High-speed and large-scale intrinsically stretchable integrated circuits.

Intrinsically stretchable electronics with skin-like mechanical properties have been identified as a promising platform for emerging applications ranging from continuous physiological monitoring to real-time analysis of health conditions, to closed-loop delivery of autonomous medical treatment1-7. However, current technologies could only reach electrical performance at amorphous-silicon level (that is, charge-carrier mobility of about 1 cm2 V-1 s-1), low integration scale (for example, 54 transistors per circuit) and limited functionalities8-11. Here we report high-density, intrinsically stretchable transistors and integrated circuits with high driving ability, high operation speed and large-scale integration. They were enabled by a combination of innovations in materials, fabrication process design, device engineering and circuit design. Our intrinsically stretchable transistors exhibit an average field-effect mobility of more than 20 cm2 V-1 s-1 under 100% strain, a device density of 100,000 transistors per cm2, including interconnects and a high drive current of around 2 µA µm-1 at a supply voltage of 5 V. Notably, these achieved parameters are on par with state-of-the-art flexible transistors based on metal-oxide, carbon nanotube and polycrystalline silicon materials on plastic substrates12-14. Furthermore, we realize a large-scale integrated circuit with more than 1,000 transistors and a stage-switching frequency greater than 1 MHz, for the first time, to our knowledge, in intrinsically stretchable electronics. Moreover, we demonstrate a high-throughput braille recognition system that surpasses human skin sensing ability, enabled by an active-matrix tactile sensor array with a record-high density of 2,500 units per cm2, and a light-emitting diode display with a high refreshing speed of 60 Hz and excellent mechanical robustness. The above advancements in device performance have substantially enhanced the abilities of skin-like electronics.

High-brightness all-polymer stretchable LED with charge-trapping dilution.

Next-generation light-emitting displays on skin should be soft, stretchable and bright1-7. Previously reported stretchable light-emitting devices were mostly based on inorganic nanomaterials, such as light-emitting capacitors, quantum dots or perovskites6-11. They either require high operating voltage or have limited stretchability and brightness, resolution or robustness under strain. On the other hand, intrinsically stretchable polymer materials hold the promise of good strain tolerance12,13. However, realizing high brightness remains a grand challenge for intrinsically stretchable light-emitting diodes. Here we report a material design strategy and fabrication processes to achieve stretchable all-polymer-based light-emitting diodes with high brightness (about 7,450 candela per square metre), current efficiency (about 5.3 candela per ampere) and stretchability (about 100 per cent strain). We fabricate stretchable all-polymer light-emitting diodes coloured red, green and blue, achieving both on-skin wireless powering and real-time displaying of pulse signals. This work signifies a considerable advancement towards high-performance stretchable displays.

High-frequency and intrinsically stretchable polymer diodes.

Skin-like intrinsically stretchable soft electronic devices are essential to realize next-generation remote and preventative medicine for advanced personal healthcare1-4. The recent development of intrinsically stretchable conductors and semiconductors has enabled highly mechanically robust and skin-conformable electronic circuits or optoelectronic devices2,5-10. However, their operating frequencies have been limited to less than 100 hertz, which is much lower than that required for many applications. Here we report intrinsically stretchable diodes-based on stretchable organic and nanomaterials-capable of operating at a frequency as high as 13.56 megahertz. This operating frequency is high enough for the wireless operation of soft sensors and electrochromic display pixels using radiofrequency identification in which the base-carrier frequency is 6.78 megahertz or 13.56 megahertz. This was achieved through a combination of rational material design and device engineering. Specifically, we developed a stretchable anode, cathode, semiconductor and current collector that can satisfy the strict requirements for high-frequency operation. Finally, we show the operational feasibility of our diode by integrating it with a stretchable sensor, electrochromic display pixel and antenna to realize a stretchable wireless tag. This work is an important step towards enabling enhanced functionalities and capabilities for skin-like wearable electronics.

A Design Strategy for Intrinsically Stretchable High-Performance Polymer Semiconductors: Incorporating Conjugated Rigid Fused-Rings with Bulky Side Groups.

