In Silico Polymerisation and Characterisation of Auxetic Liquid Crystalline Elastomers Using Atomistic Molecular Dynamics Simulations

R Mandle and T Raistrick and D Mistry and H Gleeson, POLYMERS, 17, 3011 (2025).

DOI: 10.3390/polym17223011

Using reactive atomistic molecular dynamics, we simulate the network formation and bulk properties of chemically identical liquid crystal elastomers (LCEs) and isotropic elastomers. The nematic elastomer is from a family of materials that have been shown to be auxetic at a molecular level. The network orientational order parameters and glass transition temperatures measured from our simulations are in strong agreement with experimental data. We reproduce, in silico, the magnitude and onset of strain-induced nematic order in isotropic simulations. Application of uniaxial strain to nematic LCE simulations causes biaxial order to emerge, as has been seen experimentally for these auxetic LCEs. At strains of similar to 1.0, the director reorients to be parallel to the applied strain, again as seen experimentally. The simulations shed light on the strain-induced order at a molecular level and allow insight into the individual contributions of the side-groups and crosslinker. Further, the agreement between our simulations and experimental data opens new possibilities in the computational design of high-molecular- weight liquid crystals, especially where an understanding of the properties under mechanical actuation is desired. Moreover, the simulation methodology we describe will be applicable to other combinations of orientational and/or positional order (e.g., smectics, cubics).

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