Laser-driven noncontact bubble transfer printing via a hydrogel composite stamp.

Transfer printing that enables heterogeneous integration of materials into spatially organized, functional arrangements is essential for developing unconventional electronic systems. Here, we report a laser-driven noncontact bubble transfer printing via a hydrogel composite stamp, which features a circular reservoir filled with hydrogel inside a stamp body and encapsulated by a laser absorption layer and an adhesion layer. This composite structure of stamp provides a reversible thermal controlled adhesion in a rapid manner through the liquid-gas phase transition of water in the hydrogel. The ultrasoft nature of hydrogel minimizes the influence of preload on the pick-up performance, which offers a strong interfacial adhesion under a small preload for a reliable damage-free pick-up. The strong light-matter interaction at the interface induces a liquid-gas phase transition to form a bulge on the stamp surface, which eliminates the interfacial adhesion for a successful noncontact printing. Demonstrations of noncontact transfer printing of microscale Si platelets onto various challenging nonadhesive surfaces (e.g., glass, key, wrench, steel sphere, dry petal, droplet) in two-dimensional or three-dimensional layouts illustrate the unusual capabilities for deterministic assembly to develop unconventional electronic systems such as flexible inorganic electronics, curved electronics, and micro-LED display.

Long-Term Flexible Neural Interface for Synchronous Recording of Cross-Regional Sensory Processing along the Olfactory Pathway.

Humans perceive the world through five senses, of which olfaction is the oldest evolutionary sense that enables the detection of chemicals in the external environment. Recent progress in bioinspired electronics has boosted the development of artificial sensory systems. Here, a biohybrid olfactory system is proposed by integrating living mammals with implantable flexible neural electrodes, to employ the outstanding properties of mammalian olfactory system. In olfactory perception, the peripheral organ-olfactory epithelium (OE) projects axons into the olfactory relay station-olfactory bulb (OB). The olfactory information encoded in the neural activity is recorded from both OE and OB simultaneously using flexible neural electrodes. Results reveal that spontaneous slow oscillations (<12 Hz) in both OE and OB closely follow respiration. This respiration-locked rhythm modulates the amplitude of fast oscillations (>20 Hz), which are associated with odor perception. Further, by extracting the characteristics of odor-evoked oscillatory signals, responses of different odors are identified and classified with 80% accuracy. This study demonstrates for the first time that the flexible electrode enables chronic stable electrophysiological recordings of the peripheral and central olfactory system in vivo. Overall, the method provides a novel neural interface for olfactory biosensing and cognitive processing.

Copper-Catalyzed Tertiary Alkylative Cyanation for the Synthesis of Cyanated Peptide Building Blocks.

In this paper, we report efficient cyanation of various peptides containing the α-bromocarbonyl moiety using a Cu-catalyzed radical-based methodology employing zinc cyanide as the cyanide source. Mechanistic studies revealed that in situ formed CuCN was a key intermediate during the catalytic cycle. Our method could be useful for the synthesis of modified peptides containing quaternary carbons.

Surface wrinkling of an elastic graded layer.

Surface instabilities have been extensively studied for homogeneous materials or film/substrate systems but with less studies on elastic graded materials. This paper studies surface wrinkling of an elastic graded layer theoretically, numerically and experimentally. A theoretical model for the onset of surface wrinkling with a sinusoidal mode is established. The predicted critical wrinkling strain and wavelength agree well with finite element analysis (FEA) for the elastic graded layer with exponentially decaying modulus. The influence of the layer thickness as well as the material properties on the critical conditions for the onset of surface wrinkling is fully investigated. The morphology evolution of surface wrinkling from FEA indicates the transitions of the sinusoidal mode to the arch mode and then to the period-doubling mode with a co-existing crease mode and folding mode, which agree well quantitatively with experimental observations. These results are helpful to provide physical insights into the influence of material inhomogeneity on surface instabilities.

Rapidly tunable and highly reversible bio-inspired dry adhesion for transfer printing in air and a vacuum.

