Data-driven inverse design of flexible pressure sensors.

Artificial skins or flexible pressure sensors that mimic human cutaneous mechanoreceptors transduce tactile stimuli to quantitative electrical signals. Conventional trial-and-error designs for such devices follow a forward structure-to-property routine, which is usually time-consuming and determines one possible solution in one run. Data-driven inverse design can precisely target desired functions while showing far higher productivity, however, it is still absent for flexible pressure sensors because of the difficulties in acquiring a large amount of data. Here, we report a property-to-structure inverse design of flexible pressure sensors, exhibiting a significantly greater efficiency than the conventional routine. We use a reduced-order model that analytically constrains the design scope and an iterative "jumping-selection" method together with a surrogate model that enhances data screening. As an exemplary scenario, hundreds of solutions that overcome the intrinsic signal saturation have been predicted by the inverse method, validating for a variety of material systems. The success in property design on multiple indicators demonstrates that the proposed inverse design is an efficient and powerful tool to target multifarious applications of flexible pressure sensors, which can potentially advance the fields of intelligent robots, advanced healthcare, and human-machine interfaces.

Matte surfaces with broadband transparency enabled by highly asymmetric diffusion of white light.

The long-standing paradox between matte appearance and transparency has deprived traditional matte materials of optical transparency. Here, we present a solution to this centuries-old optical conundrum by harnessing the potential of disordered optical metasurfaces. Through the construction of a random array of meta-atoms tailored in asymmetric backgrounds, we have created transparent matte surfaces that maintain clear transparency regardless of the strength of disordered light scattering or their matte appearances. This remarkable property originates in the achievement of highly asymmetric light diffusion, exhibiting substantial diffusion in reflection and negligible diffusion in transmission across the entire visible spectrum. By fabricating macroscopic samples of such metasurfaces through industrial lithography, we have experimentally demonstrated transparent windows camouflaged as traditional matte materials, as well as transparent displays with high clarity, full color, and one-way visibility. Our work introduces an unprecedented frontier of transparent matte materials in optics, offering unprecedented opportunities and applications.

Self-regulated underwater phototaxis of a photoresponsive hydrogel-based phototactic vehicle.

Incorporating a negative feedback loop in a synthetic material to enable complex self-regulative behaviours akin to living organisms remains a design challenge. Here we show that a hydrogel-based vehicle can follow the directions of photonic illumination with directional regulation inside a constraint-free, fluidic space. By manipulating the customized photothermal nanoparticles and the microscale pores in the polymeric matrix, we achieved strong chemomechanical deformation of the soft material. The vehicle swiftly assumes an optimal pose and creates directional flow around itself, which it follows to achieve robust full-space phototaxis. In addition, this phototaxis enables a series of complex underwater locomotions. We demonstrate that this versatility is generated by the synergy of photothermofluidic interactions resulting in closed-loop self-control and fast reconfigurability. The untethered, electronics-free, ambient-powered hydrogel vehicle manoeuvres through obstacles agilely, following illumination cues of moderate intensities, similar to that of natural sunlight.

Artificial axons as a biomimetic 3D myelination platform for the discovery and validation of promyelinating compounds.

Multiple sclerosis (MS), a chronic neurodegenerative disease driven by damage to the protective myelin sheath, is currently incurable. Today, all clinically available treatments modulate the immune-mediated symptoms of the disease but they fail to stop neurodegeneration in many patients. Remyelination, the regenerative process of myelin repair by oligodendrocytes, which is considered a necessary step to protect demyelinated axons and stop neuronal death, is impaired in MS patients. One of the major obstacles to finding effective remyelinating drugs is the lack of biomimetic drug screening platforms that enable quantification of compounds' potential to stimulate 3D myelination in the physiologically relevant axon-like environment. To address this need, we built a unique myelination drug discovery platform, by expanding our previously developed technology, artificial axons (AAs), which enables 3D-printing of synthetic axon mimics with the geometry and mechanical properties closely resembling those of biological axons. This platform allows for high-throughput phenotypic myelination assay based on quantification of 3D wrapping of myelin membrane around axons in response to compounds. Here, we demonstrate quantification of 3D myelin wrapping by rat oligodendrocytes around the axon mimics in response to a small library of known pro-myelinating compounds. This assay shows pro-myelinating activity for all tested compounds consistent with the published in vitro and in vivo data, demonstrating predictive power of AA platform. We find that stimulation of myelin wrapping by these compounds is dose-dependent, providing a facile means to quantify the compounds' potency and efficacy in promoting myelin wrapping. Further, the ranking of relative efficacy among these compounds differs in this 3D axon-like environment as compared to a traditional oligodendrocyte 2D differentiation assay quantifying area of deposited myelin membrane. Together, we demonstrate that the artificial axons platform and associated phenotypic myelin wrapping assay afford direct evaluation of myelin wrapping by oligodendrocytes in response to soluble compounds in an axon-like environment, providing a predictive tool for the discovery of remyelinating therapies.

