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Porous structures and micropatterning surfaces play a crucial role in the development of highly sensitive force sensors. However, achieving these two conductive architectures typically requires the synthesis of complex materials and expensive manufacturing processes. In this study, we introduce a novel conductive composite film featuring a microporous/micropyramid hybrid conductive architecture, which is achieved through a straightforward process of materials mixing and one-step screen printing. By utilizing a deep eutectic solvent in the ink component, micropores are induced in the printed composite, while the mesh of the screen mask acts as a template, resulting in a micropyramid film surface. We have successfully realized highly sensitive flexible force sensors (0.15 kPa -1 ) with multifunctional capabilities for perceiving normal force and shear force.

Techniques for noninvasively acquiring the vital information of infants and young children are considered very useful in the fields of healthcare and medical care. An unobstructive measurement method for sleeping infants and young children under the age of 6 years using a sheet-type vital sensor with a polyvinylidene fluoride (PVDF) pressure-sensitive layer is demonstrated. The signal filter conditions to obtain the ballistocardiogram (BCG) and phonocardiogram (PCG) are discussed from the waveform data of infants and young children. The difference in signal processing conditions was caused by the physique of the infants and young children. The peak-to-peak interval (PPI) extracted from the BCG or PCG during sleep showed an extremely high correlation with the R-to-R interval (RRI) extracted from the electrocardiogram (ECG). The vital changes until awakening in infants monitored using a sheet sensor were also investigated. In infants under one year of age that awakened spontaneously, the distinctive vital changes during awakening were observed. Understanding the changes in the heartbeat and respiration signs of infants and young children during sleep is essential for improving the accuracy of abnormality detection by unobstructive sensors.

We present a high-performance flexible bending strain sensor for directional motion detection of human hands and soft robotic grippers. The sensor was fabricated using a printable porous conductive composite composed of polydimethylsiloxane (PDMS) and carbon black (CB). The utilization of a deep eutectic solvent (DES) in the ink formulation induced a phase segregation between the CB and PDMS and led to a porous structure inside the printed films after being vapored. This simple and spontaneously formed conductive architecture provided superior directional bend-sensing characteristics compared to conventional random composites. The resulting flexible bending sensors displayed high bidirectional sensitivity (gauge factor of 45.6 under compressive bending and 35.2 under tensile bending), negligible hysteresis, good linearity (>0.99), and excellent bending durability (over 10,000 cycles). The multifunctional applications of these sensors, including human motion detection, object-shape monitoring, and robotic perceptions, are demonstrated as a proof-of-concept.

Organic thin-film transistors (TFTs) with an electrochemically functionalized sensing gate are promising platforms for wearable health-monitoring technologies because they are light, flexible, and cheap. Achieving both high sensitivity and low power is highly demanding for portable or wearable devices. In this work, we present flexible printed dual-gate (DG) organic TFTs operating in the subthreshold regime with ultralow power and high sensitivity. The subthreshold operation of the gate-modulated TFT-based sensors not only increases the sensitivity but also reduces the power consumption. The DG configuration has deeper depletion and stronger accumulation, thereby further making the subthreshold slope sharper. We integrate an enzymatic lactate-sensing extended-gate electrode into the printed DG TFT and achieve exceptionally high sensitivity (0.77) and ultralow static power consumption (10 nW). Our sensors are successfully demonstrated in physiological lactate monitoring with human saliva. The accuracy of the DG TFT sensing system is as good as that of a high-cost conventional assay. The developed platform can be readily extended to various materials and technologies for high performance wearable sensing applications., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier B.V. All rights reserved.)

Source-gated transistors (SGTs) are emerging devices enabling high-gain single-stage amplifiers with low complexity. To date, the p-type printed organic SGT (OSGT) has been developed and showed high gain and low power consumption. However, complementary OSGT circuits remained impossible because of the lack of n-type OSGTs. Here, we show the first n-type OSGTs, which are printed and have a high intrinsic gain over 40. A Schottky source contact is intentionally formed between an n-type organic semiconductor, poly{[N,N'-bis(2-octyldodecyl)naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5'-(2,2'-bithiophene)} (N2200), and the silver electrode. In addition, a blocking layer at the edge of the source electrode plays an important role to improve the saturation characteristics and increase the intrinsic gain. Such n-type printed OSGTs and complementary circuits based on them are promising for flexible and wearable electronic devices such as for physiological and biochemical health monitoring.

