Coin-sized, fully integrated, and minimally invasive continuous glucose monitoring system based on organic electrochemical transistors.

Continuous glucose monitoring systems (CGMs) are critical toward closed-loop diabetes management. The field's progress urges next-generation CGMs with enhanced antinoise ability, reliability, and wearability. Here, we propose a coin-sized, fully integrated, and wearable CGM, achieved by holistically synergizing state-of-the-art interdisciplinary technologies of biosensors, minimally invasive tools, and hydrogels. The proposed CGM consists of three major parts: (i) an emerging biochemical signal amplifier, the organic electrochemical transistor (OECT), improving the signal-to-noise ratio (SNR) beyond traditional electrochemical sensors; (ii) a microneedle array to facilitate subcutaneous glucose sampling with minimized pain; and (iii) a soft hydrogel to stabilize the skin-device interface. Compared to conventional CGMs, the OECT-CGM offers a high antinoise ability, tunable sensitivity and resolution, and comfort wearability, enabling personalized glucose sensing for future precision diabetes health care. Last, we discuss how OECT technology can help push the limit of detection of current wearable electrochemical biosensors, especially when operating in complicated conditions.

All-Photolithography Fabrication of Ion-Gated Flexible Organic Transistor Array for Multimode Neuromorphic Computing.

Organic ion-gated transistors (OIGTs) demonstrate commendable performance for versatile neuromorphic systems. However, due to the fragility of organic materials to organic solvents, efficient and reliable all-photolithography methods for scalable manufacturing of high-density OIGT arrays with multimode neuromorphic functions are still missing, especially when all active layers are patterned in high-density. Here, a flexible high-density (9662 devices per cm2 ) OIGT array with high yield and minimal device-to-device variation is fabricated by a modified all-photolithography method. The unencapsulated flexible array can withstand 1000 times' bending at a radius of 1 mm, and 3 months' storage test in air, without obvious performance degradation. More interesting, the OIGTs can be configured between volatile and nonvolatile modes, suitable for constructing reservoir computing systems to achieve high accuracy in classifying handwritten digits with low training costs. This work proposes a promising design of organic and flexible electronics for affordable neuromorphic systems, encompassing both array and algorithm aspects.

Organic High-Temperature Synaptic Phototransistors for Energy-Efficient Neuromorphic Computing.

Organic optoelectronic synaptic devices that can reliably operate in high-temperature environments (i.e., beyond 121°C) or remain stable after high-temperature treatments have significant potential in biomedical electronics and bionic robotic engineering. However, it is challenging to acquire this type of organic devices considering the thermal instability of conventional organic materials and the degradation of photoresponse mechanisms at high temperatures. Here, high-temperature synaptic phototransistors (HTSPs) based on thermally stable semiconductor polymer blends as the photosensitive layer are developed, successfully simulating fundamental optical-modulated synaptic characteristics at a wide operating temperature range from room temperature to 220°C. Robust optoelectronic performance can be observed in HTSPs even after experiencing 750 h of the double 85 testing due to the enhanced operational reliability. Using HTSPs, Morse-code optical decoding scheme and the visual object recognition capability are also verified at elevated temperatures. Furthermore, flexible HTSPs are fabricated, demonstrating an ultralow power consumption of 12.3 aJ per synaptic event at a low operating voltage of -0.05 mV. Overall, the conundrum of achieving reliable optical-modulated neuromorphic applications while balancing low power consumption can be effectively addressed. This research opens up a simple but effective avenue for the development of high-temperature and energy-efficient wearable optoelectronic devices in neuromorphic computing applications.

Stretchable and neuromorphic transistors for pain perception and sensitization emulation.

Pain perception nociceptors (PPN), an important type of sensory neuron, are capable of sending out alarm signals when the human body is exposed to destructive stimuli. Simulating the human ability to perceive the external environment and spontaneously avoid injury is a critical function of neural sensing of artificial intelligence devices. The demand for developing artificial PPN has subsequently increased. However, due to the application scenarios of bionic electronic devices such as human skin, electronic prostheses, and robot bodies, where a certain degree of surface deformation constantly occurs, the ideal artificial PPN should have the stretchability to adapt to real scenarios. Here, an organic semiconductor nanofiber artificial pain perception nociceptor (NAPPN) based on a pre-stretching strategy is demonstrated to achieve key pain aspects such as threshold, sensitization, and desensitization. Remarkably, while stretching up to 50%, the synaptic behaviors and injury warning ability of NAPPN can be retained. To verify the wearability of the device, NAPPN was attached to a curved human finger joint, on which PPN behaviors were successfully mimicked. This provides a promising strategy for realizing neural sensing function on either deformed or mobile electronic devices.

