How microscopic chirality is reflected in macroscopic scale to form various chiral shapes, such as straight helicoids and spiral ribbons, and how the degree of macroscopic chirality can be controlled are a focus of studies on the shape formation of many biomaterials and supramolecular systems. This article investigates both experimentally and theoretically how the chiral arrangement of liquid crystal mesogens in twist-nematic-elastomer films induces the formation of helicoids and spiral ribbons because of the coupling between the liquid crystalline order and the elasticity. It is also shown that the pitch of the formed ribbons can be tuned by temperature variation. The results of this study will facilitate the understanding of physics for the shape formation of chiral materials and the designing of new structures on basis of microscopic chirality.liquid crystal elastomers | chiral imprinting R ecent researches have revealed that chirality plays a critical role in controlling the shape of self-assembled supramolecular aggregates. A range of chiral shapes, including tubes with "barber-pole" markings, spiral ribbons (with cylindrical curvature and helical central line), and helicoids (with Gaussian saddle-like curvature and straight central line), have been observed in a rich variety of biological materials and their synthetic analogues. These materials include several amphiphiles (1-3), peptides (4-7), diacetylenic lipids (8, 9), gemini surfactants (10, 11), and multicomponent mixtures in bile (12, 13). Such aggregates often become bilayers, and the bilayer membranes form tubules, spiral ribbons, or helicoids in contrast to the normal expectation that the minimum energy state of the bilayers would be flat, or be large spherical vesicles with the minimum curvature. In addition, the correlation between material characteristics and the macroscopic shape of chiral aggregates is markedly complicated. For example, mixed bilayers of saturated and diacetylenic phospholipids change their shape between micron-scale cylindrical tubules, spiral ribbons, or nanometer-scale tubules, in response to temperature variation (14). Charged gemini surfactants with chiral counterions show a transition between spiral ribbons and helicoids as a function of molecular chain length (10). Many theoretical studies have been reported to explain what determines the size and shape of tubules, helicoids, and spiral ribbons (10,(15)(16)(17)(18).In this article, we will show, both experimentally and theoretically, how a flat twist-nematic-elastomer (TNE) film when subjected to temperature change can easily achieve the goal of shape selection between helicoids and spiral ribbons. Nematic elastomers (NEs) are a unique class of materials (19-23). Formed by cross-linking liquid crystalline polymers, NEs possess both the elastic properties of rubbers and the orientational properties of liquid crystals. The combination of these two properties makes the shape of NEs very sensitive to external stimuli. In this article, we will focus on NE films in which the...

This work describes the fabrication, characterization, and modelling of liquid crystalline polymer network films with a multiple patterned 3D nematic director profile, a stimuli‐responsive material that exhibits complex mechanical actuation under change of temperature or pH. These films have a discrete alternating striped or checkerboard director profile in the plane, and a 90‐degree twist through the depth of the film. When actuated via heating, the striped films deform into accordion‐like folds, while the film patterned with a checkerboard microstructure buckles out‐of‐plane. Furthermore, striped films are fabricated so that they also deform into an accordion shaped fold, by a change of pH in an aqueous environment. Three‐dimensional finite element simulations and elasticity analysis provide insight into the dependence of shape evolution on director microstructure and the sample's aspect ratio.

While ∼75% of commercially utilized polymers are semicrystalline, the generally low mechanical modulus of these materials, especially for those possessing a glass transition temperature below room temperature, restricts their use for structural applications. Our focus in this paper is to address this deficiency through the controlled, multiscale assembly of nanoparticles (NPs), in particular by leveraging the kinetics of polymer crystallization. This process yields a multiscale NP structure that is templated by the lamellar semicrystalline polymer morphology and spans NPs engulfed by the growing crystals, NPs ordered into layers in the interlamellar zone [spacing of (10–100 nm)], and NPs assembled into fractal objects at the interfibrillar scale, (1–10 μm). The relative fraction of NPs in this hierarchy is readily manipulated by the crystallization speed. Adding NPs usually increases the Young’s modulus of the polymer, but the effects of multiscale ordering are nearly an order of magnitude larger than those for a state where the NPs are not ordered, i.e., randomly dispersed in the matrix. Since the material’s fracture toughness remains practically unaffected in this process, this assembly strategy allows us to create high modulus materials that retain the attractive high toughness and low density of polymers.