This is the first report of conducting proof-of-concept study for amperometric acetyltransferase-based L-carnitine sensor by employing the thiol/disulfide exchange reaction. The carnitine acetyltransferase (CrAT) catalyzes the reaction between acetyl-CoA and L-carnitine to produce CoA which is difficult to detect directly by electrochemical methods owing to steric hindrance and electrostatic effect of CoA. The thiol/disulfide exchange reaction between CoA and cystamine was mediated in the enzymatic reaction to produce electrochemically detectable low molecular weight of cationic cysteamine. The sensor exhibited high sensitivity and selectivity for L-carnitine in the concentration range 0.28-50 µM with a limit of detection of 0.28 µM. This is a promising strategy for L-carnitine sensing in point-of-care testing applications., (© 2022. The Author(s), under exclusive licence to The Japan Society for Analytical Chemistry.)

In the emerging Internet of Things (IoT) society, there is a significant need for low-cost, high-performance flexible humidity sensors in wearable devices. However, commercially available humidity sensors lack flexibility or require expensive and complex fabrication methods, limiting their application and widespread use. We report a high-performance printed flexible humidity sensor using a cellulose nanofiber/carbon black (CNF/CB) composite. The cellulose nanofiber enables excellent dispersion of carbon black, which facilitates the ink preparation and printing process. At the same time, its hydrophilic and porous nature provides high sensitivity and fast response to humidity. Significant resistance changes of 120% were observed in the sensor at humidity ranging from 30% RH to 90% RH, with a fast response time of 10 s and a recovery time of 6 s. Furthermore, the developed sensor also exhibited high-performance uniformity, response stability, and flexibility. A simple humidity detection device was fabricated and successfully applied to monitor human respiration and noncontact fingertip moisture as a proof-of-concept.

Digital inkjet printing (IJP) can greatly reduce the manufacturing cost and waste of flexible large-area electronics by adding micro-fine patterns onto plastic foils. Advanced system design using IJP has been limited by the lack of an electronic design automation (EDA) approach. An EDA approach based on a vector-based layout drawing requires parameterized IJP design rules. This study proposes a layout-to-bitmap (L2B) conversion procedure and line-based design rules that leverage the existing circuit layout EDA tools for advanced IJP designs. The L2B conversion is accomplished by optimizing the parameters of the horizontal and vertical lines by varying the drop spacings and platen temperatures. Next, the line-based layouts are converted to bitmap files which are used as IJP input data for printing multiple metal layers. This study systematically investigated the development of an IJP process employing Ag nanoparticles. The physical characteristics of the proposed process were evaluated based on theories concerning inkjet-printed bead formation. The design rules for fabricating printed thin-film transistor (TFT) circuits were documented. Documentation is the first step in creating an IJP process design kit for advanced electronics design. Using the optimized L2B conversion procedure and the design rules, a 10 × 10 array of printed organic TFTs was fabricated to demonstrate the reliability of the developed process. Additionally, the fabricated printed organic TFTs indicated that the proposed process could be extended to large-scale system designs.

This is the first report demonstrating proof of concept for the passive, non-invasive extraction and in situ potentiometric detection of human sweat chloride ions (Cl - ions) using a stable printed planar liquid-junction reference electrode-integrated hydrogel-based touch-sensor pad without activities such as exercise to induce perspiration, environmental temperature control, or requiring cholinergic drug administration. The sensor pad was composed entirely of a screen-printed bare Ag/AgCl-based chloride ion-selective electrode and a planar liquid-junction Ag/AgCl reference electrode, which were fully covered by an agarose hydrogel in phosphate-buffered saline (PBS). When human skin contacted the hydrogel pad, sweat Cl - ions were continuously extracted into the gel, followed by in situ potentiometric detection. The planar liquid-junction Ag/AgCl reference electrode had a polymer-based KCl-saturated inner electrolyte layer to stabilize the potential of the Ag/AgCl electrode even with a substantial change in the chloride ion concentration in the hydrogel pad. We expect this fully screen-printed sensor to achieve the low-cost passive and non-invasive daily monitoring of human Cl - ions in sweat in the future.

