Shape-Tunable 4D Printing of LCEs via Cooling Rate Modulation: Stimulus-Free Locking of Actuated State at Room Temperature

Liquid crystal elastomers (LCEs) have garnered considerable attention in the field of four-dimensional (4D) printing due to their large, reversible, and anisotropic shape-morphing capabilities. By utilizing direct ink writing, intricate LCE structures with programmable shape morphing can be achieved. However, the maintenance of the actuated state for LCEs requires continuous and substantial external stimuli, presenting challenges for practical applications, particularly under ambient conditions. This study reports a straightforward and effective physical approach to lock the actuated state of LCEs through rapid cooling while preserving their reversible performance. Rapid cooling significantly reduces the mobility of the lightly cross-linked network in LCEs, resulting in a notably slow recovery of mesogen alignment. As a result, the locked LCE structures retain their actuated state even at room temperature. Moreover, we demonstrate the ability to achieve tunable shapes between the original and actuated states by modulating the cooling rate, i.e., varying the temperature and type of cooling medium. The proposed method opens up new possibilities to achieve stable and tunable shape locking of soft devices for engineering applications.