Towards molecular-level auxetic fibres Y Yao, K. L. Alderson, A.

Alderson Centre for Materials Research and Innovation, The University of Bolton, Deane Road, Bolton BL3 5AB, UK. This paper reports on progress towards the development of molecular-level fibres displaying auxetic (negative Poissons ratio) behaviour - in other words, fibres which expand widthwise when stretched due to structural features at the molecular- or nano- scale. To date, auxetic polymeric fibres have been produced using a melt extrusion process. The fibres have been used to demonstrate significant benefits in composites applications (e.g. enhanced fibre pullout resistance, and reduced thermal distortion and residual stresses). They have also recently been deployed in textile structures, leading to potential in personal protective equipment, blast fabrics and apparel. To fully realise the potential of auxetic fibres, however, it is necessary to reduce the diameter of the fibres and also to increase the strength and/or stiffness of the fibres. This will ultimately be achieved through the development of auxetic fibres based on molecular-scale structures and deformation mechanisms. A number of molecular-level auxetic materials exist, and others have been proposed. Of the latter, early attempts at designing molecular-level auxetics included molecular honeycomb structures which mimicked the structure of macroscale honeycombs known to be auxetic. More recently, liquid crystalline polymers have appeared the most promising route to date towards the development of the first synthetic auxetic molecular polymer. In this paper, we report modelling investigations into two alternative molecular-level structures, funded through the Northwest Composites Centre in the UK. In the first, we use molecular mechanics and analytical modelling methods to explore the conditions under which singlewalled nanotube structures, based on a hexagonal honeycomb motif, may be auxetic. Honeycomb geometry (bond lengths and angles), and bond-stretch and bond-angle force constants are considered as variable parameters, and it has been possible to identify combinations of these parameters for which auxetic behaviour is predicted. In the second investigation, crystalline cellulose has been modelled using molecular mechanics methods. Recent experimental reports have demonstrated auxetic behaviour in some forms of cellulose. Molecular mechanics simulations have now been performed and found to reproduce the structure and auxetic character of auxetic cellulose. These models have then been used in uniaxial loading simulations to determine the predominant deformation mechanisms responsibe for the auxetic effect. From these simulations, it has been possible to develop simple analytical models to explain the auxetic effect, which it is hoped will lead to the design and synthesis of new fibre-forming auxetic molecular-level polymers.