Collective chemomechanical oscillations in active hydrogels.

We report on the collective response of an assembly of chemomechanical Belousov-Zhabotinsky (BZ) hydrogel beads. We first demonstrate that a single isolated spherical BZ hydrogel bead with a radius below a critical value does not oscillate, whereas an assembly of the same BZ hydrogel beads presents chemical oscillation. A BZ chemical model with an additional flux of chemicals out of the BZ hydrogel captures the experimentally observed transition from oxidized nonoscillating to oscillating BZ hydrogels and shows this transition is due to a flux of inhibitors out of the BZ hydrogel. The model also captures the role of neighboring BZ hydrogel beads in decreasing the critical size for an assembly of BZ hydrogel beads to oscillate. We finally leverage the quorum sensing behavior of the collective to trigger their chemomechanical oscillation and discuss how this collective effect can be used to enhance the oscillatory strain of these active BZ hydrogels. These findings could help guide the eventual fabrication of a swarm of autonomous, communicating, and motile hydrogels.

Surface Functionalization of 4D Printed Substrates Using Polymeric and Metallic Wrinkles.

Wrinkle topographies have been studied as simple, versatile, and in some cases biomimetic surface functionalization strategies. To fabricate surface wrinkles, one material phenomenon employed is the mechanical-instability-driven wrinkling of thin films, which occurs when a deforming substrate produces sufficient compressive strain to buckle a surface thin film. Although thin-film wrinkling has been studied on shape-changing functional materials, including shape-memory polymers (SMPs), work to date has been primarily limited to simple geometries, such as flat, uniaxially-contracting substrates. Thus, there is a need for a strategy that would allow deformation of complex substrates or 3D parts to generate wrinkles on surfaces throughout that complex substrate or part. Here, 4D printing of SMPs is combined with polymeric and metallic thin films to develop and study an approach for fiber-level topographic functionalization suitable for use in printing of arbitrarily complex shape-changing substrates or parts. The effect of nozzle temperature, substrate architecture, and film thickness on wrinkles has been characterized, as well as wrinkle topography on nuclear alignment using scanning electron microscopy, atomic force microscopy, and fluorescent imaging. As nozzle temperature increased, wrinkle wavelength increased while strain trapping and nuclear alignment decreased. Moreover, with increasing film thickness, the wavelength increased as well.