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. Walk along: Selective polymer chain decrosslinking in a liquid crystal polymer network (LCN) actuator is demonstrated. Spatially controlled optical decrosslinking alters the distribution of the actuation (crosslinked) and non‐actuation (decrosslinked) domains, and determines the actuation behavior upon the order–disorder phase transition. By using a dye‐doped LCN actuator, a light‐fueled microwalker can be optically reconfigured. [ABSTRACT FROM AUTHOR]