Controlled Mechanical Buckling for Origami‐Inspired Construction of 3D Microstructures in Advanced Materials

Origami is a topic of rapidly growing interest in both the scientific and engineering research communities due to its promising potential in a broad range of applications. Previous assembly approaches for origami structures at the micro/nanoscale are constrained by the applicable classes of materials, topologies, and/or capability for reversible control over the transformation process. Here, a strategy is introduced that exploits mechanical buckling for autonomic origami assembly of 3D structures across material classes from soft polymers to brittle inorganic semiconductors, and length scales from nanometers to centimeters. This approach relies on a spatial variation of thickness in the initial 2D structures as a means to produce engineered folding creases during the compressive buckling process. The elastic nature of the assembly scheme enables active, deterministic control over intermediate states in the 2D to 3D transformation in a continuous and reversible manner. Demonstrations include a broad set of 3D structures formed through unidirectional, bidirectional, and even hierarchical folding, with examples ranging from half cylindrical columns and fish scales, to cubic boxes, pyramids, starfish, paper fans, skew tooth structures, and to amusing system‐level examples of soccer balls, model houses, cars, and multifloor textured buildings.     

Experimental and Theoretical Studies of Serpentine Microstructures Bonded To Prestrained Elastomers for Stretchable Electronics

Stretchable electronic devices that exploit inorganic materials are attractive due to their combination of high performance with mechanical deformability, particularly for applications in biomedical devices that require intimate integration with human body. Several mechanics and materials schemes have been devised for this type of technology, many of which exploit deformable interconnects. When such interconnects are fully bonded to the substrate and/or encapsulated in a solid material, useful but modest levels of deformation (<30–40%) are possible, with reversible and repeatable mechanics. Here, the use of prestrain in the substrate is introduced, together with interconnects in narrow, serpentine shapes, to yield significantly enhanced (more than two times) stretchability, to more than 100%. Fracture and cyclic fatigue testing on structures formed with and without prestrain quantitatively demonstrate the possible enhancements. Finite element analyses (FEA) illustrates the effects of various material and geometric parameters. A drastic decrease in the elastic stretchability is observed with increasing metal thickness, due to changes in the buckling mode, that is, from local wrinkling at small thicknesses to absence of such wrinkling at large thicknesses, as revealed by experiment. An analytic model quantitatively predicts the wavelength of this wrinkling, and explains the thickness dependence of the buckling behaviors.     

A Fabrication Strategy for Reconfigurable Millimeter-Scale Metamaterials

Rather than depending on material composition to primarily dictate performance metrics, metamaterials can leverage geometry to achieve specific properties of interest. For example, reconfigurable metamaterials have enabled programmable shape transformations, tunable mechanical properties, and energy absorption. While several methods exist to fabricate such structures, they often place severe restrictions on manufacturing materials, or require significant manual assembly. Moreover, these arrays are typically composed of unit cells that are either macro-scale or micro-scale in dimension. Here, the fabrication gap is bridged, and laminate manufacturing is used to develop a method for designing reconfigurable metamaterials at the millimeter-scale, that is compatible with a wide range of materials, and that requires minimal manual assembly. In addition to showing the versatility of this fabrication method, how the use of laminate manufacturing affects the behavior of these multi-component arrays is also characterized. To this end, a numerical model that captures the deformations exhibited by the structures is developed, and an analytic model that predicts the strain of the structure under compressive stress is built. Overall, this approach can be leveraged to develop millimeter-scale metamaterials for applications that require reconfigurable materials, such as in the design of tunable acoustics, photonic waveguides, and electromagnetic devices.     