Using both experiments and finite element simulations, we explore the shape evolution of off-axis twist nematic elastomer ribbons as a function of temperature. The elastomers are prepared by cross-linking the mesogens with planar anchoring of the director at top and bottom surfaces with a 90° left-handed twist. Shape evolution depends sensitively on the off-axis director orientation at the sample midplane. Both experiments and theoretical studies show that when the director at midplane is parallel to either the ribbon's long or short axes, ribbons form either helicoids or spirals depending on aspect ratio and temperature. Simulation studies show that if the director at midplane is off-axis, ribbons never form helicoids, instead evolving to distorted spiral shapes. Experimental studies for two samples with off-axis geometry show agreement with this prediction. Samples in all these geometries show a remarkable transition from right- to left-handed chiral shapes on change of temperature. Simulations predict off-axis samples also change their macroscopic chirality at fixed temperature, depending on the angular offset. These results provide insight into the mechanisms driving shape evolution and macroscopic chirality, enabling engineering design of these materials for future applications.

Various experimental and theoretical studies demonstrate that complex stimulus-responsive out-of-plane distortions such as twist of different chirality, emergence of cones, simple and anticlastic bending can be engineered and pre-programmed in a liquid crystalline rubbery material given a well-controlled director microstructure. Via 3-d finite element simulation studies, we demonstrate director-encoded chiral shape actuation in thin-film nematic polymer networks under external stimulus. Furthermore, we design two complex director fields with twisted nematic domains and nematic disclinations that encode a pattern of folds for an auto-origami box. This actuator will be flat at a reference nematic state and form four well-controlled bend distortions as orientational order changes. Device fabrication is applicable via current experimental techniques. These results are in qualitative agreement with theoretical predictions, provide insight into experimental observations, and demonstrate the value of finite element methods at the continuum level for designing and engineering liquid crystal polymeric devices.

Liquid crystal elastomers represent a novel class of programmable shape-transforming materials whose shape-change trajectory is encoded in the material's nematic director field. Using three-dimensional non-linear finite element elastodynamics simulation, we model a variety of different actuation geometries and device designs: thin films containing topological defects, patterns that induce formation of folds and twists, and a bas-relief structure. The inclusion of finite bending energy in the simulation model reveals features of actuation trajectory that may be absent when bending energy is neglected. We examine geometries with a director pattern uniform through the film thickness encoding multiple regions of positive Gaussian curvature. Simulations indicate that heating such a system uniformly produces a disordered state with curved regions emerging randomly in both directions due to the film's up/down symmetry. In contrast, applying a thermal gradient by heating the material first on one side breaks up/down symmetry and results in a deterministic trajectory, producing a more ordered final shape. We demonstrate that a folding zone design containing cut-out areas accommodates transverse displacements without warping or buckling, and demonstrate that bas-relief and more complex bent/ twisted structures can be assembled by combining simple design motifs.

We study the rich actuation variety displayed by elastomers that combine well-defined isotropic regions and liquid crystalline regions. Design factors for actuation include orientation of director and pattern, domain-size and sample-size.

Programming shape changes in soft materials requires precise control of the directionality and magnitude of their mechanical response. Among ordered soft materials, liquid crystal elastomers (LCEs) exhibit remarkable and programmable shape shifting when their molecular order changes. In this work, we synthesized, remotely programmed, and modeled reversible and complex morphing in monolithic LCE kirigami encoded with predesigned topological patterns in its microstructure. We obtained a rich variety of out-of-plane shape transformations, including auxetic structures and undulating morphologies, by combining different topological microstructures and kirigami geometries. The spatiotemporal shape-shifting behaviors are well recapitulated by elastodynamics simulations, revealing that the complex shape changes arise from integrating the custom-cut geometry with local director profiles defined by topological defects inscribed in the material. Different functionalities, such as a bioinspired fluttering butterfly, a flower bud, dual-rotation light mills, and dual-mode locomotion, are further realized. Our proposed LCE kirigami with topological patterns opens opportunities for the future development of multifunctional devices for soft robotics, flexible electronics, and biomedicine.