We study the relaxation of a single colloidal sphere which is periodically driven between two nonequilibrium steady states. Experimentally, this is achieved by driving the particle along a toroidal trap imposed by scanned optical tweezers. We find that the relaxation time after which the probability distributions have been relaxed is identical to that obtained by a steady state measurement. In quantitative agreement with theoretical calculations the relaxation time strongly increases when driving the system further away from thermal equilibrium.
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 present a direct experimental measurement of an effective temperature in a colloidal glass of Laponite, using a micrometric bead as a thermometer. The nonequilibrium fluctuation-dissipation relation, in the particular form of a modified Einstein relation, is investigated with diffusion and mobility measurements of the bead embedded in the glass. We observe an unusual non-monotonic behavior of the effective temperature : starting from the bath temperature, it is found to increase up to a maximum value, and then decreases back, as the system ages. We show that the observed deviation from the …
We study a nonequilibrium Langevin many-body system containing two 'test' particles and many 'background' particles. The test particles are spatially confined by a harmonic potential, and the background particles are driven by an external driving force. Employing numerical simulations of the model, we formulate an effective description of the two test particles in a nonequilibrium steady state. In particular, we investigate several different definitions of the effective force acting between the test particles. We find that the law of action and reaction does not hold for the total mechanical f…
Paramagnetic colloidal particles that are optically trapped in a linear array can form a zigzag pattern when an external magnetic field induces repulsive interparticle interactions. When the traps are abruptly turned off, the particles form a nonequilibrium expanding pattern with a zigzag symmetry, even when the strength of the magnetic interaction is weaker than that required to break the linear symmetry of the equilibrium state. We show that the transition to the equilibrium zigzag state is always potentially possible for purely harmonic traps. For anharmonic traps that have a finite height,…
Colloidal particles are considered ideal building blocks to produce materials with enhanced physical properties. The state-of-the-art techniques for synthesizing these particles provide control over shape, size, and directionality of the interactions. In spite of these advances, there is still a huge gap between the synthesis of individual components and the management of their spontaneous organization towards the desired structures. The main challenge is the control over the dynamics of self-organization. In their kinetic route towards thermodynamically stable structures, colloidal particles …
We investigate the nonequilibrium behavior of dense, plastic-crystalline suspensions of mildly anisotropic colloidal hard dumbbells under the action of an oscillatory shear field by employing Brownian dynamics computer simulations. In particular, we extend previous investigations, where we uncovered novel nonequilibrium phase transitions, to other aspect ratios and to a larger nonequilibrium parameter space, that is, a wider range of strains and shear frequencies. We compare and discuss selected results in the context of novel scattering and rheological experiments. Both simulations and experi…
Using large deviation theory and principles of stochastic optimal control, we show that rare molecular dynamics trajectories conditioned on assembling a specific target structure encode a set of interactions and external forces that lead to enhanced stability of that structure. Such a relationship can be formulated into a variational principle, for which we have developed an associated optimization algorithm and have used it to determine optimal forces for targeted self-assembly within nonequilibrium steady-states. We illustrate this perspective on inverse design in a model of colloidal cluste…
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…
We present the theoretical analysis of the steady state currents and density distributions of particles moving with Langevin dynamics, under the effects of an external potential displaced at constant rate. The Dynamic Density Functional (DDF) formalism is used to introduce the effects of the molecular interactions, from the equilibrium Helmholtz free energy density functional. We analyzed the generic form of the DDF for one-dimensional external potentials and the limits of strong and weak potential barriers. The ideal gas case is solved in a closed form for generic potentials and compared with…
The emergence of particle irreversibility in periodically driven colloidal suspensions has been interpreted as resulting either from a nonequilibrium phase transition to an absorbing state or from the chaotic nature of particle trajectories. Using a simple model of a driven suspension we show that a nonequilibrium phase transition is accompanied by hyperuniform static density fluctuations in the vicinity of the transition, where we also observe strong dynamic heterogeneities reminiscent of dynamics in glassy materials. We find that single particle dynamics becomes intermittent and strongly non…