Achieving Fast Oxygen Reduction on Oxide Electrodes by Creating 3D Multiscale Micro-Nano Structures for Low-Temperature Solid Oxide Fuel Cells.

Fast oxygen reduction reaction (ORR) at the cathode is a key requirement for the realization of low-temperature solid oxide fuel cells (SOFCs). While the design of three-dimensional (3D) structures has emerged as a new and promising approach to improving the electrochemical performance of SOFC cathodes, achieving versatile structures and structural stability is still challenging. In this study, we demonstrate a novel architectural design for a superior cathode with fast ORR activity. By employing a completely new fabrication process comprising a 3D printing technique and pulsed laser deposition (PLD), we design 3D La0.8Sr0.2CoO3-δ (LSC) micro-nano structures with the desired shape. 3D-printed yttria-stabilized ZrO2 (YSZ) microstructures significantly increase the ratio of surface area to volume while maintaining suitable ionic conductivity comparable to that of single-crystalline YSZ substrates. Scanning electron microscopy and energy dispersive X-ray microanalysis reveal the formation of crack- or void-free YSZ microstructures and the uniform deposition of LSC films by PLD on the YSZ microstructures. The 3D LSC micro-nano structures show significantly enhanced oxygen surface exchange coefficients (kchem) extracted from electrical conductivity relaxation (ECR) measurements by up to 3 orders of magnitude relative to the bulk LSC. Furthermore, electrochemical impedance spectroscopy measurements verify the kchem values from ECR and no directional difference in the measured ORR activity depending on the shape of 3D microstructures. The dramatic enhancement of the ORR activity of LSC is attributed to the increased film surface areas resulting from the 3D YSZ microstructures.

3D Printing of Interpenetrating Network Flexible Hydrogels with Enhancement of Adhesiveness.

3D printing of hydrogels has been widely explored for the rapid fabrication of complex soft structures and devices. However, using 3D printing to customize hydrogels with both adequate adhesiveness and toughness remains a fundamental challenge. Here, we demonstrate mussel-inspired (polydopamine) PDA hydrogel through the incorporation of a classical double network (2-acrylamido-2-methylpropanesulfonic acid) PAMPS/(polyacrylamide) PAAm to achieve simultaneously tailored adhesiveness, toughness, and biocompatibility and validate the 3D printability of such a hydrogel into customized architectures. The strategy of combining PDA with PAMPS/PAAm hydrogels leads to favorable adhesion on either hydrophilic or hydrophobic surfaces. The hydrogel also shows excellent flexibility, which is attributed to the reversible cross-linking of PDA and PAMPS, together with the long-chain PAAm cross-linking network. Among them, the reversible cross-linking of PDA and PAMPS is capable of dissipating mechanical energy under deformation. Meanwhile, the long-chain PAAm network contributes to maintaining a high deformation capability. We establish a theoretical framework to quantify the contribution of the interpenetrating networks to the overall toughness of the hydrogel, which also provides guidance for the rational design of materials with the desired properties. Our work manifests a new paradigm of printing adhesive, tough, and biocompatible interpenetrating network hydrogels to meet the requirements of broad potential applications in biomedical engineering, soft robotics, and intelligent and superabsorbent devices.

Underwater acoustic metamaterials.

Acoustic metamaterials have been widely investigated over the past few decades and have realized acoustic parameters that are not achievable using conventional materials. After demonstrating that locally resonant acoustic metamaterials are capable of acting as subwavelength unit cells, researchers have evaluated the possibility of breaking the classical limitations of the material mass density and bulk modulus. Combined with theoretical analysis, additive manufacturing and engineering applications, acoustic metamaterials have demonstrated extraordinary capabilities, including negative refraction, cloaking, beam formation and super-resolution imaging. Owing to the complexity of impedance boundaries and mode transitions, there are still challenges in freely manipulating acoustic propagation in an underwater environment. This review summarizes the developments in underwater acoustic metamaterials over the past 20 years, which include underwater acoustic invisibility cloaking, underwater beam formation, underwater metasurfaces and phase engineering, underwater topological acoustics and underwater acoustic metamaterial absorbers. With the evolution of underwater metamaterials and the timeline of scientific advances, underwater acoustic metamaterials have demonstrated exciting applications in underwater resource development, target recognition, imaging, noise reduction, navigation and communication.

