3D‐Architected Soft Machines with Topologically Encoded Motion

The limited range of mechanical responses achievable by materials compatible with additive manufacturing hinders the 3D printing of continuum soft robots with programmed motion. This paper describes the rapid design and fabrication of low‐density, 3D‐architected soft machines (ASMs) by combining Voronoi tessellation and additive manufacturing. On tendon‐based actuation, ASMs deform according to the topologically encoded buckling of their structure to produce a wide range of motions (contraction, twisting, bending, and cyclic motion). ASMs exhibiting densities as low as 0.094 g cm^?3 (≈8% of bulk polymer) can be rapidly built by the stereolithographic 3D printing of flexible photopolymers or the injection molding of elastomers. The buckling of ASMs can be programmed by inducing gradients in the thickness of their flexible beams or by the localized enlargement of the Voronoi cells to generate complex motions such as multi‐finger gripping or quadrupedal locomotion. The topological architecture of these low‐density soft robots confers them with the stiffness necessary to recover their original shape even after ultrahigh compression (400%) and extension (500%). ASMs expand the range of mechanical properties currently achievable by 3D printed or molded materials to enable the fabrication of soft machines with auxetic mechanical metamaterial properties.     

Programmable Hierarchical Kirigami

Kirigami—the Japanese art of cutting paper—has recently inspired the design of highly stretchable and morphable mechanical metamaterials that can be easily realized by embedding an array of cuts into a sheet. This study focuses on thin plastic sheets perforated with a hierarchical pattern of cuts arranged to form an array of hinged squares. It is shown that by tuning the geometric parameters of this hierarchy as well as thickness and material response of the sheets not only a variety of different buckling‐induced 3D deformation patterns can be triggered, but also the stress–strain response of the surface can be effectively programmed. Finally, it is shown that when multiple hierarchical patterns are brought together to create one combined heterogeneous surface, the mechanical response can be further tuned and information can be encrypted into and read out via the applied mechanical deformation.     

Non-Hierarchical Architected Materials with Extreme Stiffness and Strength

Stretch-dominated truss and plate microstructures are contenders in the quest for realizing architected materials with extreme stiffness and strength. In the low volume fraction limit, closed-cell isotropic plate microstructures meet theoretical upper bounds on stiffness but have low buckling strength, whereas open-cell truss microstructures have high buckling strength at the cost of significantly reduced stiffness. At finite volume fractions, the picture becomes less clear but both are outperformed by hollow truss lattice and hierarchical microstructures in terms of buckling strength. Despite significant advances in manufacturing methods, hollow and multi-scale hierarchical microstructures are still challenging to build. The question is if there exist realizable microstructures providing stiffness and strength matching or even beating hard-to-realize hollow or hierarchical microstructures? Herein, single-scale non-hierarchical (first order) microstructures that beat the buckling strength of hollow truss lattice structures by a factor of 2.4 and first- and second-order plate microstructures by factors of 5 and 1.4, respectively, are systematically designed, built, and tested. Stiffness of the microstructures is within 40% of theoretical bounds and beats both truss and second order plate microstructures. The microstructures are realized with 3D printing. Experiments validate theoretical predictions and additional insight is provided through numerical modeling of a CT-scanned sample.     

Three‐Dimensional Printing of Elastomeric,Cellular Architectures with Negative Stiffness

Three‐dimensional printing of viscoelastic inks to create porous, elastomeric architectures with mechanical properties governed by the ordered arrangement of their sub‐millimeter struts is reported. Two layouts are patterned, one resembling a “simple cubic” (SC)‐like structure and another akin to a “face‐centered tetragonal” (FCT) configuration. These structures exhibit markedly distinct load response with directionally dependent behavior, including negative stiffness. More broadly, these findings suggest the ability to independently tailor mechanical response in cellular solids via micro‐architected design. Such ordered materials may one day replace random foams in mechanical energy absorption applications.     

3D Transformable Modular Kirigami Based Programmable Metamaterials

Kirigami, the ancient paper art of cutting, has recently emerged as a new approach to construct metamaterials with novel properties imparted by cuts. However, most studies are limited to thin sheets-based 2D kirigami metamaterials with specific forms and limited reconfigurability due to planar connection constraints of cut units. Here, 3D modular kirigami is introduced by cutting bulk materials into spatially closed-loop connected cut cubes to construct a new class of 3D kirigami metamaterials. The module is transformable with multiple degrees of freedom that can transform into versatile distinct daughter building blocks. Their conformable assembly creates a wealth of reconfigurable and disassemblable metamaterials with diverse structures and unique properties, including reconfigurable 1D column-like materials, 2D lattice-like metamaterials with phase transition of chirality, as well as 3D frustration-free multilayered metamaterials with 3D auxetic behaviors and programmable deformation modes. This study largely expands the design space of kirigami metamaterials from 2D to 3D.     

