The dynamics of chemically propelled dimer motors on a pinning substrate.

The dynamics of self-propelled micro-motors, in a thin fluid film containing an attractive substrate, is investigated by means of a particle-based simulation. A chemically powered sphere dimer, consisting of a catalytic and a noncatalytic sphere, may be captured by a trap on the substrate and consequently rotates around the trap center. A pair of trapped dimers spontaneously forms various configurations, including anti-parallel aligned doublets and head-to-tail rotating doublets. Small traps randomly distributed on the substrate are capable of pinning the dimers. The diffusion coefficient decreases with increasing pinning force or the pinning density, and it falls quickly at a certain critical pinning force beyond which the dimer motor is pinned completely. It is found that the pin array on the substrate gives rise to the formation of clusters of dimers and the underlying mechanism is discussed.

Synthetic Nanomotors: Working Together through Chemistry.

Active matter, some of whose constituent elements are active agents that can move autonomously, behaves very differently from matter without such agents. The active agents can self-assemble into structures with a variety of forms and dynamical properties. Swarming, where groups of living agents move cooperatively, is commonly observed in the biological realm, but it is also seen in the physical realm in systems containing small synthetic motors. The existence of diverse forms of self-assembled structures has stimulated the search for new applications that involve active matter. We consider active systems where the agents are synthetic chemically powered motors with various shapes and sizes that operate by phoretic mechanisms, especially self-diffusiophoresis. These motors are able to move autonomously in solution by consuming fuel from their environment. Chemical reactions take place on catalytic portions of the motor surface and give rise to concentration gradients that lead to directed motion. They can operate in this way only if the chemical composition of the system is maintained in a nonequilibrium state since no net fluxes are possible in a system at equilibrium. In contrast to many other active systems, chemistry plays an essential part in determining the properties of the collective dynamics and self-assembly of these chemically powered motor systems. The inhomogeneous concentration fields that result from asymmetric motor reactions are felt by other motors in the system and strongly influence how they move. This chemical coupling effect often dominates other interactions due to fluid flow fields and direct interactions among motors and determines the form that the collective dynamics takes. Since we consider small motors with micrometer and nanometer sizes, thermal fluctuations are strong and cannot be neglected. The media in which the motors operate may not be simple and may contain crowding agents or molecular filaments that influence how the motors assemble and move. The collective motion is also influenced by the chemical gradients that arise from reactions in the surrounding medium. By adopting a microscopic perspective, where the motors, fluid environment, and crowding elements are treated at the coarse-grained molecular level, all of the many-body interactions that give rise to the collective behavior naturally emerge from the molecular dynamics. Through simulations and theory, this Account describes how active matter made from chemically powered nanomotors moving in simple and more complicated media can form different dynamical structures that are strongly influenced by interactions arising from cooperative chemical reactions on the motor surfaces.

Chemotactic dynamics of catalytic dimer nanomotors.

Synthetic chemically powered nanomotors possessing the ability of chemotaxis are desirable for target cargo delivery and self-assembly. The chemotactic properties of a sphere dimer motor, composed of linked catalytic and inactive monomers, are studied in a gradient field of fuel. Particle-based simulation is carried out by means of hybrid molecular dynamics/multiparticle collision dynamics. The detailed tracking and motion analysis describing the running and tumbling of the sphere dimer motor in the process of chemotaxis are investigated. Physical factors affecting chemotactic velocity are discussed, and quantitative relations are presented. The influence of the geometry of sphere dimer motors on the chemotactic dynamics is explored, which is beneficial for the design of motors with high sensitivity for detecting the surrounding environment.

Influences of periodic mechanical deformation on pinned spiral waves.