Achieving tissue-level softness on stretchable electronics through a generalizable soft interlayer design.

Soft and stretchable electronics have emerged as highly promising tools for biomedical diagnosis and biological studies, as they interface intimately with the human body and other biological systems. Most stretchable electronic materials and devices, however, still have Young's moduli orders of magnitude higher than soft bio-tissues, which limit their conformability and long-term biocompatibility. Here, we present a design strategy of soft interlayer for allowing the use of existing stretchable materials of relatively high moduli to versatilely realize stretchable devices with ultralow tissue-level moduli. We have demonstrated stretchable transistor arrays and active-matrix circuits with moduli below 10 kPa-over two orders of magnitude lower than the current state of the art. Benefiting from the increased conformability to irregular and dynamic surfaces, the ultrasoft device created with the soft interlayer design realizes electrophysiological recording on an isolated heart with high adaptability, spatial stability, and minimal influence on ventricle pressure. In vivo biocompatibility tests also demonstrate the benefit of suppressing foreign-body responses for long-term implantation. With its general applicability to diverse materials and devices, this soft-interlayer design overcomes the material-level limitation for imparting tissue-level softness to a variety of bioelectronic devices.

Emerging Iontronic Neural Devices for Neuromorphic Sensory Computing.

Living organisms have a very mysterious and powerful sensory computing system based on ion activity. Interestingly, studies on iontronic devices in the past few years have proposed a promising platform for simulating the sensing and computing functions of living organisms, because: 1) iontronic devices can generate, store, and transmit a variety of signals by adjusting the concentration and spatiotemporal distribution of ions, which analogs to how the brain performs intelligent functions by alternating ion flux and polarization; 2) through ionic-electronic coupling, iontronic devices can bridge the biosystem with electronics and offer profound implications for soft electronics; 3) with the diversity of ions, iontronic devices can be designed to recognize specific ions or molecules by customizing the charge selectivity, and the ionic conductivity and capacitance can be adjusted to respond to external stimuli for a variety of sensing schemes, which can be more difficult for electron-based devices. This review provides a comprehensive overview of emerging neuromorphic sensory computing by iontronic devices, highlighting representative concepts of both low-level and high-level sensory computing and introducing important material and device breakthroughs. Moreover, iontronic devices as a means of neuromorphic sensing and computing are discussed regarding the pending challenges and future directions.

Stretchable Redox-Active Semiconducting Polymers for High-Performance Organic Electrochemical Transistors.

Organic electrochemical transistors (OECTs) represent an emerging device platform for next-generation bioelectronics owing to the uniquely high amplification and sensitivity to biological signals. For achieving seamless tissue-electronics interfaces for accurate signal acquisition, skin-like softness and stretchability are essential requirements, but they have not yet been imparted onto high-performance OECTs, largely due to the lack of stretchable redox-active semiconducting polymers. Here, a stretchable semiconductor is reported for OECT devices, namely poly(2-(3,3'-bis(2-(2-(2-methoxyethoxy)ethoxy)ethoxy)-[2,2'-bithiophen]-5)yl thiophene) (p(g2T-T)), which gives exceptional stretchability over 200% strain and 5000 repeated stretching cycles, together with OECT performance on par with the state-of-the-art. Validated by systematic characterizations and comparisons of different polymers, the key design features of this polymer that enable the combination of high stretchability and high OECT performance are a nonlinear backbone architecture, a moderate side-chain density, and a sufficiently high molecular weight. Using this highly stretchable polymer semiconductor, an intrinsically stretchable OECT is fabricated with high normalized transconductance (≈223 S cm-1 ) and biaxial stretchability up to 100% strain. Furthermore, on-skin electrocardiogram (ECG) recording is demonstrated, which combines built-in amplification and unprecedented skin conformability.

A stretchable and strain-unperturbed pressure sensor for motion interference-free tactile monitoring on skins.

