Synergistic photoactuation of bilayered spiropyran hydrogels for predictable origami-like shape change

Abstract

<h2>Summary</h2> Development of stimuli-responsive soft matter that undergoes fast and reversible shape changes that mimic living organisms is a grand challenge for materials science. We report here on the molecular design of photoactive bilayer actuators that can rapidly respond to visible light, leading to complex but predictable bio-inspired shape changes. The mechanism of accelerated actuation is rooted in the simultaneous photoexpansion of one layer and photocontraction of the other triggered by the same light stimulus. The opposing response leads to a synergistic effect that results in fast bending actuation. The synergistic bilayers were bridged with light-inactive segments to generate macroscopic constructs capable of undergoing programmable 3D origami-like shape change upon irradiation. By controlling the anisotropic friction with the substrate, these constructs displayed unidirectional inchworm- and octopus-like locomotion over macroscopic distances. The soft matter systems investigated here demonstrate the possibility of molecularly engineering photoactuators that mimic functions we associate with living organisms.