Controlling the molecular orientation of materials is a key issue for improving the performance of organic semiconductor devices. Herein, we demonstrate the structure-property relationships of iodinated and noniodinated molecules based on an asymmetric thienoacene framework. The noniodinated molecule formed an antiparallel slip-stack structure with small orbital overlap between molecules. In contrast, the iodinated molecule formed a head-to-head layered-herringbone structure, and as a result, the transfer integrals became larger and the hole mobility increased significantly compared with the noniodinated material. The iodinated molecule was made into a stable and solution-processable p-type organic semiconductor with a mobility of 2.2 cm 2 V -1 s -1 , which was 2 orders of magnitude higher than that of the noniodinated molecule. This study reveals that controlling molecular orientations using iodine-iodine interactions is a promising strategy for accelerating the development of organic semiconductor materials.

This report is the first on heat-assisted transferable battery components, enabling manufacturing batteries on non-planer surfaces such as a curved surface and an edge. The transferrable battery components were composed of two layers: a cathode or an anode and a conductive heal-melt adhesive layer on a silicone-based flexible supporting paper. These mechanically-durable, flexible components enabled conformable adhesion even on curved surfaces and substrate edges. As a model battery, the manganese dioxide-zinc system was constructed on a curved surface using transfer techniques and showed a practical capacity of 1.8 mAh cm -2 per unit electrode area. These transferable electrodes allow arbitrary design of batteries according to the power consumption of IoT devices to be fabricated on unreported geometries where has been considered as a dead space.

The application of a multienzyme cascade reaction in electrochemical biosensors has the advantage of expanding the target substrates in addition to selectivity combining multiple enzymes on an electrode. However, the multienzyme system has the drawback of inefficient substance conversion because of the time-consuming passing of intermediates between the enzymes and/or diffusional loss of the intermediates. In this study, the optimal construction of a multienzymatic film in an ammonia detection sensor was investigated using a cascade reaction of l-glutamate oxidase and l-glutamate dehydrogenase as a model sensor. Three enzymatic films were prepared: (1) a mixed film designed to have a short diffusional distance between closely located enzymes, (2) a normal-sequential layered film arranged for the correct reaction pathway, and (3) a reverse-sequential layered film as a negative control. This was followed by comparison of the conversion efficiency of ammonia to hydrogen peroxide using time-dependent potentiometric measurements of a Prussian blue electrode determining the hydrogen peroxide amount. The results indicate that the conversion efficiency of the normal-sequential layered film was the highest among the three enzymatic films. The quantitative evaluation of the intermediate conversion efficiency of the cascade reaction showed that compared to the mixed film (34%), a higher conversion efficiency of 92% was obtained in the first enzymatic reaction step. These findings will promote the use of multienzymatic cascade reaction systems not only in biosensors and bioreactors but also in various industrial fields., Competing Interests: The authors declare no competing financial interest., (© 2020 The Authors. Published by American Chemical Society.)

We successfully demonstrated a detailed and systematic enhancement of organic field effect transistors (OFETs) performance using dithienothiophene (DTT) and furan-flanked diketopyrrolopyrrole based donor-acceptor conjugated polymer semiconductor namely PDPPF-DTT as an active semiconductor. The self-assembled monolayers (SAMs) treatments at interface junctions of the semiconductor-dielectric and at the semiconductor-metal electrodes has been implemented using bottom gate bottom contact device geometry. Due to SAM treatment at the interface using tailored approach, the significant reduction of threshold voltage (V th ) from - 15.42 to + 5.74 V has been observed. In addition to tuning effect of V th , simultaneously charge carrier mobility (µ FET ) has been also enhanced the from 9.94 × 10 -4 cm 2 /Vs to 0.18 cm 2 /Vs. In order to calculate the trap density in each OFET device, the hysteresis in transfer characteristics has been studied in detail for bare and SAM treated devices. Higher trap density in Penta-fluoro-benzene-thiol (PFBT) treated OFET devices enhances the gate field, which in turn controls the charge carrier density in the channel, and hence gives lower V th  = + 5.74 V. Also, PFBT treatment enhances the trapped interface electrons, which helps to enhance the mobility in this OFET architecture. The overall effect has led to possibility of reduction in the V th with simultaneous enhancements of µ FET in OFETs, following systematic device engineering methodology.

