotic form $Π(d\to\infty)\approx -C k_BT q_0^2/d$, where $d$ is the interwall distance, $q_0$ is the wavenumber of the scattering peak, and $C= 1/(4π)$ in the strong anchoring limit. The long-rangedness is enhanced due to continuous distribution of soft modes in the ${\bf q}$-space. An unconventionally strong Casimir force with a range of several lamella thicknesses is realistic above the transition. We also find an oscilla…
It is shown that the equilibrium Generalized Mean Spherical Model of fluid structure may be extended to nonequilibrium states with equation of state information used in equilibrium replaced by an exact condition on the two-body distribution function. The model is applied to the homogeneous cooling state of granular fluids and upon comparison to molecular dynamics simulations is found to provide an accurate picture of the pair distribution function.
We study the effective interaction between two ellipsoidal particles at the interface of two fluid phases which are mediated by thermal fluctuations of the interface. In this system the restriction of the long--ranged interface fluctuations by particles gives rise to fluctuation--induced forces which are equivalent to interactions of Casimir type and which are anisotropic in the interface plane. Since the position and the orientation of the colloids with respect to the interface normal may also fluctuate, this system is an example for the Casimir effect with fluctuating boundary conditions. In…
The notion of fluctuation-induced forces is generalized to the cases where the fluctuations have nonequilibrium origin. It is shown that a net force is exerted on a single flat plate that restricts scale-free fluctuations of a scalar field in a temperature gradient. This force tends to push the object to the colder regions, which is a manifestation of thermophoresis or the Soret effect. In the classic two-plate geometry, it is shown that the Casimir forces exerted on the two plates differ from each other, and thus the Newton's third law is violated.
We calculate the Casimir stresses in a thin layer of active fluid with nematic order. By using a stochastic hydrodynamic approach for an active fluid layer of finite thickness $L$, we generalize the Casimir stress for nematic liquid crystals in thermal equilibrium to active systems. We show that the active Casimir stress differs significantly from its equilibrium counterpart. For contractile activity, the active Casimir stress, although attractive like its equilibrium counterpart, diverges logarithmically as $L$ approaches a threshold of the spontaneous flow instability from below. In contrast…
We investigate the critical behavior of a near-critical fluid confined between two parallel plates in contact with a reservoir by calculating the order parameter profile and the Casimir amplitudes (for the force density and for the grand potential). Our results are applicable to one-component fluids and binary mixtures. We assume that the walls absorb one of the fluid components selectively for binary mixtures. We propose a renormalized local functional theory accounting for the fluctuation effects. Analysis is performed in the plane of the temperature T and the order parameter in the reservoi…
We present a detailed study of the kinetic cluster growth process during gelation of weakly attractive colloidal particles by means of experiments on critical Casimir attractive colloidal systems, simulations and analytical theory. In the experiments and simulations, we follow the mean coordination number of the particles during the growth of clusters to identify an attractive-strength independent cluster evolution as a function of mean coordination number. We relate this cluster evolution to the kinetic attachment and detachment rates of particles and particle clusters. We find that single-pa…
The fluctuation-induced, Casimir-like interaction between two parallel rods of length L adsorbed on a fluid membrane is calculated analytically at short separations d<<L. The rods are modeled as constraints imposed on the membrane curvature along a straight line. This allows to define four types of rods, according to whether the membrane can twist along the rod and/or curve across it. For stiff constraints, all the interaction potentials between the different types of rods are attractive and proportional to L/d. Two of the four types of rods are then equivalent, which yields six universal Casi…
We study numerically phase separation in a binary fluid subject to an applied shear flow in two dimensions, with full hydrodynamics. To do so, we introduce a mixed finite-differencing/spectral simulation technique, with a transformation to render trivial the implementation of Lees-Edwards sheared periodic boundary conditions. For systems with inertia, we reproduce the nonequilibrium steady states reported in a recent lattice Boltzmann study. The domain coarsening that would occur in zero shear is arrested by the applied shear flow, which restores a finite domain size set by the inverse shear r…
Nonequilibrium steady states in an open system connecting two reservoirs of platelike colloidal particles are investigated by means of a recently proposed phenomenological dynamic density functional theory [M. Bier and R. van Roij, Phys. Rev. E 76, 021405 (2007)]. The platelike colloidal particles are approximated within the Zwanzig model of restricted orientations, which exhibits an isotropic-nematic bulk phase transition. Inhomogeneities of the local chemical potential generate a diffusion current which relaxes to a nonvanishing value if the two reservoirs coupled to the system sustain diffe…
