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Stimulus‐responsive polymers are attractive for microactuators because they can be easily miniaturized and remotely actuated, enabling untethered operation. In this work, magnetic Fe microparticles are dispersed in a thermoplastic polyurethane shape memory polymer matrix and formed into artificial, magnetic cilia by solvent casting within the vertical magnetic field in the gap between two permanent magnets. Interactions of the magnetic moments of the microparticles, aligned by the applied magnetic field, drive self‐assembly of magnetic cilia along the field direction. The resulting magnetic cilia are reconfigurable using light and magnetic fields as remote stimuli. Temporary shapes obtained through combined magnetic actuation and photothermal heating can be locked by switching off the light and magnetic field. Subsequently turning on the light without the magnetic field drives recovery of the permanent shape. The permanent shape can also be reprogrammed after preparing the cilia by applying mechanical constraints and annealing at high temperature. Spatially controlled actuation is demonstrated by applying a mask for optical pattern transfer into the array of magnetic cilia. A theoretical model is developed for predicting the response of shape memory magnetic cilia and elucidates physical mechanisms behind observed phenomena, enabling the design and optimization of ciliary systems for specific applications.

 

Soft intelligent structures that are programmed to reshape and reconfigure under magnetic field can find applications such as in soft robotics and biomedical devices. Here, a new class of smart elastomeric architectures that undergo complex reconfiguration and shape change in applied magnetic fields, while floating on the surface of water, is reported. These magnetoactive soft actuators are fabricated by 3D printing with homocomposite silicone capillary ink. The ultrasoft actuators easily deform by the magnetic force exerted on carbonyl iron particles embedded in the silicone, as well as lateral capillary forces. The tensile and compressive moduli of the actuators are easily determined by their topological design through 3D printing. As a result, their responses can be engineered by the interplay of the intensity of the magnetic field gradient and the programmable moduli. 3D printing allows us to fabricate soft architectures with different actuation modes, such as isotropic/anisotropic contraction and multiple shape changes, as well as functional reconfiguration. Meshes that reconfigure in magnetic fields and respond to external stimuli by reshaping could serve as active tissue scaffolds for cell cultures and soft robots mimicking creatures that live on the surface of water.

 

The organization of plasmonic nanoparticles (NPs) determines the strength and polarization dependence of coupling of their surface plasmons. In this study, plasmon coupling of spherical Au NPs with an average diameter of 15 nm was investigated in shape-memory polymer films before and after mechanical stretching and then after thermally driving shape recovery. Clusters of Au NPs form when preparing the films that exhibit strong plasmon coupling. During stretching, a significant polarization-dependent response develops, where the optical extinction maximum corresponding to the surface plasmon resonance is redshifted by 19 nm and blueshifted by 7 nm for polarization parallel and perpendicular to the stretching direction, respectively. This result can be explained by non-uniform stretching on the nanoscale, where plasmon coupling increases parallel to the shear direction as Au NPs are pulled into each other during stretching. The polarization dependence vanishes after shape recovery, and structural characterization confirms the return of isotropy consistent with complete nanoscale recovery of the initial arrangement of Au NPs. Simulations of the polarized optical responses of Au NP dimers at different interparticle spacings establish a plasmon ruler for estimating the average interparticle spacings within the experimental samples. An investigation of the temperature-dependent recovery behavior demonstrates an application of these materials as optical thermal history sensors. 

New materials are advancing the field of soft robotics. Composite films of magnetic iron microparticles dispersed in a shape memory polymer matrix are demonstrated for reconfigurable, remotely actuated soft robots. The composite films simultaneously respond to magnetic fields and light. Temporary shapes obtained through combined magnetic actuation and photothermal heating can be locked by switching off the light and magnetic field. Subsequent illumination in the absence of the magnetic field drives recovery of the permanent shape. In cantilevers and flowers, multiple cycles of locking and unlocking are demonstrated. Scrolls show that the permanent shape of the film can be programmed, and they can be frozen in intermediate configurations. Bistable snappers can be magnetically and optically actuated, as well as biased, by controlling the permanent shape. Grabbers can pick up and release objects repeatedly. Simulations of combined photothermal heating and magnetic actuation are useful for guiding the design of new devices.