In a generic model of excitable media, we study the behavior of spiral waves interacting with obstacles and their dynamics under the influences of simple periodic mechanical deformation (PMD). Depending on the characteristics of the obstacles, i.e., size and excitability, the rotation of a pinned spiral wave shows different scenarios, e.g., embedding into or anchoring on an obstacle. Three different drift phenomena induced by PMD are observed: scattering on small partial-excitable obstacles, meander-induced unpinning on big partial-excitable obstacles, and drifting around small unexcitable obstacles. Their underlying mechanisms are discussed. The dependence of the threshold amplitude of PMD on the characteristics of the obstacles to successfully remove pinned spiral waves on big partial-excitable obstacles is studied.

Chemical Logic Gates on Active Colloids.

Recent studies have shown that active colloidal motors using enzymatic reactions for propulsion hold special promise for applications in fields ranging from biology to material science. It will be desirable to have active colloids with capability of computation so that they can act autonomously to sense their surroundings and alter their own dynamics. It is shown how small chemical networks that make use of enzymatic chemical reactions on the colloid surface can be used to construct motor-based chemical logic gates. The basic features of coupled enzymatic reactions that are responsible for propulsion and underlie the construction and function of chemical gates are described using continuum theory and molecular simulation. Examples are given that show how colloids with specific chemical logic gates, can perform simple sensing tasks. Due to the diverse functions of different enzyme gates, operating alone or in circuits, the work presented here supports the suggestion that synthetic motors using such gates could be designed to operate in an autonomous way in order to complete complicated tasks.

Emitting waves from heterogeneity by a rotating electric field.

In a generic model of excitable media, we simulate wave emission from a heterogeneity (WEH) induced by an electric field. Based on the WEH effect, a rotating electric field is proposed to terminate existed spatiotemporal turbulence. Compared with the effects resulted by a periodic pulsed electric field, the rotating electric field displays several improvements, such as lower required intensity, emitting waves on smaller obstacles, and shorter suppression time. Furthermore, due to rotation of the electric field, it can automatically source waves from the boundary of an obstacle with small curvature.

Mesoscopic dynamics of diffusion-influenced enzyme kinetics.

A particle-based mesoscopic model for enzyme kinetics is constructed and used to investigate the influence of diffusion on the reactive dynamics. Enzymes and enzyme-substrate complexes are modeled as finite-size soft spherical particles, while substrate, product, and solvent molecules are point particles. The system is evolved using a hybrid molecular dynamics-multiparticle collision dynamics scheme. Both the nonreactive and reactive dynamics are constructed to satisfy mass, momentum, and energy conservation laws, and reversible reaction steps satisfy detailed balance. Hydrodynamic interactions among the enzymes and complexes are automatically accounted for in the dynamics. Diffusion manifests itself in various ways, notably in power-law behavior in the evolution of the species concentrations. In accord with earlier investigations, regimes where the product production rate exhibits either monotonic or nonmonotonic behavior as a function of time are found. In addition, the species concentrations display both t(-1/2) and t(-3/2) power-law behavior, depending on the dynamical regime under investigation. For high enzyme volume fractions, cooperative effects influence the enzyme kinetics. The time dependent rate coefficient determined from the mass action rate law is computed and shown to depend on the enzyme concentration. Lifetime distributions of substrate molecules newly released in complex dissociation events are determined and shown to have either a power-law form for rebinding to the same enzyme from which they were released or an exponential form for rebinding to different enzymes. The model can be used and extended to explore a variety of issues related concentration effects and diffusion on enzyme kinetics.

Dynamical phase of driven colloidal systems with short-range attraction and long-range repulsion.

We study the nonequilibrium dynamics of colloidal system with short-range depletion attraction and screened electrostatic repulsion on a disordered substrate. We find a growth-melting process of the clusters as the temperature is increased. By strengthening the screened electrostatic repulsion, a depinning transition from moving cluster to plastic flow is observed, which is characterized by a peak in threshold depinning force. The corresponding phase diagram is then mapped out. Due to the influences of disorder from substrate, the clusters are polarized by the strong external force, accompanied by the appearance of interesting orientational order parallel to the force and translational order perpendicular to the force. Under the condition of strong external force, the influences of density of pins and temperature are also studied.