A Generic Soft Encapsulation Strategy for Stretchable Electronics

Recent progress in stretchable forms of inorganic electronic systems has established a route to new classes of devices, with particularly unique capabilities in functional biointerfaces, because of their mechanical and geometrical compatibility with human tissues and organs. A reliable approach to physically and chemically protect the electronic components and interconnects is indispensable for practical applications. Although recent reports describe various options in soft, solid encapsulation, the development of approaches that do not significantly reduce the stretchability remains an area of continued focus. Herein, a generic, soft encapsulation strategy is reported, which is applicable to a wide range of stretchable interconnect designs, including those based on two‐dimensional (2D) serpentine configurations, 2D fractal‐inspired patterns, and 3D helical configurations. This strategy forms the encapsulation while the system is in a prestrained state, in contrast to the traditional approach that involves the strain‐free configuration. A systematic comparison reveals that substantial enhancements (e.g., ≈6.0 times for 2D serpentine, ≈4.0 times for 2D fractal, and ≈2.6 times for 3D helical) in the stretchability can be achieved through use of the proposed strategy. Demonstrated applications in highly stretchable light‐emitting diodes systems that can be mounted onto complex curvilinear surfaces illustrate the general capabilities in functional device systems.     

Superelastic and Arbitrary‐Shaped Graphene Aerogels with Sacrificial Skeleton of Melamine Foam for Varied Applications

Elastic graphene aerogels are lightweight and offer excellent and electrical performance, expanding their significance in many applications. Recently, elastic graphene aerogels have been fabricated via various methods. However, for most reported elastic graphene aerogels, the fabrication processes are complicated and the applications are usually limited by the brittle mechanical properties. Thus, it still remains a challenge to explore facile processes for the fabrication of graphene aerogels with low density and high compressibility. Herein, arbitrary‐shaped, superelastic, and durable graphene aerogels are fabricated using melamine foam as sacrificial skeleton. The resulting graphene aerogels possess high elasticity under compressive stress of 0.556 MPa and compressive strain of 95%. Thanks to the superelasticity, high strength, excellent flexibility, outstanding thermal stability, and good electrical conductivity of graphene aerogels, they can be applied in sorbents and pressure/strain sensors. The as‐assembled graphene aerogels can adsorb various organic solvents at 176–513 g g^?1 depending on the solvent type and density. Moreover, both the squeezing and combustion methods can be adopted for reusing the graphene aerogels. Finally, the graphene aerogels exhibit stable and sensitive current responses, making them the ideal candidates for applications as multifunctional pressure/strain sensors such as wearable devices.     

Carbon Nanotube Fiber Based Stretchable Conductor

Carbon nanotube (CNT) based continuous fiber, a CNT assembly that could potentially retain the superb properties of individual CNTs on a macroscopic scale, belongs to a fascinating new class of electronic materials with potential applications in electronics, sensing, and conducting wires. Here, the fabrication of CNT fiber based stretchable conductors by a simple prestraining‐then‐buckling approach is reported. To enhance the interfacial bonding between the fibers and the poly(dimethylsiloxane) (PDMS) substrate and thus facilitate the buckling formation, CNT fibers are first coated with a thin layer of liquid PDMS before being transferred to the prestrained substrate. The CNT fibers are deformed into massive buckles, resulting from the compressive force generated upon releasing the fiber/substrate assembly from prestrain. This buckling shape is quite different from the sinusoidal shape observed previously in otherwise analogous systems. Similar experiments performed on carbon fiber/PDMS composite film, on the other hand, result in extensive fiber fracture due to the higher fiber flexural modulus. Furthermore, the CNT fiber/PDMS composite film shows very little variation in resistance (≈1%) under multiple stretching‐and‐releasing cycles up to a prestrain level of 40%, indicating the outstanding stability and repeatability in performance as stretchable conductors.     

Controlled Fabrication of 3D Chiral Microwrinkles via Asymmetrical and Biaxial Bucklings

Nano‐ and microsized chiral materials are receiving significant attention because of their unique characteristics, which include chiroptical activities and enantioselective interactions with living materials. However, the realization of chiral morphologies in such small‐scale materials has been an issue because of the complicated fabrication methods and limited material selection. In this study, a facile and reproducible method is developed for fabricating 3D chiral microwrinkles with twisted shapes by asymmetric and biaxial buckling. Soft polydimethylsiloxane (PDMS) substrates are asymmetrically stretched with angled biaxial strains and exposed to UV/ozone to prepare hard silica layers on top of the PDMS substrates to induce microwrinkles. The chiral shapes are controlled by changing the angle (θ) between the two strain axes and the UV/ozone exposure times (t₁, t₂) in each stage of buckling. The 3D chiral microwrinkles are shaped like “fusilli pasta” and occupy an area of 1.5 cm × 1.5 cm. The patterned area can be easily scaled, and no innate chiral biomaterial is necessary. This method could be widely extended to the fabrication of diverse types of chiral materials for advanced optical and bio‐applications.     

