Active matter systems exhibit rich emergent behavior due to constant injection and dissipation of energy at the level of individual agents. Since these systems are far from equilibrium, their dynamics and energetics cannot be understood using the framework of equilibrium statistical mechanics. Recent developments in stochastic thermodynamics extend classical concepts of work, heat, and energy dissipation to fluctuating non-equilibrium systems. We use recent advances in experiment and theory to study the non-thermal dissipation of individual light-activated self-propelled colloidal particles. We focus on characterizing the transition from thermal to non-thermal fluctuations and show that energy dissipation rates on the order of $\sim k_BT/$s are measurable from finite time series data.
We consider a rigid assembly of two active Brownian particles, forming an active colloidal dimer, in a gradient of activity. We show analytically that depending on the relative orientation of the two particles the active dimer accumulates in regions of either high or low activity, corresponding to, respectively, chemotaxis and antichemotaxis. Certain active dimers show both chemotactic and antichemotactic behavior, depending on the strength of the activity. Our coarse-grained Fokker-Planck approach yields an effective potential, which we use to construct a nonequilibrium phase diagram that cla…
Here, we describe a method for the enhanced self-assembly of triblock Janus colloids targeted to form a kagome lattice. Using computer simulations, we demonstrate that the formation of this elusive structure can be significantly improved by self-propelling or activating the colloids along the axis connecting their hydrophobic hemispheres. The process by which metastable aggregates are destabilized and transformed into the favored kagome lattice is quite general, and we argue this active approach provides a systematic pathway to improving the self-assembly of a large number of colloidal structu…
We consider a colloidal particle immersed in an active bath and derive a Smoluchowski equation that governs the dynamics of colloidal particle. We address this as active Smoluchowski equation. Our analysis based on this active Smoluchowski equation shows a short time superdiffusive behavior that strongly depends on the activity. Our model also predicts a non-monotonic dependence of mean energy dissipation against time, a signature of activity-induced dynamics. By introducing a frequency-dependent effective temperature, we show that the mean rate of entropy production is time dependent unlike a…
At the surfaces of autophoretic colloids, slip velocities arise from local chemical gradients that are many-body functions of particle configuration and activity. For rapid chemical diffusion, coupled with slip-induced hydrodynamic interactions, we deduce the chemohydrodynamic forces and torques between colloids. Near a no-slip wall, the forces can be expressed as gradients of a non-equilibrium potential which, by tuning the type of activity, can be varied from repulsive to attractive. When this potential has a barrier, we find arrested phase separation with a mean cluster size set by competin…
We study the motion of active patchy colloids in an optical trap using experiments, theory and numerical simulations. To achieve isotropic and harmonic confinement, we prototype microparticles with a nearly uniform refractive index and verify that, in the absence of activity, the confined motion is identical to that of optically homogeneous Brownian particles. If the activity is turned on by means of vertical AC fields, the density distributions are described by Boltzmann-like statistics (Gaussian with effective temperature) only for strongly confining traps, whereas weaker potentials give ris…
Self-organization phenomena in ensembles of self-propelled particles open pathways to the synthesis of new dynamic states not accessible by traditional equilibrium processes. The challenge is to develop a set of principles that facilitate the control and manipulation of emergent active states. Here, we report that dielectric rolling colloids energized by a pulsating electric field self-organize into alternating square lattices with a lattice constant controlled by the parameters of the field. We combine experiments and simulations to examine spatiotemporal properties of the emergent collective…
We study a two-dimensional model of an active isotropic colloid whose propulsion is linked to the interactions between solute particles of the bath. The colloid catalyzes a chemical reaction in its vicinity, that yields a local phase separation of solute particles. The density fluctuations of solute particles result in the enhanced diffusion of the colloid. Using numerical simulations, we thoroughly investigate the conditions under which activity occurs, and we establish a state diagram for the activity of the colloid as a function of the parameters of the model. We use the generated data to u…
Molecular motors are essential to the living, they generate additional fluctuations that boost transport and assist assembly. Self-propelled colloids, that consume energy to move, hold similar potential for the man-made assembly of microparticles. Yet, experiments showing their use as a powerhouse in materials science lack. Our work explores the design of man-made materials controlled by fluctuations, arising from the internal forces generated by active colloids. Here we show a massive acceleration of the annealing of a monolayer of passive beads by moderate addition of self-propelled micropar…