Strategies to improve stretchability of polymer semiconductors, such as introducing flexible conjugation-breakers or adding flexible blocks, usually result in degraded electrical properties. In this work, we propose a concept to address this limitation, by introducing conjugated rigid fused-rings with optimized bulky side groups and maintaining a conjugated polymer backbone. Specifically, we investigated two classes of rigid fused-ring systems, namely, benzene-substituted dibenzothiopheno[6,5-b:6',5'-f]thieno[3,2-b]thiophene (Ph-DBTTT) and indacenodithiophene (IDT) systems, and identified molecules displaying optimized electrical and mechanical properties. In the IDT system, the polymer PIDT-3T-OC12-10% showed promising electrical and mechanical properties. In fully stretchable transistors, the polymer PIDT-3T-OC12-10% showed a mobility of 0.27 cm2 V-1 s-1 at 75% strain and maintained its mobility after being subjected to hundreds of stretching-releasing cycles at 25% strain. Our results underscore the intimate correlation between chemical structures, mechanical properties, and charge carrier mobility for polymer semiconductors. Our described molecular design approach will help to expedite the next generation of intrinsically stretchable high-performance polymer semiconductors.

Ultrasensitive Monolayer MoS2 Field-Effect Transistor Based DNA Sensors for Screening of Down Syndrome.

Field-effect transistor (FET) biosensors based on low-dimensional materials present the advantages of low cost, high speed, small size, and excellent compatibility with integrated circuits (ICs). In this work, we fabricated highly sensitive FET-based DNA biosensors based on chemical vapor deposition (CVD)-grown monolayer MoS2 films in batches and explored their application in noninvasive prenatal testing (NIPT) for trisomy 21 syndrome. Specifically, MoS2 was functionalized with gold nanoparticles (Au NPs) of an optimized size and at an ideal density, and then, probe DNAs for the specific capture of target DNAs were immobilized on the nanoparticles. The fabricated FET biosensors are able to reliably detect target DNA fragments (chromosome 21 or 13) with a detection limit below 100 aM, a high response up to 240%, and a high specificity, which satisfy the requirement for the screening of Down syndrome. In addition, a real-time test was conducted to show that the biosensor clearly responds to the target DNA at concentrations as low as 1 fM. Our approach shows the potential for detecting the over-expression of chromosome 21 in the peripheral blood of pregnant women and achieving Down syndrome screening.

Carbon nanotube radio-frequency electronics.

Carbon nanotube (CNT) is considered a promising material for radio-frequency (RF) applications, owing to its high carrier mobility and saturated drift velocity, as well as ultra-small intrinsic gate capacitance. Here, we review progress on CNT-based devices and integrated circuits for RF applications, including theoretical projection of RF performance of CNT-based devices, preparation of CNT materials, fabrication, optimization of RF field-effect transistors (FETs) structures, and ambipolar FET-based RF applications, and we outline challenges and prospects of CNT-based RF applications.

Environmentally stable and stretchable polymer electronics enabled by surface-tethered nanostructured molecular-level protection.

Stretchable polymer semiconductors (PSCs) are essential for soft stretchable electronics. However, their environmental stability remains a longstanding concern. Here we report a surface-tethered stretchable molecular protecting layer to realize stretchable polymer electronics that are stable in direct contact with physiological fluids, containing water, ions and biofluids. This is achieved through the covalent functionalization of fluoroalkyl chains onto a stretchable PSC film surface to form densely packed nanostructures. The nanostructured fluorinated molecular protection layer (FMPL) improves the PSC operational stability over an extended period of 82 days and maintains its protection under mechanical deformation. We attribute the ability of FMPL to block water absorption and diffusion to its hydrophobicity and high fluorination surface density. The protection effect of the FMPL (~6 nm thickness) outperforms various micrometre-thick stretchable polymer encapsulants, leading to a stable PSC charge carrier mobility of ~1 cm2 V-1 s-1 in harsh environments such as in 85-90%-humidity air for 56 days or in water or artificial sweat for 42 days (as a benchmark, the unprotected PSC mobility degraded to 10-6 cm2 V-1 s-1 in the same period). The FMPL also improved the PSC stability against photo-oxidative degradation in air. Overall, we believe that our surface tethering of the nanostructured FMPL is a promising approach to achieve highly environmentally stable and stretchable polymer electronics.

