The effect of alignment on the rate-dependent behavior of a main-chain liquid crystal elastomer

This study investigated the effect of alignment on the rate-dependent behavior of a main-chain liquid crystal elastomer (LCE). Polydomain nematic LCE networks were synthesized from a thiol-acrylate Michael addition reaction in the isotropic state. The polydomain networks were stretched to different strain levels to induce alignment then crosslinked in a second stage photopolymerization process. The LCE networks were subjected to dynamic mechanical tests to measure the temperature-dependent storage modulus and uniaxial tension load-unload tests to measure the rate-dependence of the Young's modulus, mechanical dissipation, and characteristics of the soft stress response. Three-dimensional (3D) digital image correlation (DIC) was used to characterize the effect of domain/mesogen relaxation on the strain fields. All LCE networks exhibited a highly rate-dependent stress response with significant inelastic strains after unloading. The Young's modulus of the loading curve and hysteresis of the load-unload curves showed a power-law dependence on the strain rate. The Young's modulus increased with alignment and larger anisotropy and a smaller power-law exponent was measured for the Young's modulus and hysteresis for the highly aligned monodomains. The polydomain and pre-stretched networks loaded perpendicular to the alignment direction exhibited a soft stress response that featured a rate-dependent peak stress, strain-softening, and strain-stiffening. The 3D-DIC strain fields for the polydomain network and programmed networks stretched in the perpendicular direction were highly heterogeneous, showing regions of alternating higher and lower strains. The strain variations increased initially with loading, peaked during the strain softening part of the stress response, then decreased during the strain stiffening part of the stress response. Greater variability was measured for lower strain rates. These observations suggest that local domain/mesogen relaxation led to the development of the heterogeneous strain patterns and strain softening in stress response. These findings improved understanding of the kinetics of mesogen relaxation and its contributions to the rate-dependent stress response and mechanical dissipation.