Switching between 3D Surface Topographies in Liquid Crystal Elastomer Coatings Using Two-Step Imprint Lithography

While dynamic surface topographies are fabricated using liquid crystal (LC) polymers, switching between two distinct 3D topographies remains challenging. In this work, two switchable 3D surface topographies are created in LC elastomer (LCE) coatings using a two-step imprint lithography process. A first imprinting creates a surface microstructure on the LCE coating which is polymerized by a base catalyzed partial thiol-acrylate crosslinking step. The structured coating is then imprinted with a second mold to program the second topography, which is subsequently fully polymerized by light. The resulting LCE coatings display reversible surface switching between the two programmed 3D states. By varying the molds used during the two imprinting steps, diverse dynamic topographies can be achieved. For example, by using grating and rough molds sequentially, switchable surface topographies between a random scatterer and an ordered diffractor are achieved. Additionally, by using negative and positive triangular prism molds consecutively, dynamic surface topographies switching between two 3D structural states are achieved, driven by differential order/disorder transitions in the different areas of the film. It is anticipated that this platform of dynamic 3D topological switching can be used for many applications, including antifouling and biomedical surfaces, switchable friction elements, tunable optics, and beyond.     

Blueprinting Photothermal Shape-Morphing of Liquid Crystal Elastomers

Liquid crystal elastomers (LCEs) are an attractive platform for dynamic shape-morphing due to their ability to rapidly undergo large deformations. While recent work has focused on patterning the director orientation field to achieve desired target shapes, this strategy cannot be generalized to material systems where high-resolution surface alignment is impractical. Instead of programming the local orientation of anisotropic deformation, an alternative strategy for prescribed shape-morphing by programming the magnitude of stretch ratio in a thin LCE sheet with constant director orientation is developed here. By spatially patterning the concentration of gold nanoparticles, uniform illumination leads to gradients in photothermal heat generation and therefore spatially nonuniform deformation profiles that drive out-of-plane buckling of planar films into predictable 3D shapes. Experimentally realized shapes are shown to agree closely with both finite element simulations and geometric predictions for systems with unidirectional variation in deformation magnitude. Finally, the possibility to achieve complex oscillatory motion driven by uniform illumination of a free-standing patterned sheet is demonstrated.     

3D Printing of Liquid Crystal Elastomeric Actuators with Spatially Programed Nematic Order

Liquid crystal elastomers (LCEs) are soft materials capable of large, reversible shape changes, which may find potential application as artificial muscles, soft robots, and dynamic functional architectures. Here, the design and additive manufacturing of LCE actuators (LCEAs) with spatially programed nematic order that exhibit large, reversible, and repeatable contraction with high specific work capacity are reported. First, a photopolymerizable, solvent‐free, main‐chain LCE ink is created via aza‐Michael addition with the appropriate viscoelastic properties for 3D printing. Next, high operating temperature direct ink writing of LCE inks is used to align their mesogen domains along the direction of the print path. To demonstrate the power of this additive manufacturing approach, shape‐morphing LCEA architectures are fabricated, which undergo reversible planar‐to‐3D and 3D‐to‐3D′ transformations on demand, that can lift significantly more weight than other LCEAs reported to date.     

Repeatable and Reprogrammable Shape Morphing from Photoresponsive Gold Nanorod/Liquid Crystal Elastomers

Liquid crystal elastomers (LCEs) are of interest for applications such as soft robotics and shape-morphing devices. Among the different actuation mechanisms, light offers advantages such as spatial and local control of actuation via the photothermal effect. However, the unwanted aggregation of the light-absorbing nanoparticles in the LCE matrix will limit the photothermal response speed, actuation performance, and repeatability. Herein, a near-infrared-responsive LCE composite consisting of up to 0.20 wt% poly(ethylene glycol)-modified gold nanorods (AuNRs) without apparent aggregation is demonstrated. The high Young's modulus, 20.3 MPa, and excellent photothermal performance render repeated and fast actuation of the films (actuation within 5 s and recovery in 2 s) when exposed to 800 nm light at an average output power of ≈1.0 W cm⁻², while maintaining a large actuation strain (56%). Further, it is shown that the same sheet of AuNR/LCE film (100 µm thick) can be morphed into different shapes simply by varying the motifs of the photomasks.     

Bio-Inspired Soft-Rigid Hybrid Smart Artificial Muscle Based on Liquid Crystal Elastomer and Helical Metal Wire

Artificial muscles are of significant value in robotic applications. Rigid artificial muscles possess a strong load-bearing capacity, while their deformation is small; soft artificial muscles can be shifted to a large degree; however, their load-bearing capacity is weak. Furthermore, artificial muscles are generally controlled in an open loop due to a lack of deformation-related feedback. Human arms include muscles, bones, and nerves, which ingeniously coordinate the actuation, load-bearing, and sensory systems. Inspired by this, a soft-rigid hybrid smart artificial muscle (SRH-SAM) based on liquid crystal elastomer (LCE) and helical metal wire is proposed. The thermotropic responsiveness of the LCE is adopted for large reversible deformation, and the helical metal wire is used to fulfill high bearing capacity and electric heating function requirements. During actuation, the helical metal wire's resistance changes with the LCE's electrothermal deformation, thereby achieving deformation-sensing characteristics. Based on the proposed SRH-SAM, a reconfigurable blazed grating plane and the effective switch between attachment and detachment in bionic dry adhesion are accomplished. The SRH-SAM opens a new avenue for designing smart artificial muscles and can promote the development of artificial muscle-based devices.     