By means of classical density functional theory and its dynamical extension, we consider a colloidal fluid with spherically-symmetric competing interactions, which are well known to exhibit a rich bulk phase behavior. This includes complex three-dimensional periodically ordered cluster phases such as lamellae, two-dimensional hexagonally packed cylinders, gyroid structures or spherical micelles. While the bulk phase behavior has been studied extensively in earlier work, in this paper we focus on such structures confined between planar repulsive walls under shear flow. For sufficiently high she…
The density distributions and Soret coefficient in a nonequilibrium colloidal system with nonuniform temperature are studied by the overdamped Langevin equation for Brownian motion in an inhomogeneous strong friction medium. Based on the relation between the temperature gradient, the interaction potential and the q-parameter in nonextensive statistics, We show that the colloidal particle density can be a function of the temperature and anomalously follows the noted alpha-distribution, or equivalently it can also be a function of the potential energy and follows Tsallis distribution. With the q…
We develop a mesoscopic field theory for the collective nonequilibrium dynamics of multicomponent mixtures of interacting active (i.e., motile) and passive (i.e., nonmotile) colloidal particles with isometric shape in two spatial dimensions. By a stability analysis of the field theory, we obtain equations for the spinodal that describes the onset of a motility-induced instability leading to cluster formation in such mixtures. The prediction for the spinodal is found to be in good agreement with particle-resolved computer simulations. Furthermore, we show that in active-passive mixtures the spi…
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…
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…
Motivated by recent studies on the dynamics of colloidal solutions in narrow channels, we consider the steady state properties of an assembly of non interacting particles subject to the action of a traveling potential moving at a constant speed while the solvent is modeled by a heat bath at rest in the laboratory frame. Since the description, we propose here, takes into account the inertia of the colloidal particles it is necessary to consider the evolution of both positions and momenta and study the governing equation for the one-particle phase-space distribution. We first derive the asymptot…
According to Harada and Sasa [Phys. Rev. Lett. 95, 130602 (2005)], heat production generated in a non-equilibrium steady state can be inferred from measuring response and correlation functions. In many colloidal systems, however, it is a nontrivial task to determine response functions, whereas details about spatial steady state trajectories are easily accessible. Using a simple conditional averaging procedure, we show how this fact can be exploited to reliably evaluate average heat production. We test this method using Brownian dynamics simulations, and apply it to experimental data of an inte…
We establish an explicit data-driven criterion for identifying the solid-liquid transition of two-dimensional self-propelled colloidal particles in the far from equilibrium parameter regime, where the transition points predicted by different conventional empirical criteria for melting and freezing diverge. This is achieved by applying a hybrid machine learning approach that combines unsupervised learning with supervised learning to analyze over one million of the system's configurations in the nonequilibrium parameter regime. Furthermore, we establish a generic data-driven evaluation function,…
We give the explicit structure of the functional governing the dynamical density and current fluctuations for a mesoscopic system in a nonequilibrium steady state. Its canonical form determines a generalised Onsager-Machlup theory. We assume that the system is described as a Markov jump process satisfying a local detailed balance condition such as typical for stochastic lattice gases and for chemical networks. We identify the entropy current and the traffic between the mesoscopic states as extra terms in the fluctuation functional with respect to the equilibrium dynamics. The density and curre…
An expression for the energetic efficiency of a molecular motor is presented in terms of an effective temperature, which was defined based on the ratio of the correlation function to the susceptibility of its velocity. We also present a numerical result regarding this temperature for a thermal ratchet model. Furthermore, our expression of efficiency using known values for kinesin can adequately explain the experimental results. The framework presented here has a closed form phenomenologically, and is independent of any detailed models.
We study the fluctuation-dissipation theorem for a Brownian particle driven into a nonequilibrium steady state experimentally. We validate two different theoretical variants of a generalized fluctuation-dissipation theorem. Furthermore, we demonstrate that the choice of variables crucially affects the accuracy of determining the nonequilibrium response from steady state nonequilibrium fluctuations.
We analyze theoretically the dynamics of a single colloidal particle in an externally applied electric field. The thermal motions of microions lead to an anisotropic, nonequilibrium source of noise, pro- portional to the field, in the effective Langevin equation for the colloid. The fluctuation-dissipation ratio depends strongly on frequency, and the colloid if displaced from its steady-state position relaxes with a velocity not proportional to the gradient of the logarithm of the steady-state probability.