We study numerically the role of hydrodynamics in the liquid-hexatic transition of active colloids at intermediate activity, where motility induced phase separation (MIPS) does not occur. We show that in the case of active Brownian particles (ABP), the critical density of the transition decreases upon increasing the particle's mass, enhancing ordering, while self-propulsion has the opposite effect in the activity regime considered. Active hydrodynamic particles (AHP), instead, undergo the liquid-hexatic transition at higher values of packing fraction $ϕ$ than the corresponding ABP, suggesting …
We present results from Langevin dynamics simulations of a glassy active-passive mixture of soft-repulsive binary colloidal disks. Activity on the smaller particles is applied according to the quorum sensing scheme, in which a smaller particle will be active for a persistence time if its local nearest neighbors are equal to or greater than a certain threshold value. We start with a passive glassy state of the system and apply activity to the smaller particles, which shows a nonmonotonous glassy character of the active particles with the persistence time of the active force, from its passive li…
We report a systematic study of the dynamics of self-propelled particles (SPPs) over a one-dimensional periodic potential landscape, which is fabricated on a microgroove-patterned polydimethylsiloxane (PDMS) substrate. From the measured non-equilibrium probability density function of the SPPs, we find that the escape dynamics of the slow-rotating SPPs across the potential landscape can be described by an effective potential, once the self-propulsion force is included into the potential under the fixed angle approximation. This work demonstrates that the parallel microgrooves provide a versatil…
Activity enhances transport while competing interactions preserve structure in colloidal microphase formers
Instituto de Química Física Blas Cabrera, Consejo Superior de Investigaciones Científicas (CSIC)（布拉斯·卡布雷拉物理化学研究所，西班牙国家研究委员会）；Departament de Física de la Matèria Condensada, Universitat de Barcelona（巴塞罗那大学凝聚态物理系）；Instituto de Física de Líquidos y Sistemas Biológicos, CONICET-UNLP（液体与生物系统物理研究所，阿根廷国家科学研究与技术促进委员会-拉普拉塔国立大学）；Universidad Tecnológica Nacional, Facultad Regional La Plata, CIMEC - Centro de Investigación en Mecánica Experimental y Computacional（国立技术大学，拉普拉塔地区学院，实验与计算力学研究中心）
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…
Catalytically active colloids maintain non-equilibrium conditions in which they produce and deplete chemicals and hence effectively act as sources and sinks of molecules. While individual colloids that are symmetrically coated do not exhibit any form of dynamical activity, the concentration fields resulting from their chemical activity decay as $1/r$ and produce gradients that attract or repel other colloids depending on their surface chemistry and ambient variables. This results in a non-equilibrium analogue of ionic systems, but with the remarkable novel feature of action-reaction symmetry b…
A simple model of an active colloid consisting of dumbbell-shaped particles that cyclically change their length without propelling themselves is proposed and analyzed. At nanoscales, it represents an idealization for bacterial cytoplasm or for a biomembrane with active protein inclusions. Our numerical simulations demonstrate that non-equilibrium conformational activity of particles can strongly affect diffusion and structural relaxation: while a passive colloid behaves as a glass, it gets progressively fluidized when the activity is turned on. Qualitatively, this agrees with experimental resu…
We show theoretically that near a fluid-fluid interface a single active colloidal particle generating, e.g., chemicals or a temperature gradient experiences an effective force of hydrodynamic origin. This force is due to the fluid flow driven by Marangoni stresses induced by the activity of the particle; it decays very slowly with the distance from the interface, and can be attractive or repulsive depending on how the activity modifies the surface tension. We show that, for typical systems, this interaction can dominate the dynamics of the particle as compared to Brownian motion, dispersion fo…
Particle-tracking microrheology of dilute active (self-propelled) colloidal suspensions is studied by considering the external force required to maintain the steady motion of an immersed constant-velocity colloidal probe. If the probe speed is zero, the suspension microstructure is isotropic but exhibits a boundary accumulation of active bath particles at contact due to their self-propulsion. As the probe moves through the suspension, the microstructure is distorted from the nonequilibrium isotropic state, which allows us to define a microviscosity for the suspension using the Stokes drag law.…
Active colloids exhibit persistent motion, which can lead to motility-induced phase separation (MIPS). However, there currently exists no microscopic theory to account for this phenomenon. We report a first-principles theory, free of fit parameters, for active spherical colloids, which shows explicitly how an effective many-body interaction potential is generated by activity and how this can rationalize MIPS. For a passively repulsive system the theory predicts phase separation and pair correlations in quantitative agreement with simulation. For an attractive system the theory shows that phase…
