Programming Anisotropic Functionality of 3D Microdenticles by Staggered-Overlapped and Multilayered Microarchitectures.

Natural sharkskin features staggered-overlapped and multilayered architectures of riblet-textured anisotropic microdenticles, exhibiting drag reduction and providing a flexible yet strong armor. However, the artificial fabrication of three-dimensional (3D) sharkskin with these unique functionalities and mechanical integrity is a challenge using conventional techniques. In this study, it is reported on the facile microfabrication of multilayered 3D sharkskin through the magnetic actuation of polymeric composites and subsequent chemical shape fixation by casting thin polymeric films. The fabricated hydrophobic sharkskin, with geometric symmetry breaking, achieves anisotropic drag reduction in frontal and backward flow directions against the riblet-textured microdenticles. For mechanical integrity, hard-on-soft multilayered mechanical properties are realized by coating the polymeric sharkskin with thin layers of zinc oxide and platinum, which have higher hardness and recovery behaviors than the polymer. This multilayered hard-on-soft sharkskin exhibits friction anisotropy, mechanical robustness, and structural recovery. Furthermore, coating the MXene nanosheets provides the fabricated sharkskin with a low electrical resistance of ≈5.3 Ω, which leads to high Joule heating (≈229.9 °C at 2.75 V). The proposed magnetomechanical actuation-assisted microfabrication strategy is expected to facilitate the development of devices requiring multifunctional microtextures.

Multimodal collective swimming of magnetically articulated modular nanocomposite robots.

Magnetically responsive composites can impart maneuverability to miniaturized robots. However, collective actuation of these composite robots has rarely been achieved, although conducting cooperative tasks is a promising strategy for accomplishing difficult missions with a single robot. Here, we report multimodal collective swimming of ternary-nanocomposite-based magnetic robots capable of on-demand switching between rectilinear translational swimming and rotational swimming. The nanocomposite robots comprise a stiff yet lightweight carbon nanotube yarn (CNTY) framework surrounded by a magnetic polymer composite, which mimics the hierarchical architecture of musculoskeletal systems, yielding magnetically articulated multiple robots with an agile above-water swimmability (~180 body lengths per second) and modularity. The multiple robots with multimodal swimming facilitate the generation and regulation of vortices, enabling novel vortex-induced transportation of thousands of floating microparticles and heavy semi-submerged cargos. The controllable collective actuation of these biomimetic nanocomposite robots can lead to versatile robotic functions, including microplastic removal, microfluidic vortex control, and transportation of pharmaceuticals.

On-Demand Dynamic Chirality Selection in Flower Corolla-like Micropillar Arrays.

Chiral morphology has been intensively studied in various fields including biology, organic chemistry, pharmaceuticals, and optics. On-demand and dynamic chiral inversion not only cannot be realized in most intrinsically chiral materials but also has mostly been limited to chemical or light-induced methods. Herein, we report reversible real-time magneto-mechanical chiral inversion of a three-dimensional (3D) micropillar array between achiral, clockwise, and counterclockwise chiral arrangements. Inspired by the flower corolla, achiral arrays of five and six radially arranged semicylindrical micropillars were employed as model systems to investigate the dynamic symmetry properties of arrays consisting of odd and even numbers of micropillars, respectively. Each micropillar underwent twisting actuation with a different twisting angle depending on the angle with the magnetic field direction and magnetic flux density, thereby collectively changing the chirality from the achiral to chiral state. Importantly, the morphological handedness of the micropillars was inverted within a few seconds by manipulating the direction of the magnetic field. A chiral morphology consisting of magnetically twisted micropillars was shape-fixed by the introduction of a polymeric binder. This binder could be simply washed off to return the shape-fixed twisted micropillars to their initial straight state. Magnetically programmable and reproducible 3D flower corolla-like micropillar arrays are expected to expand the potential of shape-reconfigurable devices that require real-time chiral manipulation in ambient environments.

High-Speed Production of Crystalline Semiconducting Polymer Line Arrays by Meniscus Oscillation Self-Assembly.