Organic transistors are promising platforms for wearable biosensors. However, the strategies to improve signal amplification have yet to be determined, particularly regarding biosensors that generate very weak signals. In this study, an organic voltage amplifier is presented for a lactate sensor on flexible plastic foil. The preamplifier is based on a 3D complementary inverter, which is achieved by vertically stacking complementary transistors with a shared gate between them. The shared gate is extended and functionalized with a lactate oxidase enzyme to detect lactate. The sensing device successfully detects the lactate concentration in the human sweat range (20-60 mm) with high sensitivity (6.82 mV mm -1 ) due to high gain of its amplification. The 3D integration process is cost-effective as it is solution-processable and doubles the number of transistors per unit area. The device presented in this study would pave the way for the development of high-gain noninvasive sweat lactate sensors that can be wearable., (© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Tactile sensing, particularly the detection of object slippage, is required for skillful object handling by robotic grippers. The real-time measurement and identification of the dynamic shear forces that result from slippage events are crucial for slip detection and effective object interaction. In this study, a ferroelectric polymer-based printed soft sensor for object slippage detection was developed and fabricated by screen printing. The proposed sensor demonstrated a sensitivity of 8.2 μC·cm -2 and was responsive to shear forces applied in both the parallel and perpendicular directions. An amplifier circuit, based on a printed organic thin-film transistor, was applied and achieved a high sensitivity of 0.1 cm 2 /V·s. Therefore, this study experimentally demonstrates the effectiveness of the proposed printable high-sensitivity tactile sensor, which could serve as part of a wearable robotic e-skin. The sensor could facilitate the production of a system to detect and prevent the slippage of objects from robotic grippers.

There are few reports on resistive strain sensors that exhibit both high sensitivity and a wide working range under stretching. We have newly developed a high-performance strain sensor based on a brittle-stretchable conductive network that consists of both brittle and stretchable conductive layers and is fabricated on a stretchable substrate using the screen-printing method. Adding strain usually generates structural cracks in brittle conductive layers leading to a significant increase in resistance, while a stretchable conductive layer bridges these cracks to maintain the conductive pathways under high-strain conditions. This novel conductive network endows superior electrical-mechanical performance to the strain sensors, which possess high sensitivity (gauge factor > 870) over the entire working range (∼100%). Additionally, the developed sensors showed unique anisotropic bend-sensing characteristics, which could be used to detect the bending directions. This high degree of comprehensive performance results in a strain sensor with the capability for full-range human motion detection and robotic motion sensing.

This review describes recent advances in biosensors for non-invasive human healthcare applications, especially focusing on sweat analysis, along with approaches for fabricating these biosensors based on printed electronics technology. Human sweat contains various kinds of biomarkers. The relationship between a trace amount of sweat biomarkers partially partitioned from blood and diseases has been investigated by omic analysis. Recent progress in wearable or portable biosensors has enabled periodic or continuous monitoring of some sweat biomarkers while supporting the results of the omic analysis. In this review, we particularly focused on a transistor-based biosensor that is highly sensitive in quantitatively detecting the low level of sweat biomarkers. Furthermore, we showed a new approach of flexible hybrid electronics that has been applied to advanced sweat biosensors to realize fully integrated biosensing systems wirelessly connected to a networked IoT system. These technologies are based on uniquely advanced printing techniques that will facilitate mass fabrication of high-performance biosensors at low cost for future smart healthcare.

Facile fabrication and high ambient stability are strongly desired for the practical application of temperautre sensor in real-time wearable healthcare. Herein, a fully printed flexible temperature sensor based on cross-linked poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) was developed. By introducing the crosslinker of (3-glycidyloxypropyl)trimethoxysilane (GOPS) and the fluorinated polymer passivation (CYTOP), significant enhancements in humidity stability and temperature sensitivity of PEDOT:PSS based film were achieved. The prepared sensor exhibited excellent stability in environmental humidity ranged from 30% RH to 80% RH, and high sensitivity of -0.77% °C -1 for temperature sensing between 25 °C and 50 °C. Moreover, a wireless temperature sensing platform was obtained by integrating the printed sensor to a printed flexible hybrid circuit, which performed a stable real-time healthcare monitoring.

This study is the first report demonstrating proof-of-concept for a hydrogel-based touch sensor pad used for the non-invasive extraction and detection of sweat components. The sensor device was composed of an electrochemical L-lactate biosensor covered with an agarose gel in a phosphate buffer saline. When human skin contacts the agarose gel, L-lactate in sweat was continuously extracted into the gel, followed by in-situ potentiometric detection without controlled conditions. This novel type of sweat sensor is expected to enable the simple, non-invasive daily periodic monitoring of sweat biomarkers for advanced personal healthcare methods in the future.

