Liyan Qiao

Chemical shakers are active particles with zero propulsion velocity whose activity derives from chemical reactions on portions of their surfaces. Although they do not move, except through Brownian motion, the nonequilibrium concentration and velocity fields that they generate endow them with properties that differ from their equilibrium counterparts. In particular, collections of such shakers can actively move, reorient, and self-assemble into various cluster states, which are the subject of this paper. Elongated chemical shakers constructed from linked catalytic and noncatalytic spheres are considered, and it is shown how hydrodynamic, chemotactic, and shape-dependent interactions give rise to various self-assembled shaker structures. The chemical forces responsible for cluster formation are described in terms of a model based on pair-wise additive contributions. The forms of the self-assembled structures can be varied by changing the chemostat concentrations that control the nonequilibrium state. The resulting structures and their manipulation through chemical means suggest ways to construct a class of active materials for applications.

Active materials with distinctive nonequilibrium properties have diverse materials science applications. Active systems are common in living matter, such as the filament network in the cell that is activated by molecular motors, and in materials science as exemplified by hydrogels activated by chemical reactions. Here we describe another class of active polymeric filament systems where the filaments are activated by embedded chemically-powered nanomotors that have catalytic and noncatalytic parts. Chemical reactions on the catalytic surfaces produce forces that act on the polymeric filaments. By changing the nonequilibrium conditions these forces can be made to change sign and thereby compress or expand the filaments. The embedded motors provide both the source of activity and the means to control the filament conformational structure. As an example of control, we show that oscillatory variations of the chemical constraints yield gel-like networks that oscillate between expanded or compressed forms, much like those of hydrogels.

Active materials with distinctive nonequilibrium properties have diverse materials science applications. Active systems are common in living matter, such as the filament network in the cell that is activated by molecular motors, and in materials science as exemplified by hydrogels activated by chemical reactions. Here we describe another class of active polymeric filament systems where the filaments are activated by embedded chemically powered nanomotors that have catalytic and noncatalytic parts. Chemical reactions on the catalytic surfaces produce forces that act on the polymeric filaments. By changing the nonequilibrium conditions, these forces can be made to change sign and thereby compress or expand the filaments. The embedded motors provide both the source of activity and the means to control the filament conformational structure. As an example of control, we show that oscillatory variations of the chemical constraints yield gel-like networks that oscillate between expanded or compressed forms, much like those of hydrogels.

The dynamics of chemically powered sphere dimers at the micro- and nano-scales confined in a quasi-two-dimensional geometry are investigated.

The collective behavior of chemically powered nanomotors in complex filament networks is investigated. The synthetic motors are small oligomers and use self-diffusiophoresis for their active motion. Much like biological molecular machines, these motors attach to the filaments, which highly suppress orientational Brownian motion, and move along them. The collective motion is influenced by structure of the network and the forces that bind the motors to the filaments; it is characterized by strong clustering, especially near cross-links in the network, and differs substantially from that in a simple fluid phase where only weak clustering occurs. The features of the collective behavior are quantitatively examined through computations of the effective binding potentials and the dynamics of probe oligomers. The results are relevant for applications in the biological and materials sciences involving complex natural and synthetic networks activated by small chemically powered motors.

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.