Quasi-seamless stitching for large-area micropatterned surfaces enabled by Fourier spectral analysis of moiré patterns.

The main challenge in preparing a flexible mold stamp using roll-to-roll nanoimprint lithography is to simultaneously increase the imprintable area with a minimized perceptible seam. However, the current methods for stitching multiple small molds to fabricate large-area molds and functional surfaces typically rely on the alignment mark, which inevitably produces a clear alignment mark and stitched seam. In this study, we propose a mark-less alignment by the pattern itself method inspired by moiré technique, which uses the Fourier spectral analysis of moiré patterns formed by superposed identical patterns for alignment. This method is capable of fabricating scalable functional surfaces and imprint molds with quasi-seamless and alignment mark-free patterning. By harnessing the rotational invariance property in the Fourier transform, our approach is confirmed to be a simple and efficient method for extracting the rotational and translational offsets in overlapped periodic or nonperiodic patterns with a minimized stitched region, thereby allowing for the large-area and quasi-seamless fabrication of imprinting molds and functional surfaces, such as liquid-repellent film and micro-optical sheets, that surpass the conventional alignment and stitching limits and potentially expand their application in producing large-area metasurfaces.

In Situ Wide-Field Visualization of Palladium Hydrogenation.

Visualizing hydrogenation processes in palladium (Pd) in real-time is important to various hydrogen-involved applications. However, observing hydrogen diffusion of Pd was limited by its small permittivity variation, and the kinetics of lateral diffusion of hydrogen in Pd film was not reported. Here, we proposed an optical microscopy-based visualization of Pd hydrogenation from the diffusion surface to the interior by introducing a fast-response mechanical platform that transforms the hydrogen diffusion into self-organized ordered wrinkles with sharp optical contrast. This platform is a Au/Pd double layer on an elastomer, which results in directional hydrogenation from the sidewall to the interior. The kinetics of hydrogenation in the interior of the palladium along the diffusion direction was monitored in real-time. This platform will enable in situ visualization of atom/ion diffusion on metals that are crucial in energy storage and hydrogen detection.

Biomimetic on-chip filtration enabled by direct micro-3D printing on membrane.

Membrane-on-chip is of growing interest in a wide variety of high-throughput environmental and water research. Advances in membrane technology continuously provide novel materials and multi-functional structures. Yet, the incorporation of membrane into microfluidic devices remains challenging, thus limiting its versatile utilization. Herein, via micro-stereolithography 3D printing, we propose and fabricate a "fish gill" structure-integrated on-chip membrane device, which has the self-sealing attribute at structure-membrane interface without extra assembling. As a demonstration, metallic micromesh and polymeric membrane can also be easily embedded in 3D printed on-chip device to achieve anti-fouling and anti-clogging functionality for wastewater filtration. As evidenced from in-situ visualization of structure-fluid-foulant interactions during filtration process, the proposed approach successfully adopts the fish feeding mechanism, being able to "ricochet" foulant particles or droplets through hydrodynamic manipulation. When benchmarked with two common wastewater treatment scenarios, such as plastic micro-particles and emulsified oil droplets, our biomimetic filtration devices exhibit 2 ~ 3 times longer durability for high-flux filtration than devices with commercial membrane. This proposed 3D printing-on-membrane approach, elegantly bridging the fields of microfluidics and membrane science, is instrumental to many other applications in energy, sensing, analytical chemistry and biomedical engineering.

3D direct printing of mechanical and biocompatible hydrogel meta-structures.

Direct Ink Writing (DIW) has demonstrated great potential as a versatile method to 3D print multifunctional structures. In this work, we report the implementation of hydrogel meta-structures using DIW at room temperature, which seamlessly integrate large specific surface areas, interconnected porous characteristics, mechanical toughness, biocompatibility, and water absorption and retention capabilities. Robust but hydrophobic polymers and weakly crosslinked nature-origin hydrogels form a balance in the self-supporting ink, allowing us to directly print complex meta-structures without sacrificial materials and heating extrusion. Mechanically, the mixed bending or stretching of symmetrical re-entrant cellular lattices and the unique curvature patterns are combined to provide little lateral expansion and large compressive energy absorbance when external forces are applied on the printed meta-structures. In addition, we have successfully demonstrated ear, aortic valve conduits and hierarchical architectures. We anticipate that the reported 3D meta-structured hydrogel would offer a new strategy to develop functional biomaterials for tissue engineering applications in the future.

Muscle-fiber array inspired, multiple-mode, pneumatic artificial muscles through planar design and one-step rolling fabrication.

