Monolayer heterojunction interactive hydrogels for high-freedom 4D shape reconfiguration by two-photon polymerization

Mimicking natural botanical/zoological systems has revolutionarily inspired fourdimensional (4D) hydrogel robotics, interactive actuators/machines, automatic biomedical devices, and self-adaptive photonics. The controllable high-freedom shape reconfiguration holds the key to satisfying the ever-increasing demands. However, miniaturized biocompatible 4D hydrogels remain rigorously stifled due to current approach/material limits. In this research, we spatiotemporally program micro/ nano (μ/n) hydrogels through a heterojunction geometric strategy in femtosecond laser direct writing (fsLDW). Polyethylene incorporated N-isopropylacrylamide as programmable interactive materials here. Dynamic chiral torsion, site-specific mutation, anisotropic deformation, selective structural coloration of hydrogel nanowire, and spontaneous self-repairing as reusable μ/n robotics were identified. Hydrogel-materialized monolayer nanowires operate as the most fundamental block at nanometric accuracy to promise high freedom reconfiguration and high force-to-weight ratio/bending curvature under tight topological control. Taking use of this biomimetic fsLDW, we spatiotemporally constructed several in/out-plane selfdriven hydrogel grippers, diverse 2D-to-3D transforming from the same monolayer shape, responsive photonic crystal, and self-clenched fists at μ/n scale. Predictably, the geometry-modulable hydrogels would open new access to massively-reproducible robotics, actuators/sensors for microenvironments, or lab-on-chip devices.