Colloidal spheres driven through water along a circular path by an optical ring trap display unexpected dynamical correlations. We use Stokesian Dynamics simulations and a simple analytical model to demonstrate that the path's curvature breaks the symmetry of the two-body hydrodynamic interaction, resulting in particle pairing. The influence of this effective nonequilibrium attraction diminishes as either the temperature or the stiffness of the radial confinement increases. We find a well defined set of dynamically paired states whose stability relies on hydrodynamic coupling in curving trajec…
We examine the structure and dynamics of small isolated $N$-particle clusters interacting via short-ranged Morse potentials. "Ideally preprared ensembles" obtained via exact enumeration studies of sticky hard sphere packings serve as reference states allowing us to identify key statistical-geometrical properties and to quantitatively characterize how nonequilibrium ensembles prepared by thermal quenches at different rates $\dot{T}$ differ from their equilibrium counterparts. Studies of equilibrium dynamics show nontrival temperature dependence: nonexponential relaxation indicates both glassy d…
We study the coupling between the structural dynamics and rheological response of charged colloidal monolayers at water/oil interfaces, driven into steady shear by a microdisk rotating at a controlled angular velocity. The flow causes particles to layer into rotating concentric rings linked to the local, position-dependent shear rate, which triggers two distinct dynamical regimes: particles move continuously "Flowing") close to the microdisk, or exhibit intermittent "Hopping" between local energy minima farther away. The shear-rate dependent surface viscosity of a monolayer can be extracted fr…
Using fast confocal microscopy we image the three-dimensional dynamics of particles in a yielded hard-sphere colloidal glass under steady shear. The structural relaxation, observed in regions with uniform shear, is nearly isotropic but is distinctly different from that of quiescent metastable colloidal fluids. The inverse relaxation time $τ_α^{-1}$ and diffusion constant $D$, as functions of the {\it local} shear rate $\dotγ$, show marked shear thinning with $τ_α^{-1} \propto D \propto \dotγ^{0.8}$ over more than two decades in $\dotγ$. In contrast, the {\it global} rheology of the system disp…
Active colloids constitute a novel class of materials composed of colloidal-scale particles locally converting chemical energy into motility, mimicking micro-organisms. Evolving far from equilibrium, these systems display structural organizations and dynamical properties distinct from thermalized colloidal assemblies. Harvesting the potential of this new class of systems requires the development of a conceptual framework to describe these intrinsically nonequilibrium systems. We use sedimentation experiments to probe the nonequilibrium equation of state of a bidimensional assembly of active Ja…
We combine experiments, theory, and simulations to investigate the coexistence of nonequilibrium phases emerging from interacting colloidal particles that are electrokinetically propelled in a nematic liquid crystal solvent. We directly determine the mechanical pressure within the radial assemblies and measure a non-equilibrium equation of state for this athermal driven system. A generic model combines phoretic propulsion with the interplay between electrostatic effects and liquid-crystal-mediated hydrodynamics, which are effectively cast into a long-range interparticle repulsion, while elasti…
We drive a d-dimensional Heisenberg magnet using a spatially anisotropic current of mobile particles or heat. The continuum Langevin equation is analyzed using a dynamical renormalization group, stability analysis and numerical simulations. We discover a rich steady-state phase diagram, including a critical point in a new nonequilibrium universality class, and a spatiotemporally chaotic phase. The latter may be `controlled' in a robust manner to target spatially periodic steady states with helical order. We discuss several physical realizations of this model and make definite predictions which…
Large deviation functions contain information on the stability and response of systems driven into nonequilibrium steady states, and in such a way are similar to free energies for systems at equilibrium. As with equilibrium free energies, evaluating large deviation functions numerically for all but the simplest systems is difficult, because by construction they depend on exponentially rare events. In this first paper of a series, we evaluate different trajectory-based sampling methods capable of computing large deviation functions of time integrated observables within nonequilibrium steady sta…
We investigate stresses and particle motion during the start up of flow in a colloidal dispersion close to arrest into a glassy state. A combination of molecular dynamics simulation, mode coupling theory and confocal microscopy experiment is used to investigate the origins of the widely observed stress overshoot and (previously not reported) super-diffusive motion in the transient dynamics. A link between the macro-rheological stress versus strain curves and the microscopic particle motion is established. Negative correlations in the transient auto-correlation function of the potential stresse…
The nonlinear rheological properties of dense colloidal suspensions under steady shear are discussed within a first principles approach. It starts from the Smoluchowski equation of interacting Brownian particles in a given shear flow, derives generalized Green-Kubo relations, which contain the transients dynamics formally exactly, and closes the equations using mode coupling approximations. Shear thinning of colloidal fluids and dynamical yielding of colloidal glasses arise from a competition between a slowing down of structural relaxation, because of particle interactions, and enhanced decorr…
We discuss the peculiarities of the Seebeck effect in stabilized electrolytes containing the colloidal particles. Its unusual feature is the two-stage character, with the linear increase of differential thermopower as the function of colloidal particles concentration $n_{\odot}$ during the first stage and dramatic drop of it at small $n_{\odot}$ during the second one (steady state). We show that the properties of the initial state are governed by the thermo-diffusion flows of the mobile ions of the stabilizing electrolyte medium itself and how the colloidal particles participate in formation o…
Starting from the many-particle Smoluchowski equation, we derive dynamical density functional theory for Brownian particles with an arbitrary shape. Both passive and active (self-propelled) particles are considered. The resulting theory constitutes a microscopic framework to explore the collective dynamical behavior of biaxial particles in nonequilibrium. For spherical and uniaxial particles, earlier derived dynamical density functional theories are recovered as special cases. Our study is motivated by recent experimental progress in preparing colloidal particles with many different biaxial sh…
Shear history plays an important role in determining the linear and nonlinear rheological response of colloidal gels and can be used for tuning their structure and flow properties. Increasing colloidal particle aspect ratio lowers the critical volume fraction for gelation due to an increase of the particle excluded volume. Using a combination of rheology and confocal microscopy we investigate the effect of steady and oscillatory pre-shear history on the structure and rheology of colloidal gels formed by silica spheres and rods of length L and diameter D (L/D = 10) dispersed in 11 M CsCl soluti…