Advances in development of artificial muscles have enabled creation of soft robots with biological dexterity and self-adaption in unstructured environments; however, production of scalable artificial muscles with multiple-mode actuations remains elusive. Inspired by muscle-fiber arrays in muscular hydrostats, we present a class of versatile artificial muscles called MAIPAMs (muscle-fiber array inspired pneumatic artificial muscles), capable of multiple-mode actuations (such as parallel elongation-bending-spiraling actuations, 10 parallel bending actuations and cascaded elongation-bending-spiraling actuations). Our MAIPAMs consist of active 3D elastomer-balloon arrays reinforced by a passive elastomer membrane, achieved through a planar design and one-step rolling fabrication approach. We introduce prototypical designs for the MAIPAMs and demonstrate their muscle-mimic structures and versatility, as well as their scalable ability to integrate flexible but non-stretchable layers for contraction and twisting actuation modes and compliant electrodes for self-sensing. We further demonstrate that this class of artificial muscles shows potential for versatile robotic applications, such as carrying a camera for recording videos, gripping or manipulating objects, and climbing a pipe-line.

Scalable visible light 3D printing and bioprinting using an organic light-emitting diode microdisplay.

To address current unmet needs in terms of scalability and material biocompatibility for future photocrosslinking-based additive manufacturing technologies, emergent platform designs are in inexorable demand. In particular, a shift from the present use of cell-damaging UV light sources in light-based three-dimensional (3D) bioprinting methods demands new platforms. We adopted an organic light-emitting diode (OLED) microdisplay as a digital visible light modulator to create a 3D printing platform modality that offers scalability and multi-material capability while forgoing the need for UV photocrosslinking. We formulate biocompatible inks that are visible light-crosslinkable with relatively quick photoinitiation rates. We demonstrated successful attachment and rapid growth of primary human dermal fibroblast-adult (HDF-a) cells on biological substrates fabricated using the OLED platform. This platform incites new possibilities by providing a simple-yet-effective means for low-cost, high-throughput, and multi-material 3D fabrication of functional structures made of polymers, ceramic composites, and biomaterials.

Scalable 3D printing of aperiodic cellular structures by rotational stacking of integral image formation.

The limitation of projection microstereolithography in additive manufacturing methods is that they typically use a single-aperture imaging configuration, which restricts their ability to produce microstructures in large volumes owing to the trade-off between image resolution and image field area. Here, we propose an integral lithography based on integral image reconstruction coupled with a planar lens array. The individual microlenses maintain a high numerical aperture and are used to create digital light patterns that can expand the printable area by the number of microlenses (103 to 104), thereby allowing for the scalable stereolithographic fabrication of 3D features that surpass the resolution-to-area scaling limit. We extend the capability of integral lithography for programmable printing of deterministic nonperiodic structures through the rotational overlapping or stacking of multiple exposures with controlled angular offsets. This printing platform provides new possibilities for producing periodic and aperiodic microarchitectures spanning four orders of magnitude from micrometers to centimeters.

Three-Dimensional Soundproof Acoustic Metacage.

In this Letter, we theoretically propose and experimentally demonstrate a three-dimensional soundproof acoustic cage structure, hereby denoted as an acoustic metacage. The metacage is composed of six acoustic metamaterial slabs with open holes and hidden bypass space coiling tunnels connected to the holes. Band structure analysis reveals a novel physical mechanism to open a low-frequency broad partial band gap via the band folding in other directions, which can also be interpreted by an effective medium with indefinite effective mass density and negative effective modulus. Transmission loss in simulations and in the acoustic impedance tube are administered. Strikingly, we prove that the soundproofing effect of the metacage is robust against the airflow perturbation induced by a fan. Our work paves a road for low-frequency airborne soundproof structures in the presence of ventilation.

High resolution stereolithography fabrication of perfusable scaffolds to enable long-term meso-scale hepatic culture for disease modeling.

Microphysiological systems (MPS), comprising human cell cultured in formats that capture features of the three-dimensional (3D) microenvironments of native human organs under microperfusion, are promising tools for biomedical research. Here we report the development of a mesoscale physiological system (MePS) enabling the long-term 3D perfused culture of primary human hepatocytes at scales of over 106cells per MPS. A central feature of the MePS, which employs a commercially-available multiwell bioreactor for perfusion, is a novel scaffold comprising a dense network of nano- and micro-porous polymer channels, designed to provide appropriate convective and diffusive mass transfer of oxygen and other nutrients while maintaining physiological values of shear stress. The scaffold design is realized by a high resolution stereolithography fabrication process employing a novel resin. This new culture system sustains mesoscopic hepatic tissue-like cultures with greater hepatic functionality (assessed by albumin and urea synthesis, and CYP3A4 activity) and lower inflammation markers compared to comparable cultures on the commercial polystyrene scaffold. To illustrate applications to disease modeling, we established an insulin-resistant phenotype by exposing liver cells to hyperglycemic and hyperinsulinemic media. Future applications of the MePS include the co-culture of hepatocytes with resident immune cells and the integration with multiple organs to model complex liver-associated diseases.

