Selective Decrosslinking in Liquid Crystal Polymer Actuators for Optical Reconfiguration of Origami and Light‐Fueled Locomotion

The ability to optically reconfigure an existing actuator of a liquid crystal polymer network (LCN) so that it can display a new actuation behavior or function is highly desired in developing materials for soft robotics applications. Demonstrated here is a powerful approach relying on selective polymer chain decrosslinking in a LCN actuator with uniaxial LC alignment. Using an anthracene-containing LCN, spatially controlled optical decrosslinking can be realized through photocleavage of anthracene dimers under 254 nm UV light, which alters the distribution of actuation (crosslinked) and non-actuation (decrosslinked) domains and thus determines the actuation behavior upon order-disorder phase transitions. Based on this mechanism, a single actuator having a flat shape can be reconfigured in an on-demand manner to exhibit reversible shape transformation such as self-folding into origami three-dimensional structures. Moreover, using a dye-doped LCN actuator, a light-fueled microwalker can be optically reconfigured to adopt different locomotion behaviors, changing from moving in the laser scanning direction to moving in the opposite direction.