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Abstract Cholesteric liquid crystal elastomers (CLCEs) hold great promise for mechanochromic applications in anti‐counterfeiting, smart textiles, and soft robotics, thanks to the structural color and elasticity. While CLCEs are printed via direct ink writing (DIW) to fabricate free‐standing films, complex 3D structures are not fabricated due to the opposing rheological properties necessary for cholesteric alignment and multilayer stacking. Here, 3D CLCE structures are realized by utilizing coaxial DIW to print a CLC ink within a silicone ink. By tailoring the ink compositions, and thus, the rheological properties, the cholesteric phase rapidly forms without an annealing step, while the silicone shell provides encapsulation and support to the CLCE core, allowing for layer‐by‐layer printing of self‐supported 3D structures. As a demonstration, free‐standing bistable thin‐shell domes are printed. Color changes due to compressive and tensile stresses can be witnessed from the top and bottom of the inverted domes, respectively. When the domes are arranged in an array and inverted, they can snap back to their base state by uniaxial stretching, thereby functioning as mechanical sensors with memory. The additive manufacturing platform enables the rapid fabrication of 3D mechanochromic sensors thereby expanding the realm of potential applications for CLCEs. 

Abstract Direct ink writing (DIW) of core‐shell structures allows for patterning hollow or composite structures for shape morphing and color displays. Cholesteric liquid crystal elastomers (CLCEs) with liquid crystal mesogens assembled in a helix superstructure are attractive for generating tunable iridescent structural colors. Here, by fine‐tuning the rheology of the core and shell materials, respectively, this study creates droplets or a continuous filament in the core from the precursors of polydimethylsiloxane (PDMS) or poly(vinyl alcohol), whereas CLCE forms the outer shell. By introducing a dye in the droplets, the skin structures of cephalopods, consisting of chromatophores and iridocytes, are mimicked for enhanced color saturation, lightness, and camouflage. After removal of the core material, a CLCE hollow fiber is obtained, which can switch colors upon mechanical stretching and pneumatic actuation, much like papilla along with iridocytes. Further, liquid crystal mesogens assembled in the bulk of the fiber are in polydomain. Thus, the skin appears opalescent at room temperature, much like how leucophores enhance reflectins. Upon heating above the nematic to isotropic transition temperature, the skin becomes transparent. Lastly, a cephalopod model is constructed, where different parts of the model can change colors independently based on different mechanisms. 

Abstract A liquid crystalline elastomer (LCE) network consisting of dynamic covalent bonds (DCBs) is referred as a LCE vitrimer. The mesogen alignment and the network topology can be reprogrammed locally in the LCE vitrimer by activating the bond exchange reactions using an external stimulus. After removal of the external stress, a new network is formed and the reprogrammed shape can be fixed, leading to a different set of the physical properties of the LCE vitrimers. Herein, this type of emerging materials is reviewed by a brief introduction of the fundamentals of LCEs, followed by discussions of various DCBs and the design principles for LCE vitrimers. After a presentation of different strategies to improve the stability and reprogrammability of the registered mesogen alignment, approaches to prepare LCE vitrimers with complex shapes and their actuations are discussed. Potential applications such as self‐healing and recycling, mechanochromic effects, and post‐functionalization of nanopores are also reviewed, followed by the conclusion of the remaining challenges and opportunities. 

Abstract The giant circular photo‐galvanic effect is realized in chiral metals when illuminated by circularly polarized light. However, the structure itself is not switchable nor is the crystal chirality in the adjacent chiral domains. Here spindle‐shaped liquid crystalline elastomer microparticles that can switch from prolate to spherical to oblate reversibly upon heating above the nematic to isotropic transition temperature are synthesized. When arranged in a honeycomb lattice, the continuous shape change of the microparticles leads to lattice reconfiguration, from a right‐handed chiral state to an achiral one, then to a left‐handed chiral state, without breaking the translational symmetry. Accordingly, the sign of rotation of the polarized light passing through the lattices changes as measured by time‐domain terahertz spectroscopy. Further, it can locally alter the chirality in the adjacent domains using near‐infrared light illumination. The reconfigurable chiral microarrays will allow us to explore non‐trivial symmetry‐protected transport modes of topological lattices at the light–matter interface. Specifically, the ability to controllably create chiral states at the boundary of the achiral/chiral domains will lead to rich structures emerging from the interplay of symmetry and topology. 