We discuss the fluctuation-induced force, a finite-temperature analog of the Casimir force, between two inclusions embedded in a fluid membrane under tension. We suggest a method to calculate this Casimir interaction in the most general case, where membrane fluctuations are governed by the combined action of surface tension, bending modulus, and the Gaussian rigidity. We find that the surface tension strongly modifies the power law in the separation dependence of the Casimir interaction. This results in a strong suppression of the Casimir force at separations beyond a characteristic length, wh…
We have performed small-angle light-scattering measurements of the static structure factor of a critical binary mixture undergoing diffusive partial remixing. An uncommon scattering geometry integrates the structure factor over the sample thickness, allowing different regions of the concentration profile to be probed simultaneously. Our experiment shows the existence of interface capillary waves throughout the macroscopic evolution to an equilibrium interface, and allows to derive the time evolution of surface tension. Interfacial properties are shown to attain their equilibrium values quickly…
Our previous article [Phys. Rev. Lett. 104, 060401 (2010)] predicted that Casimir forces induced by the material-dispersion properties of certain dielectrics can give rise to stable configurations of objects. This phenomenon was illustrated via a dicluster configuration of non-touching objects consisting of two spheres immersed in a fluid and suspended against gravity above a plate. Here, we examine these predictions from the perspective of a practical experiment and consider the influence of non-additive, three-body, and nonzero-temperature effects on the stability of the two spheres. We conc…
We study the behavior of fluids, confined by geometrically structured substrates, upon approaching a critical point at T = Tc in their bulk phase diagram. As generic substrate structures periodic arrays of wedges and ridges are considered. Based on general renormalization group arguments we calculate, within mean field approximation, the universal scaling functions for order parameter profiles of a fluid close to a single structured substrate and discuss the decay of its spatial variation into the bulk. We compare the excess adsorption at corrugated substrates with the one at planar walls. The…
The nonequilibrium dynamics of a binary Lennard-Jones mixture in a simple shear flow is investigated by means of molecular dynamics simulations. The range of temperature investigated covers both the liquid, supercooled and glassy states, while the shear rate covers both the linear and nonlinear regimes of rheology. The results can be interpreted in the context of a nonequilibrium, schematic mode-coupling theory developed recently, which makes the theory applicable to a wide range of soft glassy materials. The behavior of the viscosity is first investigated. In the nonlinear regime, strong shea…
Granular fluids consist of collections of activated mesoscopic or macroscopic particles (e.g., powders or grains) whose flows often appear similar to those of normal fluids. To explore the qualitative and quantitative description of these flows an idealized model for such fluids, a system of smooth inelastic hard spheres, is considered. The single feature distinguishing granular and normal fluids being explored in this way is the inelasticity of collisions. The dominant differences observed in real granular fluids are indeed captured by this feature. Following a brief introductory description …
We investigate the nonequilibrium behavior of a one-dimensional binary fluid on the basis of Boltzmann equation, using an infinitely strong shock wave as probe. Density, velocity and temperature profiles are obtained as a function of the mixture mass ratio μ. We show that temperature overshoots near the shock layer, and that heavy particles are denser, slower and cooler than light particles in the strong nonequilibrium region around the shock. The shock width w(μ), which characterizes the size of this region, decreases as w(μ) ~ μ^{1/3} for μ-->0. In this limit, two very different length scale…
We use extensive computer simulations to probe local thermodynamic equilibrium (LTE) in a quintessential model fluid, the two-dimensional hard-disks system. We show that macroscopic LTE is a property much stronger than previously anticipated, even in the presence of important finite size effects, revealing a remarkable bulk-boundary decoupling phenomenon in fluids out of equilibrium. This allows us to measure the fluid's equation of state in simulations far from equilibrium, with an excellent accuracy comparable to the best equilibrium simulations. Subtle corrections to LTE are found in the fl…
We study the fluctuation-induced, time-dependent force between two plates immersed in a fluid driven out of equilibrium mechanically by harmonic vibrations of one of the plates. Considering a simple Langevin dynamics for the fluid, we explicitly calculate the fluctuation-induced force acting on the plate at rest. The time-dependence of this force is characterized by a positive lag time with respect to the driving, indicating a finite speed of propagation of stress through the medium, reminiscent of waves. We obtain two distinctive contributions to the force, where one may be understood as dire…