Evaporative self-assembly of semiconducting polymers is a low-cost route to fabricating micrometer and nanoscale features for use in organic and flexible electronic devices. However, in most cases, rate is limited by the kinetics of solvent evaporation, and it is challenging to achieve uniformity over length- and time-scales that are compelling for manufacturing scale-up. In this study, we report high-throughput, continuous printing of poly(3-hexylthiophene) (P3HT) by a modified doctor blading technique with oscillatory meniscus motion-meniscus-oscillated self-assembly (MOSA), which forms P3HT features ∼100 times faster than previously reported techniques. The meniscus is pinned to a roller, and the oscillatory meniscus motion of the roller generates repetitive cycles of contact-line formation and subsequent slip. The printed P3HT lines demonstrate reproducible and tailorable structures: nanometer scale thickness, micrometer scale width, submillimeter pattern intervals, and millimeter-to-centimeter scale coverage with highly defined boundaries. The line width as well as interval of P3HT patterns can be independently controlled by varying the polymer concentration levels and the rotation rate of the roller. Furthermore, grazing incidence wide-angle X-ray scattering (GIWAXS) reveals that this dynamic meniscus control technique dramatically enhances the crystallinity of P3HT. The MOSA process can potentially be applied to other geometries, and to a wide range of solution-based precursors, and therefore will develop for practical applications in printed electronics.

Enhancement of Magneto-Mechanical Actuation of Micropillar Arrays by Anisotropic Stress Distribution.

Magnetically active shape-reconfigurable microarrays undergo programmed actuation according to the arrangement of magnetic dipoles within the structures, achieving complex twisting and bending deformations. Cylindrical micropillars have been widely used to date, whose circular cross-sections lead to identical actuation regardless of the actuating direction. In this study, micropillars with triangular or rectangular cross-sections are designed and fabricated to introduce preferential actuation directions and explore the limits of their actuation. Using such structures, controlled liquid wetting is demonstrated on micropillar surfaces. Liquid droplets pinned on magnetic micropillar arrays undergo directional spreading when the pillars are actuated as depinning of the droplets is enabled only in certain directions. The enhanced deformation due to direction dependent magneto-mechanical actuation suggests that micropillar arrays can be fundamentally tailored to possess application specific responses and opens up opportunities to exploit more complex designs such as micropillars with polygonal cross sections. Such tunable wetting of liquids on microarray surfaces has potential to improve printing technologies via contactless reconfiguration of stamp geometry by magnetic field manipulation.

Light-driven complex 3D shape morphing of glassy polymers by resolving spatio-temporal stress confliction.

Programmable 3D shape morphing of hot-drawn polymeric sheets has been demonstrated using photothermal local shrinkage of patterned hinges. However, the hinge designs have been limited to simple linear hinges used to generate in-plane local folding or global curvature. Herein, we report an unprecedented design strategy to realize localized curvature engineering in 3D structures employing radial hinges and stress-releasing facets on 2D polymeric sheets. The shape and height of the 3D structures are readily controlled by varying the number of radial patterns. Moreover, they are numerically predictable by finite elemental modeling simulation with consideration of the spatio-temporal stress distribution, as well as of stress competition effects. Localized curvature engineering provides programming capabilities for various designs including soft-turtle-shell, sea-shell shapes, and saddle architectures with the desired chirality. The results of local curvilinear actuation with quantifiable stress implies options to advance the applicability of self-folded architectures embodying coexisting curved and linear geometric surfaces.

Shape-Programmed Fabrication and Actuation of Magnetically Active Micropost Arrays.