Tunable and reversible dry adhesion has attracted much attention in academia and industry due to its wide applications ranging from releasable joints to stamps for transfer printing. Here, a simple yet robust magnetically actuated, aphid-inspired design of an elastomeric surface that provides rapidly tunable and highly reversible adhesion strength is reported. The magnetically actuated adhesive features open reservoirs filled with magnetic particles and encapsulated by a thin surface membrane, which can be deformed in a controlled manner via the magnetic field, thus, to tune the adhesion. The combination of the rate dependent effect and magnetic actuation of the thin surface membrane offers continuously tunable adhesion with a great switchability and a quick response. Experimental and theoretical studies reveal the underlying physics and provide design guidelines to optimize geometries for the broad control of adhesion. Demonstrations of this concept in stamps for transfer printing of silicon wafers in air and in a vacuum with a selective and programmable mode illustrate the capabilities for deterministic assembly and the potential in the semiconductor industry.

Ultrathin conformal devices for precise and continuous thermal characterization of human skin.

Precision thermometry of the skin can, together with other measurements, provide clinically relevant information about cardiovascular health, cognitive state, malignancy and many other important aspects of human physiology. Here, we introduce an ultrathin, compliant skin-like sensor/actuator technology that can pliably laminate onto the epidermis to provide continuous, accurate thermal characterizations that are unavailable with other methods. Examples include non-invasive spatial mapping of skin temperature with millikelvin precision, and simultaneous quantitative assessment of tissue thermal conductivity. Such devices can also be implemented in ways that reveal the time-dynamic influence of blood flow and perfusion on these properties. Experimental and theoretical studies establish the underlying principles of operation, and define engineering guidelines for device design. Evaluation of subtle variations in skin temperature associated with mental activity, physical stimulation and vasoconstriction/dilation along with accurate determination of skin hydration through measurements of thermal conductivity represent some important operational examples.

Periodic buckling patterns of graphene/hexagonal boron nitride heterostructure.

Graphene/hexagonal boron nitride (h-BN) heterostructure has showed great potential to improve the performance of a graphene device. A graphene on an h-BN substrate may buckle due to the thermal expansion mismatch between the graphene and h-BN. We used an energy method to investigate the periodic buckling patterns including one-dimensional, square checkerboard, hexagonal, equilateral triangular and herringbone mode in a graphene/h-BN heterostructure under equi-biaxial compression. The total energy, consisting of cohesive energy, graphene membrane energy and graphene bending energy, for each buckling pattern is obtained analytically. At a compression slightly larger than the critical strain, all buckling patterns have the same total energies, which suggests that any buckling pattern may occur. At a compression much larger than the critical strain, the herringbone mode has the lowest total energy by significantly reducing the membrane energy of graphene at the expense of a slight increase of the bending energy of graphene and cohesive energy. These results may serve as guidelines for strain engineering in graphene/h-BN heterostructures.

A hemispherical electronic eye camera based on compressible silicon optoelectronics.

The human eye is a remarkable imaging device, with many attractive design features. Prominent among these is a hemispherical detector geometry, similar to that found in many other biological systems, that enables a wide field of view and low aberrations with simple, few-component imaging optics. This type of configuration is extremely difficult to achieve using established optoelectronics technologies, owing to the intrinsically planar nature of the patterning, deposition, etching, materials growth and doping methods that exist for fabricating such systems. Here we report strategies that avoid these limitations, and implement them to yield high-performance, hemispherical electronic eye cameras based on single-crystalline silicon. The approach uses wafer-scale optoelectronics formed in unusual, two-dimensionally compressible configurations and elastomeric transfer elements capable of transforming the planar layouts in which the systems are initially fabricated into hemispherical geometries for their final implementation. In a general sense, these methods, taken together with our theoretical analyses of their associated mechanics, provide practical routes for integrating well-developed planar device technologies onto the surfaces of complex curvilinear objects, suitable for diverse applications that cannot be addressed by conventional means.

Unusual strategies for using indium gallium nitride grown on silicon (111) for solid-state lighting.

Properties that can now be achieved with advanced, blue indium gallium nitride light emitting diodes (LEDs) lead to their potential as replacements for existing infrastructure in general illumination, with important implications for efficient use of energy. Further advances in this technology will benefit from reexamination of the modes for incorporating this materials technology into lighting modules that manage light conversion, extraction, and distribution, in ways that minimize adverse thermal effects associated with operation, with packages that exploit the unique aspects of these light sources. We present here ideas in anisotropic etching, microscale device assembly/integration, and module configuration that address these challenges in unconventional ways. Various device demonstrations provide examples of the capabilities, including thin, flexible lighting "tapes" based on patterned phosphors and large collections of small light emitters on plastic substrates. Quantitative modeling and experimental evaluation of heat flow in such structures illustrates one particular, important aspect of their operation: small, distributed LEDs can be passively cooled simply by direct thermal transport through thin-film metallization used for electrical interconnect, providing an enhanced and scalable means to integrate these devices in modules for white light generation.