Skin-electrode iontronic interface for mechanosensing.

Electrodermal devices that capture the physiological response of skin are crucial for monitoring vital signals, but they often require convoluted layered designs with either electronic or ionic active materials relying on complicated synthesis procedures, encapsulation, and packaging techniques. Here, we report that the ionic transport in living systems can provide a simple mode of iontronic sensing and bypass the need of artificial ionic materials. A simple skin-electrode mechanosensing structure (SEMS) is constructed, exhibiting high pressure-resolution and spatial-resolution, being capable of feeling touch and detecting weak physiological signals such as fingertip pulse under different skin humidity. Our mechanical analysis reveals the critical role of instability in high-aspect-ratio microstructures on sensing. We further demonstrate pressure mapping with millimeter-spatial-resolution using a fully textile SEMS-based glove. The simplicity and reliability of SEMS hold great promise of diverse healthcare applications, such as pulse detection and recovering the sensory capability in patients with tactile dysfunction.

Microstructured Surfaces for Reducing Chances of Fomite Transmission via Virus-Containing Respiratory Droplets.

Evaporation-induced particle aggregation in drying droplets is of significant importance in the prevention of pathogen transfer due to the possibility of indirect fomite transmission of the infectious virus particles. In this study, particle aggregation was directionally controlled using contact line dynamics (pinned or slipping) and geometrical gradients on microstructured surfaces by the systematic investigation of the evaporation process on sessile droplets and sprayed microdroplets laden with virus-simulant nanoparticles. Using this mechanism, we designed robust particle capture surfaces by significantly inhibiting the contact transfer of particles from fomite surfaces. For the proof-of-concept, interconnected hexagonal and inverted pyramidal microwall were fabricated using ultraviolet-based nanoimprint lithography, which is considered to be a promising scalable manufacturing process. We demonstrated the potentials of an engineered microcavity surface to limit the contact transfer of particle aggregates deposited with the evaporation of microdroplets by 93% for hexagonal microwall and by 96% for inverted pyramidal microwall. The particle capture potential of the interconnected microstructures was also investigated using biological particles, including adenoviruses and lung-derived extracellular vesicles. The findings indicate that the proposed microstructured surfaces can reduce the indirect fomite transmission of highly infectious agents, including norovirus, rotavirus, or SARS-CoV-2, via respiratory droplets.

Shape-Deformed Mushroom-like Reentrant Structures for Robust Liquid-Repellent Surfaces.

Artificial liquid-repellent surfaces inspired by biomimetic structures provide a wide range of functional surfaces for various practical applications, such as self-cleaning, antisticking, oil/water separation, and droplet manipulation. However, functional biomimetic structures cannot be fabricated using conventional techniques. For example, mushroom-like topologies on the skin of springtails, which are referred to as "doubly reentrant structures," have attracted significant attention owing to their extraordinary liquid-repellent properties. Current methods of fabricating these reentrant structures have several limitations, such as complex material systems, processing steps, and additional chemical treatments. This study proposed a simple micro-shape-deformed approach to fabricate mushroom-like reentrant structures by digital light processing, a three-dimensional (3D) printing technique, with volumetric shrinkage. The nonuniform cross-linking process and light propagation during photopolymerization caused the deformation of the topological patterns atop the micropillar arrays, resulting in bent structures for mushroom-like shape-deformed microarchitectures. This 3D-printed shape-deformed microstructure exhibits a highly stable liquid repellency without perfluorinated coatings.

Characterization of an underwater metamaterial made of aluminum honeycomb panels at low frequencies.

This paper presents a method to characterize the effective properties of inertial acoustic metamaterial unit cells for underwater operation. The method is manifested by a fast and reliable parameter retrieval procedure utilizing both numerical simulations and measurements. The effectiveness of the method was proved to be self-consistent by a metamaterial unit cell composed of aluminum honeycomb panels with soft rubber spacers. Simulated results agree well with the measured responses of this metamaterial in a water-filled resonator tube. A sub-unity density ratio and an anisotropic mass density are simultaneously achieved by the metamaterial unit cell, making it useful in implementations of transformation acoustics. The metamaterial, together with the approach for its characterization, are expected to be useful for underwater acoustic devices.