Micro- and nanofabrication of dynamic hydrogels with multichannel information.

Creating micro/nanostructures containing multi-channel information within responsive hydrogels presents exciting opportunities for dynamically changing functionalities. However, fabricating these structures is immensely challenging due to the soft and dynamic nature of hydrogels, often resulting in unintended structural deformations or destruction. Here, we demonstrate that dehydrated hydrogels, treated by a programmable femtosecond laser, can allow for a robust fabrication of micro/nanostructures. The dehydration enhances the rigidity of the hydrogels and temporarily locks the dynamic behaviours, significantly promoting their structural integrity during the fabrication process. By utilizing versatile dosage domains of the femtosecond laser, we create micro-grooves on the hydrogel surface through the use of a high-dosage mode, while also altering the fluorescent intensity within the rest of the non-ablated areas via a low-dosage laser. In this way, we rationally design a pixel unit containing three-channel information: structural color, polarization state, and fluorescent intensity, and encode three complex image information sets into these channels. Distinct images at the same location were simultaneously printed onto the hydrogel, which can be observed individually under different imaging modes without cross-talk. Notably, the recovered dynamic responsiveness of the hydrogel enables a multi-information-encoded surface that can sequentially display different information as the temperature changes.

Multifunctional 3D-Printed Pollen Grain-Inspired Hydrogel Microrobots for On-Demand Anchoring and Cargo Delivery.

While a majority of wireless microrobots have shown multi-responsiveness to implement complex biomedical functions, their functional executions are strongly dependent on the range of stimulus inputs, which curtails their functional diversity. Furthermore, their responsive functions are coupled to each other, which results in the overlap of the task operations. Here, a 3D-printed multifunctional microrobot inspired by pollen grains with three hydrogel components is demonstrated: iron platinum (FePt) nanoparticle-embedded pentaerythritol triacrylate (PETA), poly N-isopropylacrylamide (pNIPAM), and poly N-isopropylacrylamide acrylic acid (pNIPAM-AAc) structures. Each of these structures exhibits their respective targeted functions: responding to magnetic fields for torque-driven surface rolling and steering, exhibiting temperature responsiveness for on-demand surface attachment (anchoring), and pH-responsive cargo release. The versatile multifunctional pollen grain-inspired robots conceptualized here pave the way for various future medical microrobots to improve their projected performance and functional diversity.

Chemical Tracking of Temperature by Concurrent Periodic Precipitation Pattern Formation in Polyacrylamide Gels.

In nature, nonequilibrium systems reflect environmental changes, and these changes are often "recorded" in their solid body as they develop. Periodic precipitation patterns, aka Liesegang patterns (LPs), are visual sums of complex events in nonequilibrium reaction-diffusion processes. Here we aim to achieve an artificial system that "records" the temperature changes in the environment with the concurrent LP formation. We first illustrate the differences in 1-D LPs developing at different temperatures in terms of band spacings, which can demonstrate the time, ramp steepness, and extent of a temperature change. These results are discussed and augmented by a mathematical model. Using scanning electron microscopy, we show that the average size of the CuCrO4 precipitate also reflects the temperature changes. Finally, we show that these changes can also be "recorded" in the 2-D and 3-D LPs, which can have applications in long-term temperature tracking and complex soft material design.

Shape-programmable liquid crystal elastomer structures with arbitrary three-dimensional director fields and geometries.

Liquid crystal elastomers exhibit large reversible strain and programmable shape transformations, enabling various applications in soft robotics, dynamic optics, and programmable origami and kirigami. The morphing modes of these materials depend on both their geometries and director fields. In two dimensions, a pixel-by-pixel design has been accomplished to attain more flexibility over the spatial resolution of the liquid crystal response. Here we generalize this idea in two steps. First, we create independent, cubic light-responsive voxels, each with a predefined director field orientation. Second, these voxels are in turn assembled to form lines, grids, or skeletal structures that would be rather difficult to obtain from an initially connected material sample. In this way, the orientation of the director fields can be made to vary at voxel resolution to allow for programmable optically- or thermally-triggered anisotropic or heterogeneous material responses and morphology changes in three dimensions that would be impossible or hard to implement otherwise.

Mechanical Control of Periodic Precipitation in Stretchable Gels to Retrieve Information on Elastic Deformation and for the Complex Patterning of Matter.

Material design using nonequilibrium systems provides straightforward access to complexity levels that are possible through dynamic processes. Pattern formation through nonequilibrium processes and reaction-diffusion can be used to achieve this goal. Liesegang patterns (LPs) are a kind of periodic precipitation patterns formed through reaction-diffusion. So far, it has been shown that the periodic band structure of LPs and the geometry of the pattern can be controlled by experimental conditions and external fields (e.g., electrical or magnetic). However, there are no examples of these systems being used to retrieve information about the changes in the environment as they form, and there are no studies making use of these patterns for complex material preparation. This work shows the formation of LPs by a diffusion-precipitation reaction in a stretchable hydrogel and the control of the obtained patterns by the unprecedented and uncommon method of mechanical input. Additionally, how to use this protocol and how deviations from "LP behavior" of the patterns can be used to "write and store" information about the time, duration, extent, and direction of gel deformation are presented. Finally, an example of using complex patterning to deposit polypyrrole by using precipitation patterns is shown as a template.