Soft and stretchable organic bioelectronics for continuous intraoperative neurophysiological monitoring during microsurgery.

In microneurosurgery, it is crucial to maintain the structural and functional integrity of the nerve through continuous intraoperative identification of neural anatomy. To this end, here we report the development of a translatable system leveraging soft and stretchable organic-electronic materials for continuous intraoperative neurophysiological monitoring. The system uses conducting polymer electrodes with low impedance and low modulus to record near-field action potentials continuously during microsurgeries, offers higher signal-to-noise ratios and reduced invasiveness when compared with handheld clinical probes for intraoperative neurophysiological monitoring and can be multiplexed, allowing for the precise localization of the target nerve in the absence of anatomical landmarks. Compared with commercial metal electrodes, the neurophysiological monitoring system allowed for enhanced post-operative prognoses after tumour-resection surgeries in rats. Continuous recording of near-field action potentials during microsurgeries may allow for the precise identification of neural anatomy through the entire procedure.

Neuromorphic sensorimotor loop embodied by monolithically integrated, low-voltage, soft e-skin.

Artificial skin that simultaneously mimics sensory feedback and mechanical properties of natural skin holds substantial promise for next-generation robotic and medical devices. However, achieving such a biomimetic system that can seamlessly integrate with the human body remains a challenge. Through rational design and engineering of material properties, device structures, and system architectures, we realized a monolithic soft prosthetic electronic skin (e-skin). It is capable of multimodal perception, neuromorphic pulse-train signal generation, and closed-loop actuation. With a trilayer, high-permittivity elastomeric dielectric, we achieved a low subthreshold swing comparable to that of polycrystalline silicon transistors, a low operation voltage, low power consumption, and medium-scale circuit integration complexity for stretchable organic devices. Our e-skin mimics the biological sensorimotor loop, whereby a solid-state synaptic transistor elicits stronger actuation when a stimulus of increasing pressure is applied.

Spiral NeuroString: High-Density Soft Bioelectronic Fibers for Multimodal Sensing and Stimulation.

Bioelectronic fibers hold promise for both research and clinical applications due to their compactness, ease of implantation, and ability to incorporate various functionalities such as sensing and stimulation. However, existing devices suffer from bulkiness, rigidity, limited functionality, and low density of active components. These limitations stem from the difficulty to incorporate many components on one-dimensional (1D) fiber devices due to the incompatibility of conventional microfabrication methods (e.g., photolithography) with curved, thin and long fiber structures. Herein, we introduce a fabrication approach, ‶spiral transformation″, to convert two-dimensional (2D) films containing microfabricated devices into 1D soft fibers. This approach allows for the creation of high density multimodal soft bioelectronic fibers, termed Spiral NeuroString (S-NeuroString), while enabling precise control over the longitudinal, angular, and radial positioning and distribution of the functional components. We show the utility of S-NeuroString for motility mapping, serotonin sensing, and tissue stimulation within the dynamic and soft gastrointestinal (GI) system, as well as for single-unit recordings in the brain. The described bioelectronic fibers hold great promises for next-generation multifunctional implantable electronics.

Wireless, closed-loop, smart bandage with integrated sensors and stimulators for advanced wound care and accelerated healing.

'Smart' bandages based on multimodal wearable devices could enable real-time physiological monitoring and active intervention to promote healing of chronic wounds. However, there has been limited development in incorporation of both sensors and stimulators for the current smart bandage technologies. Additionally, while adhesive electrodes are essential for robust signal transduction, detachment of existing adhesive dressings can lead to secondary damage to delicate wound tissues without switchable adhesion. Here we overcome these issues by developing a flexible bioelectronic system consisting of wirelessly powered, closed-loop sensing and stimulation circuits with skin-interfacing hydrogel electrodes capable of on-demand adhesion and detachment. In mice, we demonstrate that our wound care system can continuously monitor skin impedance and temperature and deliver electrical stimulation in response to the wound environment. Across preclinical wound models, the treatment group healed ~25% more rapidly and with ~50% enhancement in dermal remodeling compared with control. Further, we observed activation of proregenerative genes in monocyte and macrophage cell populations, which may enhance tissue regeneration, neovascularization and dermal recovery.

