Thermomechanical Coupling in Polydomain Liquid Crystal Elastomers

Liquid crystal elastomers (LCEs) are made of liquid crystal molecules integrated with rubber-like polymer networks. An LCE exhibits both the thermotropic property of liquid crystals and the large deformation of elastomers. It can be monodomain or polydomain in the nematic phase and transforms to an isotropic phase at elevated temperature. These features have enabled various new applications of LCEs in robotics and other fields. However, despite substantial research and development in recent years, thermomechanical coupling in polydomain LCEs remains poorly studied, such as their temperature-dependent mechanical response and stretch-influenced isotropic-nematic phase transition. This knowledge gap severely limits the fundamental understanding of the structure-property relationship, as well as future developments of LCEs with precisely controlled material behaviors. Here, we construct a theoretical model to investigate the thermomechanical coupling in polydomain LCEs. The model includes a quasi-convex elastic energy of the polymer network and a free energy of mesogens. We study the working conditions where a polydomain LCE is subjected to various prescribed planar stretches and temperatures. The quasi-convex elastic energy enables a "mechanical phase diagram" that describes the macroscopic effective mechanical response of the material, and the free energy of mesogens governs their first-order nematic-isotropic phase transition. The evolution of the mechanical phase diagram and the order parameter with temperature is predicted and discussed. Unique temperature-dependent mechanical behaviors of the polydomain LCE that have never been reported before are shown in their stress-stretch curves. These results are hoped to motivate future fundamental studies and new applications of thermomechanical LCEs.