We study the glassy dynamics taking place in dense assemblies of athermal active particles that are driven solely by a nonequilibrium self-propulsion mechanism. Active forces are modeled as an Ornstein-Uhlenbeck stochastic process, characterized by a persistence time and an effective temperature, and particles interact via a Lennard-Jones potential that yields well-studied glassy behavior in the Brownian limit, obtained as the persistence time vanishes. By increasing the persistence time, the system departs more strongly from thermal equilibrium and we provide a comprehensive numerical analysi…
The Chapman-Enskog method of solution of kinetic equations, such as the Boltzmann equation, is based on an expansion in gradients of the deviations fo the hydrodynamic fields from a uniform reference state (e.g., local equilibrium). This paper presents an extension of the method so as to allow for expansions about \emph{arbitrary}, far-from equilibrium reference states. The primary result is a set of hydrodynamic equations for studying variations from the arbitrary reference state which, unlike the usual Navier-Stokes hydrodynamics, does not restrict the reference state in any way. The method …
We investigate the forces exerted on embedded inclusions by a fluid medium with long-range correlations, described by an effective scalar field theory. Such forces are the basis for the medium-mediated Casimir-like force. To study these forces beyond thermal average, it is necessary to define them in each microstate of the medium. Two different definitions of these forces are currently used in the literature. We study the assumptions underlying them. We show that only the definition that uses the stress tensor of the medium gives the sought-after force exerted by the medium on an embedded incl…
We have carried out nonequilibrium molecular dynamics simulations of a system of crosslinked particles under shear flow conditions. As the fraction of crosslinks $p$ is increased the system approaches a gel point at which the shear viscosity $η$ and the first and second normal stress coefficients $Ψ_1$ and $Ψ_2$ diverge. All three quantities seem to diverge with a power law form: $η\sim ε^{-s}$, $Ψ_{1,2}\simε^{-λ}$ where $ε=p_c-p$ and $s\approx 0.7$ and $λ\approx 3.15$ in three dimensions and $s\approx 2.0$ and $λ\approx 6.0$ in two dimensions.
The classical Coulomb gas model has served as one of the most versatile frameworks in statistical physics, connecting a vast range of phenomena across many different areas. Nonequilibrium generalisations of this model have so far been studied much more scarcely. With the abundance of contemporary research into active and driven systems, one would naturally expect that such generalisations of systems with long-ranged Coulomb-like interactions will form a fertile playground for interesting developments. Here, we present two examples of novel macroscopic behaviour that arise from nonequilibrium f…
Fluctuation-induced forces occur generically when long-ranged correlations (e.g., in fluids) are confined by external bodies. In classical systems, such correlations require specific conditions, e.g., a medium close to a critical point. On the other hand, long-ranged correlations appear more commonly in certain non-equilibrium systems with conservation laws. Consequently, a variety of non-equilibrium fluctuation phenomena, including fluctuation-induced forces, have been discovered and explored recently. Here, we address a long-standing problem of non-equilibrium critical Casimir forces emergin…
We perform a direct numerical simulation (DNS) of the forced, incompressible two-dimensional Navier-Stokes equation coupled with the FENE-P equations for the polymer-conformation tensor. The forcing is such that, without polymers and at low Reynolds numbers $\mbox{Re}$, the film attains a steady state that is a square lattice of vortices and anti-vortices. We find that, as we increase the Weissenberg number $\mbox{Wi}$, a sequence of nonequilibrium phase transitions transforms this lattice, first to spatially distorted, but temporally steady, crystals and then to a sequence of crystals that os…
We study the critical Casimir interaction between two spherical colloids immersed in a binary liquid mixture close to its critical demixing point. The surface of each colloid prefers one species of the mixture with the exception of a circular patch of arbitrary size, where the other species is preferred. For such objects we calculate, within the Derjaguin approximation, the scaling function describing the critical Casimir potential, and we use it to derive the scaling functions for all components of the forces and torques acting on both colloids. The results are compared with available experim…
We introduce a nonequilibrium off--lattice model for anisotropic phenomena in fluids. This is a Lennard--Jones generalization of the driven lattice--gas model in which the particles' spatial coordinates vary continuously. A comparison between the two models allows us to discuss some exceptional, hardly realistic features of the original discrete system --which has been considered a prototype for nonequilibrium anisotropic phase transitions. We thus help to clarify open issues, and discuss on the implications of our observations for future investigation of anisotropic phase transitions.