A Multifunctional Flexible Tactile Sensor Based on Resistive Effect for Simultaneous Sensing of Pressure and Temperature.

Flexible tactile sensors with multifunctional sensing functions have attracted much attention due to their wide applications in artificial limbs, intelligent robots, human-machine interfaces, and health monitoring devices. Here, a multifunctional flexible tactile sensor based on resistive effect for simultaneous sensing of pressure and temperature is reported. The sensor features a simple design with patterned metal film on a soft substrate with cavities and protrusions. The decoupling of pressure and temperature sensing is achieved by the reasonable arrangement of metal layers in the patterned metal film. Systematically experimental and numerical studies are carried out to reveal the multifunctional sensing mechanism and show that the proposed sensor exhibits good linearity, fast response, high stability, good mechanical flexibility, and good microfabrication compatibility. Demonstrations of the multifunctional flexible tactile sensor to monitor touch, breathing, pulse and objects grabbing/releasing in various application scenarios involving coupled temperature/pressure stimuli illustrate its excellent capability of measuring pressure and temperature simultaneously. These results offer an effective tool for multifunctional sensing of pressure and temperature and create engineering opportunities for applications of wearable health monitoring and human-machine interfaces.

Tunable and Reversible Adhesive of Liquid Metal Ferrofluid Pillars for Magnetically Actuated Noncontact Transfer Printing.

Transfer printing techniques based on tunable and reversible adhesives enable the heterogeneous integration of materials in desired layouts and are essential for developing both existing and envisioned electronic systems. Here, a novel tunable and reversible adhesive of liquid metal ferrofluid pillars for developing an efficient magnetically actuated noncontact transfer printing is reported. The liquid metal ferrofluid pillars offer the appealing advantages of gentle contact force by minimizing the preload effect and exceptional shape adaptability by maximizing the interfacial contact area due to their inherent fluidity, thus enabling a reliable damage-free pickup. Moreover, the liquid metal ferrofluid pillars harness the rapid stiffness increase and shape change with the magnetic field, generating an instantaneous ejection force to achieve a receiver-independent noncontact printing. Demonstrations of the adhesive of liquid metal ferrofluid pillars in transfer printing of diverse objects with different shapes, materials and dimensions onto various substrates illustrate its great potential in deterministic assembly.

Switchable Adhesive Based on Shape Memory Polymer with Micropillars of Different Heights for Laser-Driven Noncontact Transfer Printing.

Switchable adhesive is essential to develop transfer printing, which is an advanced heterogeneous material integration technique for developing electronic systems. Designing a switchable adhesive with strong adhesion strength that can also be easily eliminated to enable noncontact transfer printing still remains a challenge. Here, we report a simple yet robust design of switchable adhesive based on a thermally responsive shape memory polymer with micropillars of different heights. The adhesive takes advantage of the shape-fixing property of shape memory polymer to provide strong adhesion for a reliable pick-up and the various levels of shape recovery of micropillars under laser heating to eliminate the adhesion for robust printing in a noncontact way. Systematic experimental and numerical studies reveal the adhesion switch mechanism and provide insights into the design of switchable adhesives. This switchable adhesive design provides a good solution to develop laser-driven noncontact transfer printing with the capability of eliminating the influence of receivers on the performance of transfer printing. Demonstrations of transfer printing of silicon wafers, microscale Si platelets, and micro light emitting diode (µ-LED) chips onto various challenging nonadhesive receivers (e.g., sandpaper, stainless steel bead, leaf, or glass) to form desired two-dimensional or three-dimensional layouts illustrate its great potential in deterministic assembly.

Bone Fracture Healing under the Intervention of a Stretchable Ultrasound Array.