A stretchable pressure sensor is a necessary tool for perceiving physical interactions that take place on soft/deformable skins present in human bodies, prosthetic limbs, or soft robots. However, all existing types of stretchable pressure sensors have an inherent limitation, which is the interference of stretching with pressure sensing accuracy. Here, we present a design for a highly stretchable and highly sensitive pressure sensor that can provide unaltered sensing performance under stretching, which is realized through the synergistic creations of an ionic capacitive sensing mechanism and a mechanically hierarchical microstructure. Via this optimized structure, our sensor exhibits 98% strain insensitivity up to 50% strain and a low pressure detection limit of 0.2 Pa. With the capability to provide all the desired characteristics for quantitative pressure sensing on a deformable surface, this sensor has been used to realize the accurate sensation of physical interactions on human or soft robotic skin.

Retina-Inspired Organic Heterojunction-Based Optoelectronic Synapses for Artificial Visual Systems.

For the realization of retina-inspired neuromorphic visual systems which simulate basic functions of human visual systems, optoelectronic synapses capable of combining perceiving, processing, and memorizing in a single device have attracted immense interests. Here, optoelectronic synaptic transistors based on tris(2-phenylpyridine) iridium (Ir(ppy)3) and poly(3,3-didodecylquarterthiophene) (PQT-12) heterojunction structure are presented. The organic heterojunction serves as a basis for distinctive synaptic characteristics under different wavelengths of light. Furthermore, synaptic transistor arrays are fabricated to demonstrate their optical perception efficiency and color recognition capability under multiple illuminating conditions. The wavelength-tunability of synaptic behaviors further enables the mimicry of mood-modulated visual learning and memorizing processes of humans. More significantly, the computational dynamics of neurons of synaptic outputs including associated learning and optical logic functions can be successfully demonstrated on the presented devices. This work may locate the stage for future studies on optoelectronic synaptic devices toward the implementation of artificial visual systems.

Highly sensitive 2D organic field-effect transistors for the detection of lithium-ion battery electrolyte leakage.

Lithium ion batteries (LIBs) have become indispensable in daily life. Here, we fabricated a broad range of polymer semiconductor films as thin as 2 nm via a standard spin-coating method, and utilized the resulting organic transistors for the detection of LIB electrolytes, which can give an early warning signal before LIB failure.

Organic synaptic devices based on ionic gel with reduced leakage current.

In this work, we presented a solid-state hybrid electrolyte dielectric film fabricated by a facile solution process, composed of ionic liquid and high-k polymers for leakage current reduction. With ions involved in the dielectric, the organic transistor can be operated under low voltage, and some essential synaptic behaviors were successfully simulated by the electrostatic coupling effect for building neuromorphic computing systems.

Perovskite/Organic Semiconductor-Based Photonic Synaptic Transistor for Artificial Visual System.

Artificial visual system with information sensing, processing, and memory function is promoting the development of artificial intelligence techniques. Photonic synapse as an essential component can enhance the visual information processing efficiency owing to the high propagation speed, low latency, and large bandwidth. Herein, photonic synaptic transistors based on organic semiconductor poly[2,5-(2-octyldodecyl)-3,6-diketopyrrolopyrrole-alt-5,5-(2,5-di(thien-2-yl)thieno [3,2-b]thiophene)] (DPPDTT) and perovskite CsPbBr3 quantum dots are fabricated by a simple solution process. The device can simulate fundamental synaptic behaviors, including excitatory postsynaptic current, pair-pulse facilitation, the transition of short-term memory to long-term memory, and "learning experience" behavior. Combining the advantages of the high photosensitivity of perovskites and relatively high conductivity of DPPDTT, the device can exhibit excellent synaptic performances at a low voltage of -0.2 V. Even under an ultralow operation voltage of -0.0005 V, the device can still show obvious synaptic responses. Tunable synaptic integration behaviors including "AND" and "OR" light logic functions can be realized. An artificial visual system is successfully emulated by illuminating the synaptic arrays employing light of different densities. Therefore, low-voltage synaptic devices based on organic semiconductor and CsPbBr3 quantum dots with a simple fabrication technique present high potential to mimic human visual memory.

Flexible Capacitive Humidity Sensors Based on Ionic Conductive Wood-Derived Cellulose Nanopapers.