The critical Casimir force (CCF) arises from confining fluctuations in a critical fluid and thus it is a fluctuating quantity itself. While the mean CCF is universal, its (static) variance has previously been found to depend on the microscopic details of the system which effectively set a large-momentum cutoff in the underlying field theory, rendering it potentially large. This raises the question how the properties of the force variance are reflected in experimentally observable quantities, such as the thickness of a wetting film or the position of a suspended colloidal particle. Here, based …
In modeling nonequilibrium systems one usually starts with a definition of the microscopic dynamics, e.g., in terms of transition rates, and then derives the resulting macroscopic behavior. We address the inverse question for a class of steady state systems, namely complex fluids under continuous shear flow: how does an externally imposed shear current affect the microscopic dynamics of the fluid? The answer can be formulated in the form of invariant quantities, exact relations for the transition rates in the nonequilibrium steady state, as discussed in a recent letter [A. Baule and R. M. L. E…
In a recent study [Phys. Rev. E \textbf{94}, 022103 (2016)] it has been shown that, for a fluid film subject to critical adsorption, the resulting critical Casimir force (CCF) may significantly depend on the thermodynamic ensemble. Here, we extend that study by considering fluid films within the so-called ordinary surface universality class. We focus on mean-field theory, within which the OP profile satisfies Dirichlet boundary conditions and produces a nontrivial CCF in the presence of external bulk fields or, respectively, a nonzero total order parameter within the film. Our analytical resul…
In this work, we investigate the dynamics of the number density fluctuations of a dilute suspension of active particles in a linear viscoelastic fluid. We propose a model for the frequency-dependent diffusion coefficient of the active particles, which captures the effect of rotational diffusion on the persistence of their self-propelled motion and the viscoelasticity of the medium. Using fluctuating hydrodynamics, the linearized equations for the active suspension are derived, from which we calculate its dynamic structure factor and the corresponding intermediate scattering function. For a Max…
Using general scaling arguments combined with mean-field theory we investigate the critical ($T \simeq T_c$) and off-critical ($T\ne T_c$) behavior of the Casimir forces in fluid films of thickness $L$ governed by dispersion forces and exposed to long-ranged substrate potentials which are taken to be equal on both sides of the film. We study the resulting effective force acting on the confining substrates as a function of $T$ and of the chemical potential $μ$. We find that the total force is attractive both below and above $T_c$. If, however, the direct substrate-substrate contribution is subt…
Effective Casimir forces induced by thermal fluctuations in the vicinity of bulk critical points are studied by means of Monte Carlo simulations in three-dimensional systems for film geometries and within the experimentally relevant Ising and XY universality classes. Several surface universality classes of the confining surfaces are considered, some of which are relevant for recent experiments. A novel approach introduced previously EPL 80, 60009 (2007), based inter alia on an integration scheme of free energy differences, is utilized to compute the universal scaling functions of the critical …
We develop a general theory for describing phase coexistence between nonequilibrium steady states in Brownian systems, based on power functional theory (M. Schmidt and J.M. Brader, J. Chem. Phys. 138, 214101 (2013)). We apply the framework to the special case of fluid-fluid phase separation of active soft sphere swimmers. The central object of the theory, the dissipated free power, is calculated via computer simulations and compared to a simple analytical approximation. The theory describes well the simulation data and predicts motility-induced phase separation due to avoidance of dissipative …
