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Biological systems have the unique ability to self-organize and generateautonomous motion and work. Motivated by this, we investigate a 2D modelcolloidal network that can repeatedly transition between disordered states oflow connectivity and ordered states of high connectivity via rhythmic bindingand unbinding of biomimetic crosslinkers. We use Langevin dynamics toinvestigate the time-dependent changes in structure and collective propertiesof this system as a function of colloidal packing fractions and crosslinkeroscillation periods and characterize the degree of order in the system by usingnetwork connectivity, bond length distributions, and collective motion. Oursimulations suggest that we can achieve distinct states of this colloidalsystem with pronounced differences in microstructural order and large residencetimes in the ordered state when crosslinker kinetics and lifetimes dependdirectly on the oscillation period and this oscillation period is much largerthan the colloidal diffusion time. Our results will provide insights into therational design of smart active materials that can independently cycle betweenordered and disordered states with desired material properties on a programmedschedule.

Sustained Order-Disorder Transitions in a Model Colloidal System Driven by Rhythmic Crosslinking