With the growing requirements for the renewability and sustainability of electronic products, environmentally friendly cellulose-based materials have attracted immense research interests and gained increasing prominence for electronic devices. Humidity sensors play an essential role in industries, agriculture, climatology, medical services, and daily life. Here, for the first time, we fabricate capacitive humidity sensors based on ionic conductive wood-derived cellulose nanopapers (WCNs). The WCN-based humidity sensors exhibited ultrahigh sensitivity, fast response, small hysteresis, and more importantly, a wide working range of relative humidity (RH). The sensors showed >104 times increase in the sensing signal over the 7-94% RH range at 20 Hz, while many reported humidity sensors with high sensitivity often have the working range limited to high RH levels. Our sensors can realize the distinction of nuances in humidity and exhibit outstanding noncontact skin humidity sensing properties. Flexible WCN-based humidity sensors were also fabricated, and they displayed excellent sensing properties with long-time stability, endowing them with multifunctional applications. The contrast humidity sensing experiment compared to the existing commercial humidity sensor further demonstrated the higher and faster response of our WCN-based sensors. Thus, this work provides effective guidance for the design of high-performance humidity sensors using nanopapers and opens a new dimension for a variety of future applications.

Bioinspired Multifunctional Organic Transistors Based on Natural Chlorophyll/Organic Semiconductors.

Inspired by the photosynthesis process of natural plants, multifunctional transistors based on natural biomaterial chlorophyll and organic semiconductors (OSCs) are reported. Functions as photodetectors (PDs) and light-stimulated synaptic transistors (LSSTs) can be switched by gate voltage. As PDs, the devices exhibit ultrahigh photoresponsivity up to 2 × 106 A W-1 , detectivity of 6 × 1015 Jones, and Iphoto /Idark ratio of 2.7 × 106 , which make them among the best reported organic PDs. As LSSTs, important synaptic functions similar to biological synapses are demonstrated, together with a dynamic learning and forgetting process and image-processing function. Significantly, benefiting from the ultrahigh photosensitivity of chlorophyll, the lowest operating voltage and energy consumption of the LSSTs can be 10-5 V and 0.25 fJ, respectively. The devices also exhibit high flexibility and long-term air stability. This work provides a new guide for developing organic electronics based on natural biomaterials.

The Design of 3D-Interface Architecture in an Ultralow-Power, Electrospun Single-Fiber Synaptic Transistor for Neuromorphic Computing.

Synaptic electronics is a new technology for developing functional electronic devices that can mimic the structure and functions of biological counterparts. It has broad application prospects in wearable computing chips, human-machine interfaces, and neuron prostheses. These types of applications require synaptic devices with ultralow energy consumption as the effective energy supply for wearable electronics, which is still very difficult. Here, artificial synapse emulation is demonstrated by solid-ion gated organic field-effect transistors (OFETs) with a 3D-interface conducting channel for ultralow-power synaptic simulation. The basic features of the artificial synapse, excitatory postsynaptic current (EPSC), paired-pulse facilitation (PPF), and high-pass filtering, are successfully realized. Furthermore, the single-fiber based artificial synapse can be operated by an ultralow presynaptic spike down to -0.5 mV with an ultralow reading voltage at -0.1 mV due to the large contact surface between the ionic electrolyte and fiber-like semiconducting channel. Therefore, the ultralow energy consumption at one spike of the artificial synapse can be realized as low as ≈3.9 fJ, which provides great potential in a low-power integrated synaptic circuit.

Light-Stimulated Synaptic Transistors Fabricated by a Facile Solution Process Based on Inorganic Perovskite Quantum Dots and Organic Semiconductors.

Implementation of artificial intelligent systems with light-stimulated synaptic emulators may enhance computational speed by providing devices with high bandwidth, low power computation requirements, and low crosstalk. One of the key challenges is to develop light-stimulated devices that can response to light signals in a neuron-/synapse-like fashion. A simple and effective solution process to fabricate light-stimulated synaptic transistors (LSSTs) based on inorganic halide perovskite quantum dots (IHP QDs) and organic semiconductors (OSCs) is reported. Blending IHP QDs and OSCs not only improves the charge separation efficiency of the photoexcited charges, but also induces delayed decay of the photocurrent in the IHP QDs/OSCs hybrid film. The enhanced charge separation efficiency results in high photoresponsivity, while the induced delayed decay of the photocurrent is critical to achieving light-stimulating devices with a memory effect, which are important for achieving high synaptic performance. The LSSTs can respond to light signals in a highly neuron-/synapse-like fashion. Both short-term and long-term synaptic behaviors have been realized, which may lay the foundation for the future implementation of artificial intelligent systems that are enabled by light signals. More significantly, LSSTs are fabricated by a facile solution process which can be easily applied to large-scale samples.