Ultrasound treatment has been recognized as an effective and noninvasive approach to promote fracture healing. However, traditional rigid ultrasound probe is bulky, requiring cumbersome manual operations and inducing unfavorable side effects when functioning, which precludes the wide application of ultrasound in bone fracture healing. Here, we report a stretchable ultrasound array for bone fracture healing, which features high-performance 1-3 piezoelectric composites as transducers, stretchable multilayered serpentine metal films in a bridge-island pattern as electrical interconnects, soft elastomeric membranes as encapsulations, and polydimethylsiloxane (PDMS) with low curing agent ratio as adhesive layers. The resulting ultrasound array offers the benefits of large stretchability for easy skin integration and effective affecting region for simple skin alignment with good electromechanical performance. Experimental investigations of the stretchable ultrasound array on the delayed union model in femoral shafts of rats show that the callus growth is more active in the second week of treatment and the fracture site is completely osseous healed in the sixth week of treatment. Various bone quality indicators (e.g., bone modulus, bone mineral density, bone tissue/total tissue volume, and trabecular bone thickness) could be enhanced with the intervention of a stretchable ultrasound array. Histological and immunohistochemical examinations indicate that ultrasound promotes osteoblast differentiation, bone formation, and remodeling by promoting the expression of osteopontin (OPN) and runt-related transcription factor 2 (RUNX2). This work provides an effective tool for bone fracture healing in a simple and convenient manner and creates engineering opportunities for applying ultrasound in medical applications.

Skin-Inspired All-Natural Biogel for Bioadhesive Interface.

Natural material-based hydrogels are considered ideal candidates for constructing robust bio-interfaces due to their environmentally sustainable nature and biocompatibility. However, these hydrogels often encounter limitations such as weak mechanical strength, low water resistance, and poor ionic conductivity. Here, inspired by the role of natural moisturizing factor (NMF) in skin, a straightforward yet versatile strategy is proposed for fabricating all-natural ionic biogels that exhibit high resilience, ionic conductivity, resistance to dehydration, and complete degradability, without necessitating any chemical modification. A well-balanced combination of gelatin and sodium pyrrolidone carboxylic acid (an NMF compound) gives rise to a significant enhancement in the mechanical strength, ionic conductivity, and water retention capacity of the biogel compared to pure gelatin hydrogel. The biogel manifests temperature-controlled reversible fluid-gel transition properties attributed to the triple-helix junctions of gelatin, which enables in situ gelation on diverse substrates, thereby ensuring conformal contact and dynamic compliance with curved surfaces. Due to its salutary properties, the biogel can serve as an effective and biocompatible interface for high-quality and long-term electrophysiological signal recording. These findings provide a general and scalable approach for designing natural material-based hydrogels with tailored functionalities to meet diverse application needs.

Restoration of coherent reach-grasp-pull movement via sequential intraneural peripheral nerve stimulation in rats.

Objective.Peripheral nerve stimulation (PNS) has been demonstrated as an effective way to selectively activate muscles and to produce fine hand movements. However, sequential multi-joint upper limb movements, which are critical for paralysis rehabilitation, has not been tested with PNS. Here, we aimed to restore multiple upper limb joint movements through an intraneural interface with a single electrode, achieving coherent reach-grasp-pull movement tasks through sequential stimulation.Approach.A transverse intrafascicular multichannel electrode was implanted under the axilla of the rat's upper limb, traversing the musculocutaneous, radial, median, and ulnar nerves. Intramuscular electrodes were implanted into the biceps brachii (BB), triceps brachii (TB), flexor carpi radialis (FCR), and extensor carpi radialis (ECR) muscles to record electromyographic (EMG) activity and video recordings were used to capture the kinematics of elbow, wrist, and digit joints. Charge-balanced biphasic pulses were applied to different channels to recruit distinct upper limb muscles, with concurrent recording of EMG signals and joint kinematics to assess the efficacy of the stimulation. Finally, a sequential stimulation protocol was employed by generating coordinated pulses in different channels.Main results.BB, TB, FCR and ECR muscles were selectively activated and various upper limb movements, including elbow flexion, elbow extension, wrist flexion, wrist extension, digit flexion, and digit extension, were reliably generated. The modulation effects of stimulation parameters, including pulse width, amplitude, and frequency, on induced joint movements were investigated and reach-grasp-pull movement was elicited by sequential stimulation.Significance.Our results demonstrated the feasibility of sequential intraneural stimulation for functional multi-joint movement restoration, providing a new approach for clinical rehabilitation in paralyzed patients.

Kirigami-Triggered Spoof Plasmonic Interconnects for Radiofrequency Elastronics.