Abstract Direct ink writing of liquid crystal elastomers (LCEs) offers a new opportunity to program geometries for a wide variety of shape transformation modes toward applications such as soft robotics. So far, most 3D‐printed LCEs are thermally actuated. Herein, a 3D‐printable photoresponsive gold nanorod (AuNR)/LCE composite ink is developed, allowing for photothermal actuation of the 3D‐printed structures with AuNR as low as 0.1 wt.%. It is shown that the printed filament has a superior photothermal response with 27% actuation strain upon irradiation to near‐infrared (NIR) light (808 nm) at 1.4 W cm⁻²(corresponding to 160 °C) under optimal printing conditions. The 3D‐printed composite structures can be globally or locally actuated into different shapes by controlling the area exposed to the NIR laser. Taking advantage of the customized structures enabled by 3D printing and the ability to control locally exposed light, a light‐responsive soft robot is demonstrated that can climb on a ratchet surface with a maximum speed of 0.284 mm s⁻¹(on a flat surface) and 0.216 mm s⁻¹(on a 30° titled surface), respectively, corresponding to 0.428 and 0.324 body length per min, respectively, with a large body mass (0.23 g) and thickness (1 mm). 

Pyroelectric materials that can generate electric charges when subjected to temperature changes are of interest for renewable energy. However, current flexible pyroelectric energy harvesters suffer from low output. Here, we present a nanocomposite of liquid crystalline elastomer (LCE) and pyroelectric lead zirconate titanate (PZT) nanoparticles and demonstrate a flexible heat harvesting device with high output. The overall pyroelectricity is enhanced by the secondary pyroelectricity generated from the thermal stress imposed on the LCE. Calculations and simulations corroborate with experiments, suggesting that the monodomain LCE/PZT with fixed boundaries offers the most enhancement. At a maximum heating rate of 0.20 kelvin per second, the fixed monodomain film (42.7 weight % PZT) shows an output current of 2.81 nanoamperes and a voltage of 6.23 volts, corresponding to a pyroelectric coefficientpof −4.01 nanocoulombs per square centimeter per kelvin, 49% higher than that of the widely used polyvinylidene fluoride. Our energy harvester can charge capacitors and power electronic devices such as light-emitting diodes. 

Connecting pre-bent liquid crystal elastomer fibers into a loop generates a self-regulated synchronized motion with snap through. 

Abstract Liquid crystal elastomers that offer exceptional load-deformation response at low frequencies often require consideration of the mechanical anisotropy only along the two symmetry directions. However, emerging applications operating at high frequencies require all five true elastic constants. Here, we utilize Brillouin light spectroscopy to obtain the engineering moduli and probe the strain dependence of the elasticity anisotropy at gigahertz frequencies. The Young’s modulus anisotropy, E || / E ⊥ ~2.6, is unexpectedly lower than that measured by tensile testing, suggesting disparity between the local mesogenic orientation and the larger scale orientation of the network strands. Unprecedented is the robustness of E || / E ⊥ to uniaxial load that it does not comply with continuously transformable director orientation observed in the tensile testing. Likewise, the heat conductivity is directional, κ || / κ ⊥ ~3.0 with κ ⊥ = 0.16 Wm −1 K −1 . Conceptually, this work reveals the different length scales involved in the thermoelastic anisotropy and provides insights for programming liquid crystal elastomers on-demand for high-frequency applications.