Reversible Programing of Soft Matter with Reconfigurable Mechanical Properties

Biology uses various cross‐linking mechanisms to tailor material properties, and this is inspiring technological efforts to couple independent cross‐linking mechanisms to create hydrogels with complex mechanical properties. Here, it is reported that a hydrogel formed from a single polysaccharide can be triggered to reversibly switch cross‐linking mechanisms and switch between elastic and viscoelastic properties. Specifically, the pH‐responsive self‐assembling aminopolysaccharide chitosan is used. Under acidic conditions, chitosan is polycationic and can be electrostatically cross‐linked by sodium dodecyl sulfate (SDS) micelles to confer viscoelastic and self‐healing properties. Under basic conditions, chitosan becomes neutral, the electrostatic SDS–chitosan interactions are no longer operative, and chitosan chains can self‐assemble to form crystalline network junctions that serve as strong physical cross‐links that confer elastic properties. Mechanical measurements performed in water demonstrate these different mechanical behaviors and the repeated pH‐induced switching between these behaviors. Printing of SDS micelles onto a neutral chitosan film allows the cross‐linking mechanisms to be spatially programed to confer anisotropic mechanical properties. The reversibility of these cross‐linking mechanisms allows the patterned films to be erased and reprogramed with reconfigured mechanical properties. Potentially, the ability to reversibly program hydrogel networks enables fabrication of the dynamically reconfigurable networks required for soft machines.     

Elastic Energy Storage Enables Rapid and Programmable Actuation in Soft Machines

Storage of elastic energy is key to increasing the efficiency, speed, and power output of many biological systems. This paper describes a simple design strategy for the rapid fabrication of prestressed soft actuators (PSAs), exploiting elastic energy storage to enhance the capabilities of soft robots. The elastic energy that PSAs store in their prestressed elastomeric layer enables the fabrication of grippers capable of zero‐power holding up to 100 times their weight and perching upside down from angles of up to 116°. The direction and magnitude of the force used to prestress the elastomeric layer can be controlled not only to define the final shape of the PSA but also to program its actuation sequence. Additionally, the release of the elastic energy stored by PSAs causes their high‐speed recovery (≈50 ms), which significantly improves the actuation rates of soft pneumatic actuators, especially after motions requiring large deformations. Moreover, judicious prestressing of PSAs can also create bistable soft robotic systems, which use their stored elastic energy as a source of power amplification for rapid movements. These strategies serve as a basis for a new class of entirely soft robots capable of recreating bioinspired high‐powered and high‐speed motions using stored elastic energy.     

Morphodynamic Tissues via Integrated Programmable Shape Memory Actuators

Manipulating the shape of preformed living tissues can present a novel fabrication route toward complex biological architectures. However, external manipulation of tissues can be challenging to implement robustly at multiple length scales and with high degrees of freedom, particularly in soft fibrous tissue constructs. Here, a versatile platform is developed to drive soft tissue morphodynamics using embeddable shape memory actuators that generate multiscale, repetitive, and highly customized tissue deformation on demand. To achieve this, a thermally isolating coating technique is designed and developed for programmable shape memory wires, which protects surrounding biological materials from cytotoxic heating effects during wire actuation. The coated tissue actuators (CTAs) can then be embedded in engineered tissues and activated to produce both large‐ and small‐scale tissue deformations in a highly customized and reproducible manner. Using this strategy, tissues can be forced to adopt specified shapes, with precise control over cell elongation and orientation within an encapsulating matrix. Furthermore, the system can produce predictable, highly localized, and customizable strains within fibrous matrices, capable of elongating cells and biasing their orientation within degrees of a desired direction. This strategy may hence have broad applicability in both applied tissue biofabrication and for fundamental studies of cell–matrix interactions.     