Micro- and nanotextured surfaces with reconfigurable textures can enable advancements in the control of wetting and heat transfer, directed assembly of complex materials, and reconfigurable optics, among many applications. However, reliable and programmable directional shape in large scale is significant for prescribed applications. Herein, we demonstrate the self-directed fabrication and actuation of large-area elastomer micropillar arrays, using magnetic fields to both program a shape-directed actuation response and rapidly and reversibly actuate the arrays. Specifically, alignment of magnetic microparticles during casting of micropost arrays with hemicylindrical shapes imparts a deterministic anisotropy that can be exploited to achieve the prescribed, large-deformation bending or twisting of the pillars. The actuation coincides with the finite element method, and we demonstrate reversible, noncontact magnetic actuation of arrays of tens of thousands of pillars over hundreds of cycles, with the bending and twisting angles of up to 72 and 61°, respectively. Moreover, we demonstrate the use of the surfaces to control anisotropic liquid spreading and show that the capillary self-assembly of actuated micropost arrays enables highly complex architectures to be fabricated. The present technique could be scaled to indefinite areas using cost-effective materials and casting techniques, and the principle of shape-directed pillar actuation can be applied to other active material systems.

On-demand orbital maneuver of multiple soft robots via hierarchical magnetomotility.

Magnetic soft robots facilitate the battery-free remote control of soft robots. However, parallel control of multiple magnetic robots is challenging due to interference between robots and difficult maneuvers. Here we present the orbital maneuvering of manifold magnetic soft robots. Magneto-induced motion (magnetomotility) that includes the hierarchy of rotation and resultant revolution allows for the independent control of the robot's velocity and orbital radius. The soft robot achieves a speed of 60 body length (BL) s-1, which is approximately 50, 000 times faster with 1/7 the weight of the current lightest legged soft robot. The hierarchical magnetomotility is suitable for versatile locomotion such as stairs and uphill climbing, underwater and above water swimming. Owing to their swimming functionality, a swarm of such soft robots is capable of transportation of cargo. On-demand orbital maneuvering of magnetic soft robots provides a new methodology for concurrent actuation of multiple robots exhibiting collective behaviors.

Contactless Manipulation of Soft Robots.

In recent years, jointless soft robots have demonstrated various curvilinear motions unlike conventional robotic systems requiring complex mechanical joints and electrical design principles. The materials employed to construct soft robots are mainly programmable anisotropic polymeric materials to achieve contactless manipulation of miniaturized and lightweight soft robots through their anisotropic strain responsivity to external stimuli. Although reviews on soft actuators are extensive, those on untethered soft robots are scant. In this study, we focus on the recent progress in the manipulation of untethered soft robots upon receiving external stimuli such as magnetic fields, light, humidity, and organic solvents. For each external stimulus, we provide an overview of the working principles along with the characteristics of programmable anisotropic materials and polymeric composites used in soft robotic systems. In addition, potential applications for untethered soft robots are discussed based on the physicochemical properties of programmable anisotropic materials for the given external stimuli.

Magnetomotility of untethered helical soft robots.

Magnetically active helical soft robots were synthesized to achieve tether-less manipulation of the magnetomotility in order to avoid the on-board weight penalty and the distance restrictions originating from connection lines. Magnetic iron particles were dispersed in elastomeric polymer matrices and pre-cured in a two-dimensional film geometry, followed by post-curing in a three-dimensional (3D) helical geometry. To manipulate movements of the 3D helical soft robots, an external magnetic field was applied by placing a neodymium permanent magnet on a motorized linear translation stage. The 3D helical geometry of the soft robots enabled efficient maneuvering with local deformations and a low magnetic threshold for actuation by the introduction of the rolling resistance unlike the absence of the local deformations observed for rigid 3D coils. As rolling is induced by the action and reaction with the substrate, the helix angle causes divergence of the soft robots from linear translational motility. In order to regulate the directionality of rolling and to minimize temporal and spatial deviation of the soft robots, the magnitude of the magnetic flux density and the velocity of the permanent magnet on the linear stage were investigated.

Chan-Lam coupling reaction of sulfamoyl azides with arylboronic acids for synthesis of unsymmetrical N-arylsulfamides.

An efficient method was developed for the synthesis of unsymmetrical N-arylsulfamides using sulfamoyl azides and arylboronic acids in the presence of 10 mol% of copper chloride as the catalyst. The reaction was facilitated in MeOH in an open flask at room temperature. Unlike the coupling of sulfamides and boronic acids, the use of sulfamoyl azides was found to be beneficial with respect to the yield and reaction time.