The flexible and conformal interconnects for electronic systems as a potential signal transmission device have great prospects in body-worn or wearable applications. High-efficiency wave propagation and conformal structure deformation around human body at radio communication are still confronted with huge challenges due to the lack of methods to control the wave propagation and achieve the deformable structure simultaneously. Here, inspired by the kirigami technology, a new paradigm to construct spoof plasmonic interconnects (SPIs) that support radiofrequency (RF) surface plasmonic transmission is proposed, together with high elasticity, strong robustness, and multifunction performance. Leveraging the strong field-confinement characteristic of spoof surface plasmons polaritons, the Type-I SPI opens its high-efficiency transmission band after stretching from a simply connected metallic surface. Meanwhile, the broadband transmission of the kirigami-based SPI exhibits strong robustness and excellent stability undergoing complex deformations, i.e., bending, twisting, and stretching. In addition, the prepared Type-II SPI consisting of 2 different subunit cells can achieve band-stop transmission characteristics, with its center frequency dynamically tunable by stretching the buckled structure. Experimental measurements verify the on-off switching performance in kirigami interconnects triggered by stretching. Overcoming the mechanical limitation of rigid structure with kirigami technology, the designer SPIs exhibit high stretchability through out-of-plane structure deformation. Such kirigami-based interconnects can improve the elastic functionality of wearable RF electronics and offer high compatibility to large body motion in future body network systems.

Decatungstate-Catalyzed C(sp3)-H Alkylation of a Val Residue Proximal to the N-Terminus Controlled by an Electrostatic Interaction.

The decatungstate photocatalyst [W10O32]4- efficiently promoted the C(sp3)-H alkylation of the trifluoroacetic acid salt of valine methyl ester (H-Val-OMe·TFA) with electron-deficient alkenes under UV irradiation. The electrostatic interaction between the cationic ammonium group (+NH3) of the main chain and anionic [W10O32]4- played an important role in this reaction. The influence of various protected amino acids in the C(sp3)-H alkylation was investigated as the model reaction for the alkylation of Val-containing peptides. The introduction of an alkyne moiety into Val through this alkylation was successful, and successive copper-catalyzed azide-alkyne cycloaddition (CuAAC) was demonstrated. The C(sp3)-H bond of a Val residue located at the second from the N-terminus was also successfully converted. C(sp3)-H alkylation of oligopeptides containing two Val residues selectively proceeded proximally to the N-terminus.

High-efficiency, microscale GaN light-emitting diodes and their thermal properties on unusual substrates.

A method for forming efficient, ultrathin GaN light-emitting diodes (LEDs) and for their assembly onto foreign substances is reported. The LEDs have lateral dimensions ranging from ~1 mm × 1 mm to ~25 µm × 25 µm. Quantitative experimental and theoretical studies show the benefits of small device geometry on thermal management, for both continuous and pulsed-mode operation, the latter of which suggests the potential use of these technologies in bio-integrated contexts.

Materials for multifunctional balloon catheters with capabilities in cardiac electrophysiological mapping and ablation therapy.

Developing advanced surgical tools for minimally invasive procedures represents an activity of central importance to improving human health. A key challenge is in establishing biocompatible interfaces between the classes of semiconductor device and sensor technologies that might be most useful in this context and the soft, curvilinear surfaces of the body. This paper describes a solution based on materials that integrate directly with the thin elastic membranes of otherwise conventional balloon catheters, to provide diverse, multimodal functionality suitable for clinical use. As examples, we present sensors for measuring temperature, flow, tactile, optical and electrophysiological data, together with radiofrequency electrodes for controlled, local ablation of tissue. Use of such 'instrumented' balloon catheters in live animal models illustrates their operation, as well as their specific utility in cardiac ablation therapy. The same concepts can be applied to other substrates of interest, such as surgical gloves.

Implantable Thermal Therapeutic Device with Precise Temperature Control Enabled by Foldable Electronics and Heat-Insulating Pads.

Thermal therapy has continued to attract the attention of researchers and clinicians due to its important applications in tumor ablation, wound management, and drug release. The lack of precise temperature control capability in traditional thermal treatment may cause the decrease of therapeutic effect and thermal damage to normal tissues. Here, we report an implantable thermal therapeutic device (ITTD), which offers precise closed loop heating, in situ temperature monitoring, and thermal protection. The ITTD features a multifunctional foldable electronics device wrapped on a heat-insulating composite pad. Experimental and numerical studies reveal the fundamental aspects of the design, fabrication, and operation of the ITTD. In vivo experiments of the ITTD in thermal ablation for antitumor demonstrate that the proposed ITTD is capable of controlling the ablation temperature precisely in real time with a precision of at least 0.7°C and providing effective thermal protection to normal tissues. This proof-of-concept research creates a promising route to develop ITTD with precise temperature control capability, which is highly desired in thermal therapy and other disease diagnosis and treatments.