2D Nanomaterial Arrays for Electronics and Optoelectronics

Two‐dimensional (2D) materials, benefitting from their unique planar structure and various appealing electronic properties, have attracted much attention for novel electronic and optoelectronic applications. As a basis for practical devices, the study of micro/nano‐2D material arrays based on coupling effects and synergistic effects is critical to the functionalization and integration of 2D materials. Moreover, micro/nano‐2D material arrays are compatible with traditional complementary metal oxide semiconductor (CMOS) electronics, catering well to high‐integration, high‐sensitivity, and low‐cost sensing and imaging systems. This review presents some recent studies on 2D material arrays in sequence from their novel preparations to high‐integration applications as well as explorations on dimension tuning. A first focus is on various typical fabrication methods for 2D material arrays, including photolithography, 2D printing, seeded growth, van der Waals epitaxial growth, and self‐assembly. Then, the applications of 2D material arrays, such as field effect transistors, photodetectors, pressure sensors, as well as flexible electronic devices of photodetectors and strain sensors, are elaborately introduced. Furthermore, the recent burgeoning exploration of mixed‐dimensional heterostructure arrays including 0D/2D, 1D/2D, and 3D/2D is discussed. Ultimately, conclusions and an outlook based on the current developments in this promising field are presented.     

Lateral Buckling of High Aspect Ratio Janus Nanowalls

In recent years, the fabrication of Janus materials and their potential applications has been of much interest in Materials Science. Here, we report the fabrication of an entirely novel structure–Janus nanowalls and the phenomenon of lateral buckling in them. Polymeric nanowalls were prepared with the replica molding technique and metal films, of comparable thicknesses, were then deposited on one side of the polymer nanowalls by vacuum process. During the metal deposition, the nanowalls themselves buckle laterally; this buckling is induced by the compressive residual stress in the metal film and geometric confining constraints. The feature of wrinkle patterns resulting from the lateral buckling was theoretically investigated using the scaling analysis. Theoretical results are in good agreement with the experimental observations.     

Buckling Instability Control of 1D Nanowire Networks for a Large‐Area Stretchable and Transparent Electrode

A commonly used strategy to impose deformability on conductive materials is the prestrain method, in which conductive materials are placed on prestretched elastic substrates and relaxed to create wavy or wrinkled structures. However, 1D metallic nanowire (NW) networks typically result in out‐of‐plane buckling defects and NW fractures, due to their rigid and brittle nature and nonuniform load transfer to specific points of NW. To resolve these problems, an alternative method is proposed to control the elastic modulus of 1D NW networks through contact with various solvents during compressive strain. Through solvent contact, the interface interactions between the NWs and between the NW and substrate can be controlled, and it is shown that the surface instability of the 1D random network is formed differently from a uniform bilayer film, which also can vary with the modulus of the network. For modulus values lower than the critical point, slippage and rearrangement of NW strands mainly occur and individual strands in the network show an in‐plane wavy configuration, which is ideal for structural stretchability. Based on the solvent‐assisted prestrain method, letter‐sized, large‐area stretchable, and transparent electrodes with high transparency and conductivity are achieved, and stretchable and transparent alternating current electroluminescent devices for stretchable display applications are also realized.     

Interfacial Sliding and Buckling of Monolayer Graphene on a Stretchable Substrate

The nonlinear mechanical response of monolayer graphene on polyethylene terephthalate (PET) is characterised using in‐situ Raman spectroscopy and atomic force microscopy. While interfacial stress transfer leads to tension in graphene as the PET substrate is stretched, retraction of the substrate during unloading imposes compression in the graphene. Two interfacial failure mechanisms, shear sliding under tension and buckling under compression, are identified. Using a nonlinear shear‐lag model, the interfacial shear strength is found to range between 0.46 and 0.69 MPa. The critical strain for onset of interfacial sliding is ～0.3%, while the maximum strain that can be transferred to graphene ranges from 1.2% to 1.6% depending on the interfacial shear strength and graphene size. Beyond a critical compressive strain of around ?0.7%, buckling ridges are observed after unloading. The results from this work provide valuable insight and design guidelines for a broad spectrum of applications of graphene and other 2D nanomaterials, such as flexible and stretchable electronics, strain sensing, and nanocomposites.     