The dynamical arrest of attractive colloidal particles into out-of-equilibrium structures, known as gelation, is central to biophysics, materials science, nanotechnology, and food and cosmetic applications, but a complete understanding is lacking. In particular, for intermediate particle density and attraction, the structure formation process remains unclear. Here, we show that the gelation of short-range attractive particles is governed by a nonequilibrium percolation process. We combine experiments on critical Casimir colloidal suspensions, numerical simulations, and analytical modeling with…
To develop an understanding of recent experiments on the turbulence-induced melting of a periodic array of vortices in a thin fluid film, we perform a direct numerical simulation of the two-dimensional Navier-Stokes equations forced such that, at low Reynolds numbers, the steady state of the film is a square lattice of vortices. We find that, as we increase the Reynolds number, this lattice undergoes a series of nonequilibrium phase transitions, first to a crystal with a different reciprocal lattice and then to a sequence of crystals that oscillate in time. Initially the temporal oscillations …
We derive the transient-time correlation function (TTCF) expression for the computation of phase variables of inhomogenous confined atomistic fluids undergoing boundary-driven planar shear (Couette) flow at constant pressure. Using nonequilibrium molecular dynamics simulations, we then apply the TTCF formalism to the computation of the shear stress and the slip velocity for atomistic fluids at realistic low shear rates, in systems under constant pressure and constant volume. We show that, compared to direct averaging of multiple trajectories, the TTCF method dramatically improves the accuracy …
Patterns are quotidian in nature. Distinct multiscale patterns are generally a consequence of nonequilibrium dynamical processes associated with mechanical or hydrodynamic instabilities. In this thesis, I report experimental investigations on pattern formation in a few examples of fluid and granular systems, and uncover the underlying mechanisms that give rise to those patterns. Leidenfrost drops are known to experience star-shaped oscillations with little damping. However, the underlying mechanism remains unclear. Here I report that the hydrodynamic coupling between the rapid evaporated vapor…
Using field-theoretical methods and exploiting conformal invariance, we study Casimir forces at tricritical points exerted by long-range fluctuations of the order-parameter field. Special attention is paid to the situation where the symmetry is broken by the boundary conditions (extraordinary transition). Besides the parallel-plate configuration, we also discuss the geometries of two separate spheres and a single sphere near a planar wall, which may serve as a model for colloidal particles immersed in a fluid. In the concrete case of ternary mixtures a quantitative comparison with critical Cas…
A nonlinear two-fluid stochastic hydrodynamical description of velocity and concentration fluctuations in sedimenting suspensions is constructed, and analyzed using self-consistent (SC) and renormalization group (RG) methods. The advection of particles by velocity fluctuations is shown to be ``relevant'' in all dimensions $d < 6$ . Both RG and SC analyses predict a strong reduction in the dependence of velocity fluctuations on system-size $L$ relative to the $L^{1/2}$ obtained in the linearized theory of Caflisch and Luke [Phys. Fluids {\bf 28}, 785 (1985)]. This is an important step towards r…
We investigate the response of a dense monodisperse quasi-two-dimensional (q2D) colloid suspension when a particle is dragged by a constant velocity optical trap. Consistent with microrheological studies of other geometries, the perturbation induces a leading density wave and trailing wake, and we use Stokesian Dynamics (SD) simulations to parse direct colloid-colloid and hydrodynamic interactions. We go on to analyze the underlying individual particle-particle collisions in the experimental images. The displacements of particles form chains reminiscent of stress propagation in sheared granula…
Composite colloidal assembly by critical Casimir forces
University of Amsterdam（阿姆斯特丹大学）；Wageningen University and Research（瓦赫宁根大学和研究机构）；Polish Academy of Sciences（波兰科学院）；Max-Planck-Institut für Intelligente Systeme（马克斯·普朗克智能系统研究所）