3D Printable and Reconfigurable Liquid Crystal Elastomers with Light-Induced Shape Memory via Dynamic Bond Exchange

3D printable and reconfigurable liquid crystal elastomers (LCEs) that reversibly shape-morph when cycled above and below their nematic-to-isotropic transition temperature (T_NI) are created, whose actuated shape can be locked-in via high-temperature UV exposure. By synthesizing LCE-based inks with light-triggerable dynamic bonds, printing can be harnessed to locally program their director alignment and UV light can be used to enable controlled network reconfiguration without requiring an imposed mechanical field. Using this integrated approach, 3D LCEs are constructed in both monolithic and heterogenous layouts that exhibit complex shape changes, and whose transformed shapes could be locked-in on demand.     

Enhanced Dynamic Adhesion in Nematic Liquid Crystal Elastomers

Smart adhesives that undergo reversible detachment in response to external stimuli enable a wide range of applications in household products, medical devices, or manufacturing. Here, a new model system for the design of smart soft adhesives that dynamically respond to their environment is presented. By exploiting the effect of dynamic soft elasticity in nematic liquid crystal elastomers (LCE), the temperature‐dependent control of adhesion to a solid glass surface is demonstrated. The adhesion strength of LCE is more than double in the nematic phase, in comparison to the isotropic phase, further increasing at higher detachment rates. The static work of adhesion, related to the interfacial energy of adhesive contact, is shown to change very little within the explored temperature range. Accordingly, the observed enhanced adhesion in the nematic phase is primarily attributable to the increased internal energy dissipation during the detachment process. This adhesion effect is correlated with the inherent bulk dynamic‐mechanical response in the nematic LCE. The reported enhanced dynamic adhesion can lead to the development of a new class of stimuli‐responsive adhesives.     

Enabling and Localizing Omnidirectional Nonlinear Deformation in Liquid Crystalline Elastomers

Liquid crystalline elastomers (LCEs) are widely recognized for their exceptional promise as actuating materials. Here, the comparatively less celebrated but also compelling nonlinear response of these materials to mechanical load is examined. Prior examinations of planarly aligned LCEs exhibit unidirectional nonlinear deformation to mechanical loads. A methodology is presented to realize surface‐templated homeotropic orientation in LCEs and omnidirectional nonlinearity in mechanical deformation. Inkjet printing of the homeotropic alignment surface localizes regions of homeotropic and planar orientation within a monolithic LCE element. The local control of the self‐assembly and orientation of the LCE, when subject to rational design, yield functional materials continuous in composition with discontinuous mechanical deformation. The variation in mechanical deformation in the film can enable the realization of nontrivial performance. For example, a patterned LCE is prepared and shown to exhibit a near‐zero Poisson's ratio. Further, it is demonstrated that the local control of deformation can enable the fabrication of rugged, flexible electronic devices. An additively manufactured device withstands complex mechanical deformations that would normally cause catastrophic failure.     

Photodeformable Azobenzene‐Containing Liquid Crystal Polymers and Soft Actuators

Photodeformable liquid crystal polymers (LCPs) that adapt their shapes in response to light have aroused a dramatic growth of interest in the past decades, since light as a stimulus enables the remote control and diverse deformations of materials. This review focuses on the growing research on photodeformable LCPs, including their basic actuation mechanisms, the various deformation modes, the newly designed molecular structures, and the improvement of processing techniques. Special attention is devoted to the novel molecular structures of LCPs, which allow for easy processing and alignment. The soft actuators with various deformation modes such as bending, twisting, and rolling in response to light are also covered with the emphasis on their photo‐induced bionic functions. Potential applications in energy harvesting, self‐cleaning surfaces, sensors, and photo‐controlled microfluidics are further illustrated. The existing challenges and future directions are discussed at the end of this review.     

Tunable Photocontrolled Motions Using Stored Strain Energy in Malleable Azobenzene Liquid Crystalline Polymer Actuators

A new strategy for enhancing the photoinduced mechanical force is demonstrated using a reprocessable azobenzene‐containing liquid crystalline network (LCN). The basic idea is to store mechanical strain energy in the polymer beforehand so that UV light can then be used to generate a mechanical force not only from the direct light to mechanical energy conversion upon the trans–cis photoisomerization of azobenzene mesogens but also from the light‐triggered release of the prestored strain energy. It is shown that the two mechanisms can add up to result in unprecedented photoindued mechanical force. Together with the malleability of the polymer stemming from the use of dynamic covalent bonds for chain crosslinking, large‐size polymer photoactuators in the form of wheels or spring‐like “motors” can be constructed, and, by adjusting the amount of prestored strain energy in the polymer, a variety of robust, light‐driven motions with tunable rolling or moving direction and speed can be achieved. The approach of prestoring a controllable amount of strain energy to obtain a strong and tunable photoinduced mechanical force in azobenzene LCN can be further explored for applications of light‐driven polymer actuators.     

Light‐Directed Liquid Manipulation in Flexible Bilayer Microtubes

Flexible microfluidic systems have potential in wearable and implantable medical applications. Directional liquid transportation in these systems typically requires mechanical pumps, gas tanks, and magnetic actuators. Herein, an alternative strategy is presented for light‐directed liquid manipulation in flexible bilayer microtubes, which are composed of a commercially available supporting layer and the photodeformable layer of a newly designed azobenzene‐containing linear liquid crystal copolymer. Upon moderate visible light irradiation, various liquid slugs confined in the flexible microtubes are driven in the preset direction over a long distance due to photodeformation‐induced asymmetric capillary forces. Several light‐driven prototypes of parallel array, closed‐loop channel, and multiple micropump are established by the flexible bilayer microtubes to achieve liquid manipulation. Furthermore, an example of a wearable device attached to a finger for light‐directed liquid motion is demonstrated in different gestures. These unique photocontrollable flexible microtubes offer a novel concept of wearable microfluidics.