Multifunctional Mechanical Metamaterials with Embedded Triboelectric Nanogenerators

The flexibility of planar triboelectric nanogenerators (TENGs) enables them to be embedded into structures with complex geometries and to conform with any deformation of these structures. In return, the embedded TENGs function as either strain‐sensitive active sensors or energy harvesters while negligibly affecting the structure's original mechanical properties. This advantage inspires a new class of multifunctional materials where compliant TENGs are distributed into local operational units of mechanical metamaterial, dubbed TENG‐embedded mechanical metamaterials. This new class of metamaterial inherits the advantages of a traditional mechanical metamaterial, in that the deformation of the internal topology of material enables unusual mechanical properties. The concept is illustrated with experimental investigations and finite element simulations of prototypes based on two exemplar metamaterial geometries where functions of self‐powered sensing, energy harvesting, as well as the designated mechanical behavior are investigated. This work provides a new framework in producing multifunctional triboelectric devices.     

Zero-Power Shape Retention in Soft Pneumatic Actuators with Extensional and Bending Multistability

Power-free shape retention enables soft pneumatic robots to reduce energy cost and avoid unexpected collapse due to burst or puncture. Existing strategies for pneumatic actuation cannot attain motion locking for trajectories combining extension and bending, one of the most common modes of operation. Here, a design paradigm is introduced for soft pneumatic actuators to enable zero-power locking for shape retention in both extension and bending. The underpinning mechanism is the integration of a pneumatic transmitter and a multistable guider, which are programmed to interact for balanced load transfer, flexural and extension steering, and progressive snapping leading to state locking. Through theory, simulations, and experiments on proof-of-concept actuators, the existence of four distinct regimes of deformation is unveiled, where the constituents first interact during inflation to attain locking in extension and bending, and then cooperate under vacuum to enable fully reversible functionality. Finally, the design paradigm is demonstrated to realize a soft robotic arm capable to lock at desired curvature states at zero-power, and a gripper that safely operates with puncture resistance to grasp and hold objects of various shapes and consistency. The study promises further development for zero-power soft robots endowed with multiple deformation modes, sequential deployment, and tunable multistability.     

Programmable Melt Electrowriting to Engineer Soft Connective Tissues with Prescribed,Biomimetic, Biaxial Mechanical Properties

Appropriate load-bearing function of soft connective tissues is provided by their nonlinear and often anisotropic mechanics. Recapitulating such complex mechanical behavior in tissue-engineered structures is particularly crucial, as deviation from native tissue mechanics can trigger pathological biomechanical pathways, causing adverse tissue remodeling and dysfunction. Here, a novel method combining computational modeling, melt electrowriting (MEW), and design of experiments (DOE) is reported to generate scaffolds composed of sinusoidal fibers with prescribed biaxial mechanical properties, recapitulating the distinct nonlinear, anisotropic stress–strain behavior of three model tissues: adult aortic valve, pediatric pulmonary valve, and pediatric pericardium. Finite element analysis is used to efficiently optimize scaffold architecture over a broad parameter space, representing up to 65 conditions, to define MEW print parameters to achieve polycaprolactone scaffolds with target mechanical properties. Architectural parameters are further optimized experimentally using DOE and regression to account for uncertainties involved in the simulation, yielding functional scaffolds with accurate, prescribed mechanics. The prescribed architecture also primarily governs the mechanics of hybrid structures generated by casting cell-laden fibrin hydrogel within the scaffolds. This high-fidelity approach recapitulates biaxial mechanical properties over a broad range of mechanical nonlinearity and anisotropy and is generalizable for programmed biofabrication in a variety of tissue engineering applications.     

Data-Driven Approach to Tailoring Mechanical Properties of a Soft Material

Data-driven, machine learning (ML)-assisted approaches have been used to study structure-property relationships at the atomic scale, which have greatly accelerated the screening process and new material discovery. However, such approaches are not easily applicable to modulating material properties of a soft material in a laboratory with specific ingredients. Moreover, it is desirable to relate material properties directly to the experimental recipes. Herein, a data-driven approach to tailoring mechanical properties of a soft material is demonstrated using ML-assisted predictions of mechanical properties based on experimental synthetic recipes. Polyurethane (PU) elastomer is used as a model soft material to demonstrate the approach and experimentally varied mechanical properties of the PU elastomer by modulating the mixing ratio between components of the elastomer. Twenty-five experimental conditions are selected based on the design of experiment and use those data points to train a linear regression model. The resulting model takes desired mechanical properties as input and returns synthetic recipes of a soft material, which is subsequently validated by experiments. Lastly, the prediction accuracies of different machine learning algorithms is compared. It is believed that the approach is widely applicable to other material systems to establish experimental conditions and material property relationships for soft materials.     