The lack of detailed balance in active colloidal suspensions allows dissipation to determine stationary states. Here we show that slow viscous flow produced by polar or apolar active colloids near plane walls mediates attractive hydrodynamic forces that drive crystallization. Hydrodynamically mediated torques tend to destabilize the crystal but stability can be regained through critical amounts of bottom-heaviness or chiral activity. Numerical simulations show that crystallization is not nucleational, as in equilibrium, but is preceded by a spinodal-like instability. Harmonic excitations of th…
We review recent work on active colloids or swimmers, such as self-propelled microorganisms, phoretic colloidal particles, and artificial micro-robotic systems, moving in fluid-like environments. These environments can be water-like and Newtonian but can frequently contain macromolecules, flexible polymers, soft cells, or hard particles, which impart complex, nonlinear rheological features to the fluid. While significant progress has been made on understanding how active colloids move and interact in Newtonian fluids, little is known on how active colloids behave in complex and non-Newtonian f…
In equilibrium, colloidal suspensions governed by short-range attractive and long-range repulsive interactions form thermodynamically stable clusters. Using Brownian dynamics computer simulations, we investigate how this equilibrium clustering is affected when such particles are self-propelled. We find that the clustering process is stable under self-propulsion. For the range of interaction parameters studied and at low particle density, the cluster size increases with the speed of self-propulsion (activity) and for higher activity the cluster size decreases, showing a non-monotonic variation …
Various aspects of self-motility of chemically active colloids in Newtonian fluids can be captured by simple models for their chemical activity plus a phoretic slip hydrodynamic boundary condition on their surface. For particles of simple shapes (e.g., spheres) -- as employed in many experimental studies -- which move at very low Reynolds numbers in an unbounded fluid, such models of chemically active particles effectively map onto the well studied so-called hydrodynamic squirmers [S. Michelin and E. Lauga, J. Fluid Mech. \textbf{747}, 572 (2014)]. Accordingly, intuitively appealing analogies …
From studies via Molecular Dynamics simulations, we report results on structure and dynamics in mixtures of active colloids and passive polymers that are confined inside a spherical container with a repulsive boundary. Such systems mimic the presence of bacteria in the background of bio-polymers. All interactions in the fully passive case are chosen in such a way that in equilibrium coexistence between colloid-rich and polymer-rich phases occurs. For most part of the studies the chosen compositions give rise to Janus structure; one side of the sphere is occupied by the colloids and the rest by…
The phenomenon that a system at a hot temperature cools faster than at a warm temperature, referred to as the Mpemba effect, has been recently realized for trapped colloids. Here, we investigate the cooling and heating process of a self-propelling active colloid using numerical simulations and theoretical calculations with a model that can directly be tested in experiments. Upon cooling the particles' active motion induces a Mpemba effect. Transiently the system can even exhibit smaller temperatures than its final temperature, a surprising phenomenon which we refer to as activity-induced overc…
We study the dynamics of quasi-two-dimensional concentrated suspensions of colloidal particles in active gels by computer simulations. Remarkably, we find that activity induces a dynamic clustering of colloids even in the absence of any preferential anchoring of the active nematic director at the particle surface. When such an anchoring is present, active stresses instead compete with elastic forces and re-disperse the aggregates observed in passive colloid-liquid crystal composites. Our quasi-two-dimensional "inverse" dispersions of passive particles in active fluids (as opposed to the more c…
Spherical colloids that catalyze the interconversion reaction $A \leftrightharpoons B$ between solute molecules $A$ and $B$ whose concentration at infinity is maintained away from equilibrium effectively interact due to the non-uniform fields of solute concentrations. We show that this long range $1/r$ interaction is suppressed via a mechanism that is superficially reminiscent but qualitatively very different from electrostatic screening: catalytic activity drives the concentrations of solute molecules towards their equilibrium values and reduces the chemical imbalance that drives the interact…
Active colloids and externally actuated semi-flexible filaments provide basic building blocks for designing autonomously motile micro-machines. Here, we show that a passive semi-flexible filament can be actuated and transported by attaching an active colloid to its terminus. We study the dynamics of this assembly when it is free, tethered, or clamped using overdamped equations of motion that explicitly account for active fluid flow and the forces it mediates. Linear states are destabilized by buckling instabilities to produce stable states of non-zero curvature and writhe. We demarcate boundar…
Active colloids in liquid crystals (ACLCs) is an active matter with qualitatively new facets of behavior as compared to active matter that becomes isotropic when relaxed into an equilibrium state. We discuss two classes of ACLCs: (i) externally driven ACLCs, in which the motion of colloidal particles is powered by an externally applied electric field, and (ii) internally driven ACLCs, formed by self-propelled particles such as bacteria. The liquid crystal (LC) medium is of a thermotropic type in the first case and lyotropic (water based) in the second case. In the absence of external fields an…