Mechanical design failure models for buckling

This tutorial illustrates design situations where elastic buckling of slender columns and thin plates under compressive loads can result in large deformations, and eventual failure, of the structure. This is a classical example of an overstress failure mechanism, and analytic methods, based on continuum mechanics principles, are presented to design against such failures. Examples illustrate the use of these models in practical design situations in mechanical engineering and electronic packaging applications     

Engineered Elastomer Substrates for Guided Assembly of Complex 3D Mesostructures by Spatially Nonuniform Compressive Buckling

Approaches capable of creating 3D mesostructures in advanced materials (device‐grade semiconductors, electroactive polymers, etc.) are of increasing interest in modern materials research. A versatile set of approaches exploits transformation of planar precursors into 3D architectures through the action of compressive forces associated with release of prestrain in a supporting elastomer substrate. Although a diverse set of 3D structures can be realized in nearly any class of material in this way, all previously reported demonstrations lack the ability to vary the degree of compression imparted to different regions of the 2D precursor, thus constraining the diversity of 3D geometries. This paper presents a set of ideas in materials and mechanics in which elastomeric substrates with engineered distributions of thickness yield desired strain distributions for targeted control over resultant 3D mesostructures geometries. This approach is compatible with a broad range of advanced functional materials from device‐grade semiconductors to commercially available thin films, over length scales from tens of micrometers to several millimeters. A wide range of 3D structures can be produced in this way, some of which have direct relevance to applications in tunable optics and stretchable electronics.     

Lowering Internal Friction of 0D–1D–2D Ternary Nanocomposite‐Based Strain Sensor by Fullerene to Boost the Sensing Performance

The development of strain sensors with both large strain range (>50%) and high gauge factor (>100) is a grand challenge. High sensitivity requires material to perform considerable structural deformation under tiny strain, whereas high stretchability demands structural connection or morphological integrity for materials upon large deformation, yet both features are hard to be achieved in one thin film. A new 0D–1D–2D ternary nanocomposite–based strain sensor is developed that possesses high sensitivity in broad working strain range (gauge factor 2392.9 at 62%), low hysteresis, good linearity, and long‐term durability. The skin‐mountable strain sensor, fabricated through one‐step screen‐printing process, is made of 1D silver nanowire offering high electrical conductivity, 2D graphene oxide offering brittle layered structure, and 0D fullerene offering lubricity. The fullerene constitutes a critical component that lowers the friction between graphene oxide–based layers and facilitates the sliding between adjacent layers without hurting the brittle nature of the nanocomposite film. When stretching, layer slippage induced by fullerene can accommodate partial applied stress and boost the strain, while cracks originating and propagating in the brittle nanocomposite film ensure large resistance change over the whole working strain range. Such high comprehensive performance renders the strain sensor applicable to full‐spectrum human motion detection.     

Multiscale Colloidal Assembly of Silica Nanoparticles into Microspheres with Tunable Mesopores

Colloidal assembly of silica (nano)particles is a powerful method to design functional materials across multiple length scales. Although this method has enabled the fabrication of a wide range of silica‐based materials, attempts to design and synthesize porous materials with a high level of tuneability and control over pore dimensions have remained relatively unsuccessful. Here, the colloidal assembly of silica nanoparticles into mesoporous silica microspheres (MSMs) is reported using a discrete set of silica sols within the confinement of a water‐in‐oil emulsion system. By studying the independent manipulation of different assembly parameters during the sol–gel process, a design strategy is outlined to synthesize MSMs with excellent reproducibility and independent control over pore size and overall porosity, which does not require additional ageing or post‐treatment steps to reach pore sizes as large as 50 nm. The strategy presented here can provide the necessary tools for the microstructural design of the next generation of tailor‐made silica microspheres for use in separation applications and beyond.     

