Light‐Triggered Locally Accelerated Healing in a Multi‐Functional Integrated Liquid Crystal Elastomer for Sustainable Information Storage Media

Abstract Liquid crystal elastomers (LCEs), endowed with self‐adaptive capabilities, exhibit the unique ability to enable on‐demand customization of their material properties. However, the on‐demand photo‐regulation of self‐healing ability in the LCEs has not yet been explored. Here, a multi‐functional integrated LCE with dynamic imine covalent networks is developed, in which the self‐healing ability can be switched with light irradiations by controlling the local network exchange dynamics. Specifically, a thermally stable diarylethene (DAE) switch as a photoswitchable crosslinker is successfully integrated into the dynamic covalent network to obtain DAE‐LCEs. The self‐healing ability of the resultant DAE‐LCEs as well as the apparent color and clusteroluminescence can be simultaneously modulated through open ‐/ closed ‐ring photoisomerization of DAE, which are attributed to the modulation of imine bond reactivity, photochromism and fluorescence resonance energy transfer, respectively. Model small molecule experiments and further theoretical calculations indicate that the decrease in the electron density of the imine bond and hence covalent strength of the polymer chain result in accelerated healing under certain conditions after a light stimulus. Ultimately, the potential applications for light‐controllable dual‐mode information storage and sustainable materials are demonstrated. This work holds significant implications for the design and development of multifunctional LCEs with on‐demand customizable properties.