In living cells, molecular motors create activity that enhances the diffusion of particles throughout the cytoplasm, and not just ones attached to the motors. We demonstrate initial steps toward creating artificial cells that mimic this phenomenon. Our system consists of active, Pt-coated Janus particles and passive tracers confined to emulsion droplets. We track the motion of both the active particles and passive tracers in a hydrogen peroxide solution, which serves as the fuel to drive the motion. We first show that correcting for bulk translational and rotational motion of the droplets indu…
We present a simple chemical strategy for the formation of a self-propelling cluster via the process of capture and assembly of passive colloids on the surface of a chemically active colloid. The two species of colloids that are isotropic and Brownian otherwise interact to form propelling cluster. With the help of coarse-grained numerical simulations, we show that a chemically active colloid can induce diffusiophoretic motility to nearby chemically inert colloids towards itself. This propulsion and then self-assembly can then lead to the formation of active cluster. We observe the formation of…
Active fluids comprise a variety of systems composed of elements immersed in a fluid environment which can convert some form of energy into directed motion; as such they are intrinsically out-of-equilibrium in the absence of any external forcing. A fundamental problem in the physics of active matter concerns the understanding of how the characteristics of the autonomous propulsion and agent-agent interactions determine the collective dynamics of the system. We study numerically suspensions of self-propelled diffusiophoretic colloids, in (quasi)-2d configurations, accounting for both dynamicall…
We study experimentally a sediment of self-propelled Brownian particles with densities ranging from dilute to ergodic supercooled, to nonergodic glass, to nonergodic polycrystal. In a compagnon letter, we observe a nonmonotonic response to activity of relaxation of the nonergodic glass state: a dramatic slowdown when particles become weakly self-propelled, followed by a speedup at higher activities. Here we map ergodic supercooled states to standard passive glassy physics, provided a monotonic shift of the glass packing fraction and the replacement of the ambient temperature by the effective t…
We explore phase separation and kinetic arrest in a model active colloidal system consisting of self-propelled, hard-core particles with nonconvex shapes. The passive limit of the model, namely cross-shaped particles on a square lattice, exhibits a first-order transition from a fluid phase to a solid phase with increasing density. Quenches into the two-phase coexistence region exhibit an aging regime. The nonconvex shape of the particles eases jamming in the passive system and leads to strong inhibition of rotations of the active particles. Using numerical simulations and analytical modeling, …
Switching on high activity in a relatively dense system of active Janus colloids, we observe fast clustering, followed by cluster aggregation towards full phase separation. The phase separation process is however interrupted when large enough clusters start breaking apart. Following the cluster size distribution as a function of time, we identify three successive dynamical regimes. Tracking both the particle positions and orientations, we characterize the structural ordering and alignment in the growing clusters and thereby unveil the mechanisms at play in these regimes. In particular, we iden…
The traction on the surface of a spherical active colloid in a thermally fluctuating Stokesian fluid contains passive, active, and Brownian contributions. Here we derive these three parts systematically, by "projecting out" the fluid using the boundary-domain integral representation of slow viscous flow. We find an exact relation between the statistics of the Brownian traction and the thermal forces in the fluid and derive, thereby, fluctuation-dissipation relations for every irreducible tensorial harmonic traction mode. The first two modes give the Brownian force and torque, from which we con…
Achieving control over the directionality of active colloids is essential for their use in practical applications such as cargo carriers in microfluidic devices. So far, guidance of spherical Janus colloids was mainly realized using specially engineered magnetic multilayer coatings combined with external magnetic fields. Here, we demonstrate that step-like sub-micron topographical features can be used as reliable docking and guiding devices for chemically active spherical Janus colloids. For various topographic features (stripes, squares or circular posts) docking of the colloid at the feature…
Transport phenomena in out-of-equilibrium systems is immensely important in a myriad of applications in biology, engineering and physics. Complex environments, such as the cytoplasm or porous media, can substantially affect the transport properties of such systems. In particular, recent interest has focused on how such environments affect the motion of active systems, such as colloids and organisms propelled by directional driving forces. Nevertheless, the transport of active matter with non-directional (rotational) activity is yet to be understood, despite the ubiquity of rotating modes of mo…