Nanoparticle-Based Strain Gauges: Anisotropic Response Characteristics,Multidirectional Strain Sensing,and Novel Approaches to Healthcare Applications

Directional strain sensing is essential for advanced sensor applications in the field of human-machine interfaces and healthcare. Here, the angle dependent anisotropic strain sensitivity caused by charge carriers percolating through cross-linked gold nanoparticle (GNP) networks is studied and these versatile materials are used for the fabrication of wearable triaxial pulse and gesture sensors. More specifically, the anisotropic response of 1,9-nonanedithiol cross-linked GNP films is separated into geometric and piezoresistive contributions by fitting the measured data with an analytic model. Hereby, piezoresistive coefficients of g₁₁ ∼ 32 and g₁₂ ∼ 21 are extracted, indicating a slightly anisotropic response behavior of the GNP-based material. To use the material for healthcare applications, arrangements of three GNP transducers are patterned lithographically and fully embedded into a highly flexible silicone polymer (Dragon Skin 30). The new encapsulation method ensures good and robust electrical contacts and enables facile handling and protection from external influences. A facile read-out with wireless data transmission using off-the-shelf electrical components underlines the great potential of these devices for applications as skin-wearable healthcare sensors.     

Direct Freeform Laser Fabrication of 3D Conformable Electronics

3D conformable electronic devices on freeform surfaces show superior performance to the conventional, planar ones. They represent a trend of future electronics and have witnessed exponential growth in various applications. However, their potential is largely limited by a lack of sophisticated fabrication techniques. To tackle this challenge, a new direct freeform laser (DFL) fabrication method enabled by a 5-axis laser processing platform for directly fabricating 3D conformable electronics on targeted arbitrary surfaces is reported. Accordingly, representative laser-induced graphene (LIG), metals, and metal oxides are successfully fabricated as high-performance sensing and electrode materials from different material precursors on various types of substrates for applications in temperature/light/gas sensing, energy storage, and printed circuit board for circuit. Last but not the least, to demonstrate an application in smart homes, LIG-based conformable strain sensors are fabricated and distributed in designated locations of an artificial tree. The distributed sensors have the capability of monitoring the wind speed and direction with the assistance of well-trained machine-learning models. This novel process will pave a new and general route to fabricating 3D conformable electronic devices, thus creating new opportunities in robotics, biomedical sensing, structural health, environmental monitoring, and Internet of Things applications.     

Detection of buckling in steel pipeline and column by the distributed Brillouin sensor

We conducted a strain characterization experiment to monitor steel pipe and column buckling for the first time using a distributed Brillouin sensor system. Two specimens (steel pipe and column) were prepared by locally thinning the inner wall to initiate buckling. An axial load was applied to the specimens and increased while compressive strain was measured by both Brillouin sensor and strain gauges. With the Brillouin sensor, we observed compression on the whole specimens while elongation was detected in the neighborhood of the thinned wall at onset of the buckling. Both tension and compression are measured simultaneously from the same spectrum. This capability to extract both informations at the same time makes the Brillouin sensor a unique tool for structural health monitoring. The buckling was identified and localized thanks to this original approach.     

Rapid Fabrication of Soft,Multilayered Electronics for Wearable Biomonitoring

Soft integrated electronics are key components for emerging applications in wearable biomonitoring, soft co‐robotics, and physical human–machine interaction. They are composed of soft and elastically deformable circuits and sensors that are combined with packaged microelectronics for signal processing, power regulation, and communication. While promising, widespread use of soft wearable electronics is currently limited by the lack of robust fabrication techniques to rapidly, efficiently, and precisely assemble soft and rigid components into multilayered systems. Here, an efficient digital fabrication approach is presented to create highly customizable wearable electronics through rapid laser machining and adhesion controlled soft materials assembly. Well aligned, multilayered materials are created from 2D and 3D elements that stretch and bend while seamlessly integrating with rigid components such as microchip integrated circuits, discrete electrical components, and interconnects. These techniques are applied using commercially available materials and components and the fabrication of thin, lightweight, customized sensor skins is demonstrated in under an hour. These fully integrated wireless devices conformably bond to the hand and are successfully used for monitoring hand gesture, pulse rate, and blood oxygenation. These materials and methods enable custom wearable electronics while offering versatility in design and functionality for a variety of applications through material selection and construction.