Topological supramolecular network enabled high-conductivity, stretchable organic bioelectronics.

Intrinsically stretchable bioelectronic devices based on soft and conducting organic materials have been regarded as the ideal interface for seamless and biocompatible integration with the human body. A remaining challenge is to combine high mechanical robustness with good electrical conduction, especially when patterned at small feature sizes. We develop a molecular engineering strategy based on a topological supramolecular network, which allows for the decoupling of competing effects from multiple molecular building blocks to meet complex requirements. We obtained simultaneously high conductivity and crack-onset strain in a physiological environment, with direct photopatternability down to the cellular scale. We further collected stable electromyography signals on soft and malleable octopus and performed localized neuromodulation down to single-nucleus precision for controlling organ-specific activities through the delicate brainstem.

Monolithic optical microlithography of high-density elastic circuits.

Polymeric electronic materials have enabled soft and stretchable electronics. However, the lack of a universal micro/nanofabrication method for skin-like and elastic circuits results in low device density and limited parallel signal recording and processing ability relative to silicon-based devices. We present a monolithic optical microlithographic process that directly micropatterns a set of elastic electronic materials by sequential ultraviolet light-triggered solubility modulation. We fabricated transistors with channel lengths of 2 micrometers at a density of 42,000 transistors per square centimeter. We fabricated elastic circuits including an XOR gate and a half adder, both of which are essential components for an arithmetic logic unit. Our process offers a route to realize wafer-level fabrication of complex, high-density, and multilayered elastic circuits with performance rivaling that of their rigid counterparts.

A molecular design approach towards elastic and multifunctional polymer electronics.

Next-generation wearable electronics require enhanced mechanical robustness and device complexity. Besides previously reported softness and stretchability, desired merits for practical use include elasticity, solvent resistance, facile patternability and high charge carrier mobility. Here, we show a molecular design concept that simultaneously achieves all these targeted properties in both polymeric semiconductors and dielectrics, without compromising electrical performance. This is enabled by covalently-embedded in-situ rubber matrix (iRUM) formation through good mixing of iRUM precursors with polymer electronic materials, and finely-controlled composite film morphology built on azide crosslinking chemistry which leverages different reactivities with C-H and C=C bonds. The high covalent crosslinking density results in both superior elasticity and solvent resistance. When applied in stretchable transistors, the iRUM-semiconductor film retained its mobility after stretching to 100% strain, and exhibited record-high mobility retention of 1 cm2 V-1 s-1 after 1000 stretching-releasing cycles at 50% strain. The cycling life was stably extended to 5000 cycles, five times longer than all reported semiconductors. Furthermore, we fabricated elastic transistors via consecutively photo-patterning of the dielectric and semiconducting layers, demonstrating the potential of solution-processed multilayer device manufacturing. The iRUM represents a molecule-level design approach towards robust skin-inspired electronics.

Strengthened Complementary Metal-Oxide-Semiconductor Logic for Small-Band-Gap Semiconductor-Based High-Performance and Low-Power Application.

Silicon-based complementary metal-oxide-semiconductor (CMOS) has been the mainstream logic style for modern digital integrated circuits (ICs) for decades but will meet its performance limits soon. Extensive investigations have thus been carried out using other semiconductors, especially those with extremely high carrier mobility. However, these materials usually have small or even zero band gap, which leads inevitably to large leakage current or voltage loss in ICs based on these semiconductors. In this work, we propose and demonstrate a strengthened CMOS (SCMOS) logic style using modified field-effect transistors (FETs) to solve this problem, that is, to achieve high performance, utilizing the high carrier mobility in these materials, and to reduce the current leakage resulting from their small band gap. Conventional CMOS FETs are modified to have an asymmetric structure where an additional assistant gate is introduced near the drain to further lower the potential barrier in on-state and to increase the barrier in off-state. SCMOS ICs are constructed using these modified asymmetric CMOS FETs, which demonstrate perfect rail-to-rail output with negligible voltage loss and 3 orders of magnitude suppression of the static power consumption and an operating speed similar to or even higher than that of CMOS ICs. Here, SCMOS is demonstrated using carbon nanotubes, but, in principle, this logic style can be used in ICs based on any small-band-gap semiconductors to provide simultaneously high performance and low power consumption.

