Toward In Silico Design of Highly Tunable Liquid Crystal Elastomers

In this work, a two-component acrylate liquid crystal elastomer, with varying composition and templating phase, is synthesized in the laboratory and investigated in parallel using atomistic molecular dynamics simulations. The anisotropic nature of both the mono- and bifunctional acrylates used in this study enables a large tunability in the compositional range while still retaining liquid crystalline properties in the final elastomer. The use of simulations allows important evaluation and comparison of physical properties such as glass transition temperature, nematic to isotropic phase transition temperature, and order parameter. The dependence of physical properties (glass transition, nematic to isotropic transition, order parameter, coefficient of thermal expansion, and mechanical properties) is established as a function of chemical composition, showing a high degree of tunability. Interestingly, the templating phase (nematic or isotropic) is also shown to impact the subsequent elastomer properties, with excellent agreement shown here between experiments and simulations. The in silico approach to polymerization, coupled with excellent comparison with the experimental system, represents a new methodology for the targeted design of liquid crystal elastomers with specific physical properties.