Lewis, Kristin L; Hoang, Jonathan D; Aye, Sarah S; Kennedy, David T; Toney, Michael F; White, Timothy J

DOI:

Abstract

The directional deformation of liquid crystalline elastomers (LCEs) is predicated on alignment, enforced by variousprocessing techniques. Specifically, surface-aligned LCEs can exhibit higher temperature thermomechanical responses and weakenedstrain−temperature coupling in comparison to LCEs subjected to mechanical or rheological alignment. Recently, we reportedenhanced stimuli response of mechanically aligned LCEs containing supramolecular liquid crystals. Here, we prepare supramolecularLCEs via surface-enforced alignment to study the impact of the supramolecular bond strength and intermolecular forces. This wasevaluated using oxybenzoic acid (OBA) derivatives with and without pendant methyl groups as well as via oxybenzoic acid-pyridinecomplexes. Increased incorporation of supramolecular mesogens reduces the isotropic transition temperature and generally increasesthe strain−temperature coupling. The number of elastically active strands per unit volume, hydrogen bond conformations, andnetwork morphology are affected by the supramolecular mesogens and influence the observed stimuli response. Overall, reducedintermolecular interactions correlate with more desirable actuation properties, demonstrating the influence of the supramolecularmesogen’s structure.

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