Electroplasticization of Liquid Crystal Polymer Networks

[Image: see text] Shape-shifting liquid crystal networks (LCNs) can transform their morphology and properties in response to external stimuli. These active and adaptive polymer materials can have impact in a diversity of fields, including haptic displays, energy harvesting, biomedicine, and soft robotics. Electrically driven transformations in LCN coatings are particularly promising for application in electronic devices, in which electrodes are easily integrated and allow for patterning of the functional response. The morphing of these coatings, which are glassy in the absence of an electric field, relies on a complex interplay between polymer viscoelasticity, liquid crystal order, and electric field properties. Morphological transformations require the material to undergo a glass transition that plasticizes the polymer sufficiently to enable volumetric and shape changes. Understanding how an alternating current can plasticize very stiff, densely cross-linked networks remains an unresolved challenge. Here, we use a nanoscale strain detection method to elucidate this electric-field-induced devitrification of LCNs. We find how a high-frequency alternating field gives rise to pronounced nanomechanical changes at a critical frequency, which signals the electrical glass transition. Across this transition, collective motion of the liquid crystal molecules causes the network to yield from within, leading to network weakening and subsequent nonlinear expansion. These results unambiguously prove the existence of electroplasticization. Fine-tuning the induced emergence of plasticity will not only enhance the surface functionality but also enable more efficient conversion of electrical energy into mechanical work.