Structure-Property Relationships in Auxetic Liquid Crystal Elastomers-The Effect of Spacer Length

Auxetics are materials displaying a negative Poisson's ratio, i.e., getting thicker in one or both transverse axes when subject to strain. In 2018, liquid crystal elastomers (LCEs) displaying auxetic behaviour, achieved via a biaxial reorientation, were first reported. Studies have since focused on determining the physics underpinning the auxetic response, with investigations into structure-property relationships within these systems so far overlooked. Herein, we report the first structure-property relationships in auxetic LCEs, examining the effect of changes to the length of the spacer chain. We demonstrate that for LCEs with between six and four carbons in the spacer, an auxetic response is observed, with the threshold strain required to achieve this response varying from 56% (six carbon spacers) to 81% (four carbon spacers). We also demonstrate that Poisson's ratios as low as -1.3 can be achieved. Further, we report that the LCEs display smectic phases with spacers of seven or more carbons; the resulting internal constraints cause low strains at failure, preventing an auxetic response. We also investigate the dependence of the auxetic threshold on the dynamics of the samples, finding that when accounting for the glass transition temperature of the LCEs, the auxetic thresholds converge around 56%, regardless of spacer length.