3D Printing of Small-Scale Soft Robots with Programmable Magnetization

Soft magnetic structures having a non-uniform magnetization profile can achieve multimodal locomotion that is helpful to operate in confined spaces. However, incorporating such magnetic anisotropy into their body is not straightforward. Existing methods are either limited in the anisotropic profiles they can achieve or too cumbersome and time-consuming to produce. Herein, a 3D printing method allowing to incorporate magnetic anisotropy directly into the printed soft structure is demonstrated. This offers at the same time a simple and time-efficient magnetic soft robot prototyping strategy. The proposed process involves orienting the magnetized particles in the magnetic ink used in the 3D printer by a custom electromagnetic coil system acting onto the particles while printing. The resulting structures are extensively characterized to confirm the validity of the process. The extent of orientation is determined to be between 92% and 99%. A few examples of remotely actuated small-scale soft robots that are printed through this method are also demonstrated. Just like 3D printing gives the freedom to print a large number of variations in shapes, the proposed method also gives the freedom to incorporate an extensive range of magnetic anisotropies.     

Tailored Mechanical Metamaterials with Programmable Quasi-Zero-Stiffness Features for Full-Band Vibration Isolation

Quasi-zero-stiffness (QZS) isolators of high-static-low-dynamic stiffness play an important role in ultra-low frequency vibration mitigation. While the current designs of QZS mainly exploit the combination of negative-stiffness corrector and positive-stiffness element, and only have a single QZS working range, here a class of tailored mechanical metamaterials with programmable QZS features is proposed. These programmed structures contain curved beams with geometries that are specifically designed to enable the prescribed QZS characteristics. When these metamaterials are compressed, the curved beams reach the prescribed QZS working range in sequence, thus enabling tailored stair-stepping force-displacement curves with multiple QZS working ranges. Compression tests demonstrate that a vast design space is achieved to program the QZS features of the metamaterials. Further vibration tests confirm the ultra-low frequency vibration isolation capability of the proposed mechanical metamaterials. The mechanism of QZS stems solely from the structural geometry of the curved beams and is therefore materials-independent. This design strategy opens a new avenue for innovating compact and scalable QZS isolators with multiple working ranges.     

3D Printed Fractal Metamaterials with Tunable Mechanical Properties and Shape Reconfiguration

Lattice metamaterials constructed by curved microstructures exhibit large stretchability and are promising in soft electronics and soft robotics. Fractal structures are particularly efficient in improving stretchability as it shows multiple-order uncurling. However, the development of fractal metamaterials is hindered by hierarchical structures and large deformations. In this study, a design framework combining experiments, hierarchical theoretical models, and finite element simulations is developed to program the mechanical behaviors of fractal metamaterials. For 3D printing, a digital design tool is developed to visualize the structure and automatically generate the manufacturing representations. Results show that large stretchability (≈360%), bionic stress–strain curve matching, and imperfection insensitivity can be programmed by tuning the geometric parameters. An integrated device of an electromyogram sensor embedded in an imperfection-insensitive fractal metamaterial that matches the J-shaped stress–strain curve of human skin is demonstrated. Light-emitting diode devices based on fractal metamaterial with shape reconfiguration are also presented. This st paves a new way to realize multifunctional soft devices using fractal metamaterials.     

Gradient Porous Elastic Hydrogels with Shape‐Memory Property and Anisotropic Responses for Programmable Locomotion

Programmable locomotion of responsive hydrogels has gained increasing attention for potential applications in soft robotics, microfluidic components, actuators, and artificial muscle. Modulation of hydrogel pore structures is essential for tailoring their mechanical strength, response speeds, and motion behaviors. Conventional methods forming hydrogels with homogeneous or stepwise‐distributed pore structures are limited by the required compromise to simultaneously optimize these aspects. Here, a heterobifunctional crosslinker enabled hydrothermal process is introduced to synthesize responsive hydrogels with well‐defined gradient pore construction. According to gradient porosity controls, the hydrogels simultaneously exhibit rapid responses to external stimuli, high elasticity/compressibility, and programmable locomotion capability. By incorporating polypyrrole nanoparticles as photothermal transducers, photo/thermal responsive composite hydrogels are formed to enable programmable control of locomotion such as bending, curving, twisting, and octopus‐like swimming under near‐infrared laser stimulation. The tunable pore structures, mechanical properties, and locomotion of this new class of materials make these gradient porous hydrogels potentially suitable for a variety of applications.