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NoElastocaloric cooling is a promising solid-state alternative to vapor-compression refrigeration. In conventional systems, such as natural rubber, deformation induces entropy change accompanied by temperature release. Unloading the material restores the entropic state and is accompanied by cooling. Inverse elastocaloric effects have been detailed in shape memory alloys, where deformation induces loss of order and cooling. Here, we report on a distinctive inverse elastocaloric effect in liquid crystalline elastomers (LCEs) containing supramolecular hydrogen bonds. Upon deformation, the supramolecular LCE exhibits initial organization but then disorganizes as the intramesogenic hydrogen bonds are broken. Due to the liquid crystalline nature of the dimeric supramolecular bonds, the mechanochemical bond breakage manifests in a disruption in order. By disrupting the extent of liquid crystallinity in the system, we hypothesize that the network disorganizes to the deformation (e.g., entropy increases) and produces an inverse elastocaloric output.t Available 

Cholesteric liquid crystals (CLCs) exhibit Bragg reflection due to their spontaneous self-assembly into a one-dimensional photonic structure. Retaining this cholesteric order in a polymer network requires functionalizing liquid crystals with reactive end groups. However, conventional chemistries for synthesizing cholesteric liquid crystalline polymers often result in poor surface alignment and reduced optical quality. In this work, we investigate a thiol−ene step-growth polymerization approach to fabricate cholesteric liquid crystalline elastomers (CLCEs) with tunable mechanical properties and improved optical quality. By varying the cross-link density, we systematically study the effects on haze, cross-linking degree, and mechanical response. Compared to existing cholesteric liquid crystalline polymers, the thiol−ene-based CLCEs exhibit enhanced surface alignment, reduced haze, and greater mechanical tunability. These materials are further benchmarked against CLCEs synthesized via thiol−acrylate chain transfer polymerization, highlighting the advantages of the thiol−ene reaction for achieving precisely controlled properties in cholesteric polymer networks. 

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