Exploiting the interplay of anisotropic diamagnetic susceptibility of liquid crystalline monomers and site selective photopolymerization enables the fabrication of 3D freeforms with highly refined microstructures. Utilizing chain transfer agents in the mesogenic inks presents a pathway for broadly tuning the mechanical properties of liquid crystalline polymers and their response to stimuli. In particular, the combination of 1,4-benzenedimethanethiol and tetrabromomethane is shown to enable voxelated blueprinting of molecular order, while allowing for a modulation of the crosslink density and the mechanical properties. The formulation of these monomers allows for the resolution of the voxels to approach the limits set by the coherence lengths defined by the anchoring from surfaces. These compositions demonstrate the expected thermotropic responses while allowing for their functionalization with photochromic switches to elicit photomechanical responses. Actuation strains are shown to outstrip that accomplished with prior systems that did not access chain transfer agents to modulate the structure of the macromolecular network. Test cases of this system are shown to create freeform actuators that exploit the refined director patterns during high-resolution printing. These include topological defects, hierarchically-structured light responsive grippers, and biomimetic flyers whose flight dynamics can be actively modulated via irradiation with light. Exploiting the interplay of anisotropic diamagnetic susceptibility of liquid crystalline monomers and site selective photopolymerization enables the fabrication of 3D freeforms with highly refined microstructures.

Transversely curved composite shells of liquid crystal elastomer and polyethylene terephthalate with innervated electrodes present millisecond‐scale actuation with ≈200 mW electrical power inputs at low voltages (≈1 V). The molecular orientation is aligned to direct the thermomechanical work‐content to evert the native curvature. When powered, the curved structure initially remains latent and builds up strain energy. Thereafter, the work content is released in an ms‐scale impulse. The thin‐film actuators are powered against opposing loads to perform up to 10−5 J of work. High speed imaging reveals tip velocities of several 100 mm s−1 with powers approaching 10−4 J s−1. The design eschews bistability. After snap‐through, when the power is off, the actuator spontaneously resets to its native state. The actuation profiles are functions of the geometry and the electrical pulse patterns. The latency of actuation is reduced by powering the actuators with pulses that trigger snap‐through, allow its reset to the native state, but prevent its cooling to the ambient before subsequent actuation cycles. The actuation is harnessed in sub‐gram scale robots, including water‐strider mimicking configurations and steerable robots that can navigate on compliant (sand) and hard (slippery) surfaces. A viable template for impulsive actuation using frugal electrical power emerges.

The effect of chain extender structure and composition on the thermomechanical properties of liquid crystal elastomers (LCE) synthesized using thiol-acrylate Michael addition is presented. The intrinsic molecular stiffness of the thiol chain extender and its relative molar ratio to acrylate-based host mesogens determine the magnitudes of the thermomechanical strains, temperatures at which they are realized and the mechanical work-content. A non-linear structure-property relationship emerges, wherein higher concentrations of flexible extenders first magnify the thermomechanical sensitivity, but a continued increase leads to weaker actuation. Understanding this interplay leads to a composite material platform, enabling a peak specific work production of ∼2 J kg-1 using ∼115 mW of electrical power supplied at 2 V. Composites of LCE with eGaIn liquid metal (LM) are prepared, which act as heaters, while being capable of actuation themselves. The thermomechanically active electrodes convert the electrical power into Joule heat, which they efficiently couple with the neat LCE to which they are bound. This system harnesses the nascent responsiveness of the LCE using electrodes that work with them, instead of fighting against them (or passively standing in the way). Specific work generated increases when subjected to increasing levels of load, reaching a peak at loads ∼260× the actuator weight. These ideas are extended to tri-layered actuators, where LCE films with orthogonal molecular orientations sandwich LCE-LM composite heaters. Torsional actuation modes are harnessed to twist under load.

Contactless actuation powered using light is shown to generate torque densities approaching 10 N m kg-1 at angular velocities ∼102 rad s-1: metrics that compare favorably against tethered electromechanical systems. This is possible even though the extinction of actinic light limits the characteristic thickness of photoresponse in polymers to tens of μm. Confinement of molecularly patterned developable shells fabricated from azobenzene-functionalized liquid crystalline polymers encodes torque-dense photoactuation. Photostrain gradients from unstructured irradiation segment this geometry into two oppositely curved regions connected by a curved crease. A monolithic curved shell spontaneously bifurcates into a jointed, arm-like mechanism that generates flexure over sweep angles exceeding a radian. Strain focusing at the crease is hierarchical: an integral crease nucleates at smaller magnitudes of the prebiased curvature, while a crease decorated with point-like defects emerges at larger curvatures. The phase-space of morphogenesis is traceable to the competition between stretch and bending energies and is parameterizable as a function of the geometry. The framework for generating repetitive torque-dense actuation from slender light-powered actuators holds broader implications for the design of soft, remotely operated machines. Here, it is harnessed in illustrative mechanisms including levers, lifters and grabbers that are powered and regulated exclusively using light.

Wearable electronics, conformable sensors, and soft/micro-robotics require conductive yet stretchable thin films. However, traditional free standing metallic thin films are often brittle, inextensible, and must be processed in strict environments. This limits implementation into soft technologies where high electrical conductivity must be achieved while maintaining high compliance and conformability. Here we show a liquid metal elastomeric thin film (LET) composite with elastomer-like compliance (modulus < 500 kPa) and stretchability (>700%) with metallic conductivity (sheet resistance < 0.1 Ω/□). These 30–70 µm thin films are highly conformable, free standing, and display a unique Janus microstructure, where a fully conductive activated side is accompanied with an opposite insulated face. LETs display exceptional electro-mechanical characteristics, with a highly linear strain-resistance relationship beyond 700% deformation while maintaining a low resistance. We demonstrate the multifunctionality of LETs for soft technologies by leveraging the unique combination of high compliance and electrical conductivity with transfer capabilities for strain sensing on soft materials, as compliant electrodes in a dielectric elastomeric actuator, and as resistive heaters for a liquid crystal elastomer.

Laterally constrained arches driven between stable states by light, represent a unique space for compliant mechanism design. Exploiting mechanical multistability can overcome limitations of functional photomechanical actuators, which include limited repeatability, actuation speed, and positioning characteristics. Here, the addition of lateral constraints to an elastic bistable arch system is proposed as a method for toggling between bifurcated states by controlling the location of actinic irradiation. This approach expands the design space for photomechanical, mutistable structures and actuators. Arch behavior as a function of system parameters is simulated, including conditions leading to multistability. An experimental demonstration and exploration of a constrained photomechanical arch is also presented. It is expected that the concepts presented here could lead to innovations in areas such as energy harvesting, soft robotics, and multistable architected materials.