4D Printing of Surface Morphing Hydrogels

Polymeric systems displaying spontaneous formation of surface wrinkling patterns are useful for a wide range of applications, such as diffraction gratings, flexible electronics, smart adhesives, optical devices, and cell culture platforms. Conventional fabrication techniques for wrinkling patterns involves multitude of processing steps and impose significant limitations on fabrication of hierarchical patterns, creating wrinkles on 3D and nonplanar structures, the scalability of the manufacturing process, and the integration of wrinkle fabrication process into a continuous manufacturing process. In this work, 4D printing of surface morphing hydrogels enabling direct fabrication of wrinkling patterns on curved and/or 3D structures with user-defined and spatially controlled pattern geometry and size is reported. The key to successful printing is to tailor the photopolymerization time and partial crosslinking time of the hydrogel inks. The interplay between crosslinker concentration and postprinting crosslinking time allow for the control over wrinkling morphology and the characteristic size of the patterns. The pattern alignment is controlled by the print strut size—the size of the solid material extruded from the print nozzle in the form of a line. To demonstrate the utility of the approach, tunable optical devices, a solvent/humidity sensor for microchips, and cell culture platforms to control stem cell shape are fabricated.