Carbon Nanotube Film-Based Radio Frequency Transistors with Maximum Oscillation Frequency above 100 GHz.

Carbon nanotubes (CNTs) have been considered a preferred channel material for constructing high-performance radio frequency (RF) transistors with outstanding current gain cutoff frequency (fT) and power gain cutoff frequency (fmax) but the highest reported fmax is only 70 GHz. Here, we explore how good RF transistors based on solution-derived randomly oriented semiconducting CNT films, which are the most mature CNT materials for scalable fabrication of transistors and integrated circuits, can be achieved. Owing to the significantly reduced number of CNT/CNT junctions obtained by scaling the channel length down to below 100 nm, we realized RF field-effect transistors (FETs) with maximum transconductance Gm up to 0.38 mS/µm, which is the record among CNT-based RF FETs. After de-embedding the pad-induced capacitances and resistances, the CNT FETs with different gate lengths (Lg) exhibit fT as high as 103 GHz (intrinsically 281 GHz) or fmax up to 107 GHz (intrinsically 190 GHz), which are the records among CNT-based RF FETs. In particular, the CNT FETs with an Lg of 50 nm present pad de-embedding fT of 86 GHz and fmax of 85 GHz, and represent the best CNT RF transistor in terms of comprehensive performance to date. To demonstrate the actual high-speed and scalable fabrication of our CNT RF FETs, we fabricated CNT FET-based five-stage ring oscillators with oscillation frequencies above 5 GHz.

Carbon Nanotube Complementary Gigahertz Integrated Circuits and Their Applications on Wireless Sensor Interface Systems.

Along with ultralow-energy delay products and symmetric complementary polarities, carbon nanotube field-effect transistors (CNT FETs) are expected to be promising building blocks for energy-efficient computing technology. However, the work frequencies of the existing CNT-based complementary metal-oxide-semiconductor (CMOS) integrated circuits (ICs) are far below the requirement (850 MHz) in state-of-art wireless communication applications. In this work, we fabricated deep submicron CMOS FETs with considerably improved performance of n-type CNT FETs and hence significantly promoted the work frequency of CNT CMOS ICs to 1.98 GHz. Based on these high-speed and sensitive voltage-controlled oscillators, we then presented a wireless sensor interface circuit with working frequency up to 1.5 GHz spectrum. As a preliminary demonstration, an energy-efficient wireless temperature sensing interface system was realized combining a 150 mAh flexible Li-ion battery and a flexible antenna (center frequency of 915 MHz). In general, the CMOS-logic high-speed CNT ICs showed outstanding energy efficiency and thus may potentially advance the application of CNT-based electronics.

Scalable Preparation of High-Density Semiconducting Carbon Nanotube Arrays for High-Performance Field-Effect Transistors.

Although chemical vapor deposition (CVD)-grown carbon nanotube (CNT) arrays are considered ideal materials for constructing high-performance field-effect transistors (FETs) and integrated circuits (ICs), a significant gap remains between the required and achieved densities and purities of CNT arrays. Here, we develop a directional shrinking transfer method to realize up to 10-fold density amplification of CNT array films without introducing detectable damage or defects. In addition, the method improves the film uniformity while retaining the perfect alignment and high carrier mobility of 1600 cm2 V-1 s-1 of CVD-grown CNT arrays. By combining the density amplification method with the thermocapillary flow method developed by Rogers et al., semiconducting CNT arrays with high densities and high qualities are obtained. High-performance FETs with a channel length of 200 nm are demonstrated using these high-density semiconducting CNT arrays, yielding a record-high on-state current density of 150 µA/µm, a peak transconductance of 80 µS/µm, and a current on/off ratio of more than 104 among the CVD-grown CNT-based FETs.