The dynamics and self-assembly of chemically self-propelled sphere dimers.

The dynamics of chemically powered sphere dimers at the micro- and nano-scales confined in a quasi-two-dimensional geometry are investigated. The dimer consists of a Janus particle and a non-catalytic sphere. A chemical reaction taking place on the catalytic surface of the Janus particle creates asymmetric concentration gradients that give rise to the self-propulsion of both rotation and translation of the dimer. Due to the chemical interactions, ensembles of dimers spontaneously form anti-parallel aligned doublets that exhibit the same rotation direction and lose translational motion. The chirality of the dimer plays an important role in the process of doublet formation. The study displays new collective dynamics and structures when both translational and rotational self-propulsion occur.

Separation of nanoparticles via surfing on chemical wavefronts.

The separation of micro and nanoscale colloids is a necessary step in most biological microassay techniques, and is a common practice in microchemical processing. Chemical waves are frequently encountered in biochemical systems driven far from equilibrium. Here, we put forward a strategy for separating small suspending colloids by means of their surfing on substrate chemical wavefronts. The colloids with catalytic activities sensitive to the substrates are activated to show self-propulsion and consequently exhibit a chemotactic response to the traveling wavefronts, which results in their spontaneous separation from the multicomponent complex mixture via self-diffusiophoresis. The dynamics of the process is analyzed through a particle-based simulation. In addition, it is found that separation can be carried out according to particle size. The mechanisms underpinning the chemical and physical separation processes are discussed, and the dependencies on the reaction rate constant and particle size are presented. The results may prove relevant for further experimental and theoretical studies of separation in complex active environments.

Influences of periodic mechanical deformation on spiral breakup in excitable media.

Influences of periodic mechanical deformation (PMD) on spiral breakup that results from Doppler instability in excitable media are investigated. We present a new effect: a high degree of homogeneous PMD is favored to prevent the low-excitability-induced breakup of spiral waves. The frequency and amplitude of PMD are also significant for achieving this purpose. The underlying mechanism of successful control is also discussed, which is believed to be related to the increase of the minimum temporal period of the meandering spiral when the suitable PMD is applied.

Synchronization of a spiral by a circularly polarized electric field in reaction-diffusion systems.

Synchronization of a spiral by a circularly polarized electric field (CPEF) in reaction-diffusion systems is investigated since they both possess rotation symmetry. It is found that spirals in different regimes (including rigidly rotating, meandering, and drifting spirals) can be forced to be rigidly rotating ones by CPEFs. Moreover, the rotational frequency of the entrained spiral is found to be synchronized with the frequency of the electric field in a ratio of 1:1.

Suppression of spirals and turbulence in inhomogeneous excitable media.

Suppression of spiral and turbulence in inhomogeneous media due to local heterogeneity with higher excitability is investigated numerically. When the inhomogeneity is small, control tactics by boundary periodic forcing (BPF) is effective against the existing spiral and turbulence. When the inhomogeneity of excitability is large, a rotating electric field (REF) is utilized to "smooth" regional heterogeneity based on driven synchronization. Consequently, a control approach combining BPF with REF is proposed to suppress the spiral and turbulence. The underlying mechanism of successful suppression is discussed in terms of dispersion relation.

Chemically Propelled Motors Navigate Chemical Patterns.

Very small synthetic motors that use chemical reactions to drive their motion are being studied widely because of their potential applications, which often involve active transport and dynamics on nanoscales. Like biological molecular machines, they must be able to perform their tasks in complex, highly fluctuating environments that can form chemical patterns with diverse structures. Motors in such systems can actively assemble into dynamic clusters and other unique nonequilibrium states. It is shown how chemical patterns with small characteristic dimensions may be utilized to suppress rotational Brownian motions of motors and guide them to move along prescribed paths, properties that can be exploited in applications. In systems with larger pattern length scales, domains can serve as catch basins for motors through chemotactic effects. The resulting collective motor dynamics in such confining domains can be used to explore new aspects of active particle collective dynamics or promote specific types of active self-assembly. More generally, when chemically self-propelled motors operate in far-from-equilibrium active chemical media the variety of possible phenomena and the scope of their potential applications are substantially increased.