A novel flexible lactate sensor based on organic field-effect transistors (OFETs) is demonstrated. Because lactate is known as a biomarker for assessing our physical performance, wearable lactate sensors could contribute to the monitoring of human health conditions. The flexible and low-voltage operatable OFET possesses an extended-gate modified with enzymes and an osmium-redox polymer for the lactate detection, meaning that the continuous measurement of lactate levels (0 - 10 mM) has been successfully achieved. We believe that insight obtained will open up opportunities for applying OFETs in wearable biosensors.

Direct printing of thin-film transistors has enormous potential for ubiquitous and lightweight wearable electronic applications. However, advances in printed integrated circuits remain very rare. Here we present a three-dimensional (3D) integration approach to achieve technology scaling in printed transistor density, analogous to Moore's law driven by lithography, as well as enhancing device performance. To provide a proof of principle for the approach, we demonstrate the scalable 3D integration of dual-gate organic transistors on plastic foil by printing with high yield, uniformity, and year-long stability. In addition, the 3D stacking of three complementary transistors enables us to propose a programmable 3D logic array as a new route to design printed flexible digital circuitry essential for the emerging applications. The 3D monolithic integration strategy demonstrated here is applicable to other emerging printable materials, such as carbon nanotubes, oxide semiconductors and 2D semiconducting materials.

The important concept of printable functional materials is about to cause a paradigm shift that we will be able to fabricate electronic devices by printing methods in air at room temperature. One of the promising applications of the printed electronics is a disposable electronic patch sensing system which can monitor the health conditions without any restraint. Operational amplifiers (OPAs) are an essential component for such sensing system, since an OPA enables a wide variety of signal processing. Here we demonstrate printed OPAs based on complementary organic semiconductor technology. They can be operated with a standard safe power source of 5 V with a minimal power consumption of 150 nW, and used as amplifiers, a variety of mathematical operators, signal converters, and oscillators. The printed micropower organic OPAs with the low voltage operation and the high versatility will open up the disposable electronic patch sensing system in near future.

We evaluated the electrochemical behaviors and reliability of printed silver (Ag) electrodes prepared from nanoparticle inks with the use of protective self-assembled monolayers (SAMs) under electronic bias conditions. The printed Ag electrodes were fabricated by inkjet printing on a hydrophobic substrate. The SAMs, which acted as barriers to moisture, were prepared by immersing the substrate in a pentafluorobenzenethiol solution at ambient temperature (25 °C). We investigated the electrochemical migration phenomenon using the water drop method, and the results showed that the formation of dendrites connecting the cathode and the anode, which can affect the electrochemical reliability of an electric device, was suppressed in the presence of the SAMs. The time before short circuit occurred was found to depend on the spacing between the electrodes, i.e., 130 s, when the distance between the electrodes was 200 μm in the presence of an SAM. We demonstrated that Ag electrodes treated using the procedure described in this work suppress the occurrence of electrical short circuits caused by Ag dendrite formation and thus their electrochemical properties are substantially improved.

Wearable sensor device technologies, which enable continuous monitoring of biological information from the human body, are promising in the fields of sports, healthcare, and medical applications. Further thinness, light weight, flexibility and low-cost are significant requirements for making the devices attachable onto human tissues or clothes like a patch. Here we demonstrate a flexible and printed circuit system consisting of an enzyme-based amperometric sensor, feedback control and amplification circuits based on organic thin-film transistors. The feedback control and amplification circuits based on pseudo-CMOS inverters were successfuly integrated by printing methods on a plastic film. This simple system worked very well like a potentiostat for electrochemical measurements, and enabled the quantitative and real-time measurement of lactate concentration with high sensitivity of 1 V/mM and a short response time of a hundred seconds.

The ability to monitor subtle changes in vital and arterial signals using flexible devices attached to the human skin can be valuable for the detection of various health conditions such as cardiovascular disease. Conventional Si device technologies are being utilised in traditional clinical systems; however, its fabrication is not easy owing to the difficulties in adapting to conventional processes. Here, we present the development of a fully printed, wearable, ferroelectric-polymer vital sensor for monitoring the human pulse wave/rate on the skin. This vital sensor is compact, thin, sufficiently flexible, and conforms to the skin while providing high pressure sensitivity, fast response time, superior operational stability, and excellent mechanical fatigue properties. Moreover, the vital sensor is connected to a communication amplifier circuit for monitoring the pulse waves with a wireless sensing system. This sensor system can realise the development of new healthcare devices for wearable sensor applications.

