Thermoviscoelasticity of polydomain liquid crystal elastomers regulated by soft elasticity

Abstract

Liquid crystal elastomers (LCEs) are elastomeric networks with rod-like mesogens that reorient under load. In polydomain LCEs, this reorientation drives a polydomain-to-monodomain transition that produces a soft-elastic plateau. Coupling between this soft elasticity and polymer-network viscoelasticity yields a path-dependent thermoviscoelastic response, central to applications in damping, impact protection, and tough adhesives. However, the physics governing this response under complex thermomechanical histories remains insufficiently studied. We present a combined experimental and theoretical study of polydomain LCEs under three uniaxial protocols: single-cycle loading-unloading, stress-free recovery from various pre-stretches, and multi-cycle loading with progressively increasing amplitude. We develop a finite-deformation constitutive model combining two parallel mechanisms: rate-independent, temperature-dependent soft elasticity from mesogen reorientation, and time- and temperature-dependent viscoelasticity. With a single parameter set, the model quantitatively reproduces all three protocols and resolves each mechanism's contribution. A temperature-dependent soft-elastic limit governs the low-rate response and the long-time recovered stretch, while viscoelasticity controls the rate-dependent deviation and the cycle-wise accumulation of residual stretch away from this limit. A thermal recovery test above the nematic-isotropic transition confirms that all hysteresis and residual deformation are reversible, ruling out irreversible damage. The framework provides mechanistic understanding and a predictive basis for designing polydomain LCE components under complex thermomechanical histories.