Pair Interaction of Catalytical Sphere Dimers in Chemically Active Media.

We study the pair dynamics of two self-propelled sphere dimers in the chemically active medium in which a cubic autocatalytic chemical reaction takes place. Concentration gradient around the dimer, created by reactions occurring on the catalytic sphere surface and responsible for the self-propulsion, is greatly influenced by the chemical activities of the environment. Consequently, the pair dynamics of two dimers mediated by the concentration field are affected. In the particle-based mesoscopic simulation, we combine molecular dynamics (MD) for potential interactions and reactive multiparticle collision dynamics (RMPC) for solvent flow and bulk reactions. Our results indicate three different configurations between a pair of dimers after the collision, i.e., two possible scenarios of bound dimer pairs and one unbound dimer pair. A phase diagram is sketched as a function of the rate coefficients of the environment reactions. Since the pair interactions are the basic elements of larger scale systems, we believe the results may shed light on the understanding of the collective dynamics.

Dynamics of Scroll Wave in a Three-Dimensional System with Changing Gradient.

The dynamics of a scroll wave in an excitable medium with gradient excitability is studied in detail. Three parameter regimes can be distinguished by the degree of gradient. For a small gradient, the system reaches a simple rotating synchronization. In this regime, the rigid rotating velocity of spiral waves is maximal in the layers with the highest filament twist. As the excitability gradient increases, the scroll wave evolutes into a meandering synchronous state. This transition is accompanied by a variation in twisting rate. Filament twisting may prevent the breakup of spiral waves in the bottom layers with a low excitability with which a spiral breaks in a 2D medium. When the gradient is large enough, the twisted filament breaks up, which results in a semi-turbulent state where the lower part is turbulent while the upper part contains a scroll wave with a low twisting filament.

Control of turbulence in heterogeneous excitable media.

Control of turbulence in two kinds of typical heterogeneous excitable media by applying a combined method is investigated. It is found that local-low-amplitude and high-frequency pacing (LHP) is effective to suppress turbulence if the deviation of the heterogeneity is minor. However, LHP is invalid when the deviation is large. Studies show that an additional radial electric field can greatly increase the efficiency of LHP. The underlying mechanisms of successful control in the two kinds of cases are different and are discussed separately. Since the developed strategy of combining LHP with a radial electric field can terminate turbulence in excitable media with a high degree of inhomogeneity, it has the potential contribution to promote the practical low-amplitude defibrillation approach.

Noise-induced anomalous diffusion over a periodically modulated saddle.

We study analytically and numerically the anomalous diffusion across periodically modulated parabolic potential within Langevin and Fokker-Planck descriptions. We find that the probability of particles passing over the saddle is affected strikingly by the periodical modulation with average zero bias. Particularly, the initial phase plays an important role in the modulation effect. The effect of the correlation time of external Ornstein-Uhlenbeck noise on dynamical process is also discussed. A reduction in overpassing probability is observed due to finite correlation time.

Transition from Turing stripe patterns to hexagonal patterns induced by polarized electric fields.

The effect of a circularly polarized electric field on the Turing stripe patterns is studied. The numerical results show that stripe patterns may change to hexagonal wave patterns by choosing the intensity and the frequency of the circularly polarized electric field suitably. Our findings indicate that a pattern tends to organize itself to the pattern with the same symmetry of the applied field with the fact that compared to the stripe patterns, hexagonal wave patterns possess hexagonal symmetry which is closer to the rotation symmetry of the circularly polarized electric field.