Coincident Molecular Auxeticity and Negative Order Parameter in a Liquid Crystal Elastomer

TL;DR

This paper demonstrates the first synthetic molecular auxetic using a liquid crystal elastomer, which exhibits negative Poisson's ratio behavior at high strains, aligning with theoretical predictions and opening new avenues for material design.

Contribution

It provides the first experimental proof of molecular auxeticity in a synthetic material, specifically a liquid crystal elastomer, and links auxetic behavior to a negative liquid crystal order parameter.

Findings

LCE becomes auxetic at strains > 0.8 with PR of -0.8

Auxeticity coincides with negative liquid crystal order parameter

Results agree with Warner and Terentjev theory of LCEs

Abstract

"Auxetic" materials have the counter-intuitive property of expanding rather than contracting perpendicular to an applied stretch, formally they have negative Poisson's Ratios (PRs).[1,2] This results in properties such as enhanced energy absorption and indentation resistance, which means that auxetics have potential for applications in areas from aerospace to biomedical industries.[3,4] Existing synthetic auxetics are all created by carefully structuring porous geometries from positive PR materials. Crucially, their geometry causes the auxeticity.[3,4] The necessary porosity weakens the material compared to the bulk and the structure must be engineered, for example, by using resource-intensive additive manufacturing processes.[1,5] A longstanding goal for researchers has been the development of a synthetic material that has intrinsic auxetic behaviour. Such "molecular auxetics" would avoid porosity-weakening and their very existence implies chemical tuneability.[1,4-9] However molecular auxeticity has never previously been proven for a synthetic material.[6,7] Here we present a synthetic molecular auxetic based on a monodomain liquid crystal elastomer (LCE). When stressed perpendicular to the alignment direction, the LCE becomes auxetic at strains greater than approximately 0.8 with a minimum PR of -0.8. The critical strain for auxeticity coincides with the occurrence of a negative liquid crystal order parameter (LCOP). We show the auxeticity agrees with theoretical predictions derived from the Warner and Terentjev theory of LCEs.[10] This demonstration of a synthetic molecular auxetic represents the origin of a new approach to producing molecular auxetics with a range of physical properties and functional behaviours. Further, it demonstrates a novel feature of LCEs and a route for realisation of the molecular auxetic technologies that have been proposed over the years.