Cross-Hierarchical Transduction of Dynamic Behaviors from Self-Oscillating Microgels to Colloidosomes

Inspired by living systems, hierarchical materials have been developed to integrate multiple levels of organization, enabling complex behaviors to emerge from interactions among simpler components. However, understanding how dynamic behaviors are transduced across hierarchical levels in synthetic materials remains a major challenge. Here, we demonstrate the cross-hierarchical transduction of dynamic behaviors in life-like autonomous materials by investigating self-oscillating colloidosomes as a model system. Self-oscillating colloidosomes are composed of self-oscillating microgels, which exhibit autonomous flocculation/dispersion oscillation driven by a self-promoted Belousov-Zhabotinsky reaction at certain temperatures. We identified chemomechanical transduction across hierarchical levels in self-oscillating colloidosomes under out-of-equilibrium conditions. The self-oscillating colloidosomes exhibited swelling/deswelling or shape deformation oscillations in a stochastic manner, originating from flocculation/dispersion oscillations at the microgel level. We found that the choice between these two oscillation modes is determined by the oscillation modes of their constituent self-oscillating microgels. These findings pave the way for the cross-hierarchical design of chemically powered autonomous materials.