Wood-Derived Nanopaper Dielectrics for Organic Synaptic Transistors.

The use of biocompatible and biodegradable materials in electronic devices can be an important trend in the development of the next-generation green electronics. In addition, by integrating the advantages of low power consumption, low-cost processing, and flexibility, organic synaptic devices will be promising elements for the construction of brain-inspired computers. However, previously reported electrolyte-gated synaptic transistors are mainly made of non-biocompatible and non-biodegradable electrolytes. Woods are widely considered as one kind of sustainable and renewable materials. We found that wood-derived cellulose nanopapers have ionic conductivity and, therefore, can be used as dielectric materials for organic synaptic transistors. The fabricated wood-derived cellulose nanopapers exhibit decent ionic conductivity of 7.3 × 10-4 S m-1 and a high lateral coupling effective capacitance of 18.65 nF cm-2 at 30 Hz. The laterally coupled organic synaptic transistors using wood-derived cellulose nanopapers as the dielectric layer present excellent transistor performances at the operating voltage below 1.5 V. More significantly, some important synaptic behaviors, such as excitatory postsynaptic current, signal-filtering characteristics, and dendritic integration are successfully simulated in our synaptic transistors. Because the development of electronic devices with biocompatible and biodegradable materials is essential, this work may inspire new directions for the development of "green" neuromorphic electronics.

A flexible ionic synaptic device and diode-based aqueous ion sensor utilizing asymmetric polyelectrolyte distribution.

This work reported the development of an ionic diode of high rectification ratio with a simple device structure and a quick fabrication process by utilizing asymmetric polyelectrolyte distribution. Detection of aqueous ions was demonstrated by applying this diode as a pH sensor. Two terminal ionic synaptic devices utilizing a similar structural design were also successfully developed.

Intrinsically ionic conductive cellulose nanopapers applied as all solid dielectrics for low voltage organic transistors.

Biodegradability, low-voltage operation, and flexibility are important trends for the future organic electronics. High-capacitance dielectrics are essential for low-voltage organic field-effect transistors. Here we report the application of environmental-friendly cellulose nanopapers as high-capacitance dielectrics with intrinsic ionic conductivity. Different with the previously reported liquid/electrolyte-gated dielectrics, cellulose nanopapers can be applied as all-solid dielectrics without any liquid or gel. Organic field-effect transistors fabricated with cellulose nanopaper dielectrics exhibit good transistor performances under operation voltage below 2 V, and no discernible drain current change is observed when the device is under bending with radius down to 1 mm. Interesting properties of the cellulose nanopapers, such as ionic conductivity, ultra-smooth surface (~0.59 nm), high transparency (above 80%) and flexibility make them excellent candidates as high-capacitance dielectrics for flexible, transparent and low-voltage electronics.

Light-Stimulated Synaptic Devices Utilizing Interfacial Effect of Organic Field-Effect Transistors.

Synaptic transistors stimulated by light waves or photons may offer advantages to the devices, such as wide bandwidth, ultrafast signal transmission, and robustness. However, previously reported light-stimulated synaptic devices generally require special photoelectric properties from the semiconductors and sophisticated device's architectures. In this work, a simple and effective strategy for fabricating light-stimulated synaptic transistors is provided by utilizing interface charge trapping effect of organic field-effect transistors (OFETs). Significantly, our devices exhibited highly synapselike behaviors, such as excitatory postsynaptic current (EPSC) and pair-pulse facilitation (PPF), and presented memory and learning ability. The EPSC decay, PPF curves, and forgetting behavior can be well expressed by mathematical equations for synaptic devices, indicating that interfacial charge trapping effect of OFETs can be utilized as a reliable strategy to realize organic light-stimulated synapses. Therefore, this work provides a simple and effective strategy for fabricating light-stimulated synaptic transistors with both memory and learning ability, which enlightens a new direction for developing neuromorphic devices.