Electrochemical sensor systems with integrated amplifier circuits play an important role in measuring physiological signals via in situ human perspiration analysis. Signal processing circuitry based on organic thin-film transistors (OTFTs) have significant potential in realizing wearable sensor devices due to their superior mechanical flexibility and biocompatibility. Here, we demonstrate a novel potentiometric electrochemical sensing system comprised of a potassium ion (K + ) sensor and amplifier circuits employing OTFT-based pseudo-CMOS inverters, which have a highly controllable switching voltage and closed-loop gain. The ion concentration sensitivity of the fabricated K + sensor was 34 mV/dec, which was amplified to 160 mV/dec (by a factor of 4.6) with high linearity. The developed system is expected to help further the realization of ultra-thin and flexible wearable sensor devices for healthcare applications.

Mellitic triimide derivatives with N-benzyl groups form conformations with concave cavities, that are capable of including aromatic molecules such as benzene, nitrobenzene, etc. In addition, they act as supramolecular gelators, which enable the detection of aromatic molecules as a gel-sol phase transition.

The front cover artwork is provided by the group of Dr. Tsuyoshi Minami at the Institute of Industrial Science, the University of Tokyo (Japan). Easy-to-use sensing systems for on-site biomarker testing have been researched numerously, because conventional approaches for biomarker detection (e.g. enzyme linked-immunosorbent assays, etc.) are too complicated. In that regard, organic filed-effect transistors (OFETs) are some of the most promising platforms for construction of on-site testing systems. As OFETs can be easily fabricated on flexible substrates using wet processes, these are not only valuable transducers for chemo-/biosensors, but also the prospective device for rollable displays and low-cost radio frequency identification tags. Thus, the components of the sensing system could be integrated into a single chip by using OFET-based circuits. For more details, see the full text of the Communication at 10.1002/open.201700070.

We propose a novel strategy for a high-throughput sensing of metal ions using a molecular self-assembled colourimetric chemosensor array. The proposed colourimetric assay has been achieved by only using the combination of commercially available materials. Importantly, the easy-to-prepare assay can be utilised to quantitatively detect metal ions under competitive conditions.

The benchmark of soluble organic semiconductors based on acenes is the 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-PEN). However TIPS-PEN still suffers from photoinduced oxidation due to its low degree of aromaticity. Increasing the aromaticity while keeping similar optical and electrochemical properties as well as a shape suitable for good hole transport can be achieved with two-dimensional polycyclic aromatic hydrocarbons (2D-PAHs). Herein, we present an efficient synthesis and characterization of bistetracene derivatives that exhibit a band gap up to 1.71 eV and an increased stability up to 21 times compared to TIPS-PEN and mobility over 0.1 cm 2  V -1  s -1 in solution-processed organic field-effect transistors. Based on simple structural consideration, the high stability is attributed to the aromaticity of the bistetracene which is comparable to an anthrancene along each tetracene. According to Clar's sextet rule, the bistetracene should be best regarded as two anthracenes fused at the face bridged by two ethylenic spacers. The synthesis path paves the way towards the preparation of ambipolar and/or longer 2D-PAHs such as bispentacenes and could give rise to organic semiconductors with interesting properties., (© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Anthra[2,3-b]thieno[2,3-d]thiophene (ATT), which is readily accessed from thieno[3,2-b]thiophene and 2,3-naphthalenedicarboxylic anhydride, allows for selective substitution at the terminal thiophene ring, thereby providing asymmetric monoalkyl and monoalkylthienyl thienoacenes. Alkyl-substituted ATT (CnATT, n = 6, 8, 10, 12) has characteristics of a p-type field-effect transistor (FET), with mobility on the order of 0.01 cm 2 V -1 s -1 , which is the same as ATT. Conversely, alkylthienyl-substituted ATT (CnTATT, n = 6, 8, 10, 12) exhibits FET mobility of 0.15-1.9 cm 2 V -1 s -1 , which is up to 2 orders of magnitude greater than that of ATT and CnATT. Moreover, CnTATT forms crystalline thin films both by spin coating and drop casting, and C8TATT in particular exhibits a mobility of up to 1.6 cm 2 V -1 s -1 in the drop-cast film. X-ray diffraction patterns of CnTATT thin films indicate that the molecules become oriented edge-on at the substrate surface with a highly ordered structure in the in-plane direction. Accordingly, CnTATT serves as a solution-processable p-type organic field-effect transistor, where the additional thiophene ring contributes significantly to the highly ordered thin-film structure and the high carrier mobility.

We report on the mechanical fatigue behavior of printed, organic, thin-film transistors (OTFTs) based on a polymer semiconductor, investigated by repeatedly applying strain to the flexible OTFT devices and assessing their electrical characteristics after 60,000 bending cycles. As part of our investigation, we established that the rates of reduction in source/drain currents in the OTFT device depended on bending directions. Our improved understanding of the mechanical fatigue behavior of the flexible printed OTFT devices provides valuable insights into their employment in practical flexible electronics applications.

Herein, we report on the fabrication of an extended-gated organic field-effect transistor (OFET)-based immunosensor and its application in the detection of human chromogranin A (hCgA). The fabricated OFET device possesses an extended-gate electrode immobilized with an anti-CgA antibody. The titration results of hCgA showed that the electrical changes in the OFET characteristics corresponded to the glycoprotein recognition ability of the monoclonal antibody (anti-CgA). The observed sensitivity (detection limit: 0.11 µg/mL) and selectivity indicate that the OFET-based immunosensor can be potentially applied to the rapid detection of the glycoprotein concentration without any labeling., Competing Interests: The authors declare no conflict of interest.

In this paper, we demonstrate three-dimensional (3D) integrated circuits (ICs) based on a 3D complementary organic field-effect transistor (3D-COFET). The transistor-on-transistor structure was achieved by vertically stacking a p-type OFET over an n-type OFET with a shared gate joining the two transistors, effectively halving the footprint of printed transistors. All the functional layers including organic semiconductors, source/drain/gate electrodes, and interconnection paths were fully inkjet-printed except a parylene dielectric which was deposited by chemical vapor deposition. An array of printed 3D-COFETs and their inverter logic gates comprising over 100 transistors showed 100% yield, and the uniformity and long-term stability of the device were also investigated. A full-adder circuit, the most basic computing unit, has been successfully demonstrated using nine NAND gates based on the 3D structure. The present study fulfills the essential requirements for the fabrication of organic printed complex ICs (increased transistor density, 100% yield, high uniformity, and long-term stability), and the findings can be applied to realize more complex digital/analogue ICs and intelligent devices.

Printed organic thin-film transistors (OTFTs) are well suited for low-cost electronic applications, such as radio frequency identification (RFID) tags and sensors. Achieving both high carrier mobility and uniform electrical characteristics in printed OTFT devices is essential in these applications. Here, we report on printed high-performance OTFTs and circuits using silver nanoparticle inks for the source/drain electrodes and a blend of dithieno[2,3-d;2',3'-d']benzo[1,2-b;4,5-b']dithiophene (DTBDT-C 6 ) and polystyrene for the organic semiconducting layer. A high saturation region mobility of 1.0 cm 2  V -1  s -1 at low operation voltage of -5 V was obtained for relatively short channel lengths of 9 μm. All fifteen of the printed pseudo-CMOS inverter circuits were formed on a common substrate and operated at low operation voltage of 2 V with the total variation in threshold voltage of 0.35 V. Consequently, the printed OTFT devices can be used in more complex integrated circuit applications requiring low manufacturing cost over large areas.

First selective nitrate biosensor device based on an extended-gate type organic field-effect transistor (OFET) is reported. The fabricated sensor device consists of the extended-gate electrode functionalized by a nitrate reductase with a mediator (=a bipyridinium derivative) and an OFET-based transducer. The mechanism of the nitrate detection can be explained by an electron-relay on the extended-gate electrode, resulting in changes of the electric properties of the OFET. The detection limit of nitrate in water is estimated to be 45 ppb, which suggests that the sensitivity of our fabricated sensor is comparable to those of some conventional detection methods. As a practical application of the OFET sensor, the nitrate detection in diluted human saliva has been successfully demonstrated; the results agreed well with those by conventional colorimetric measurement. The advantages of OFETs are printability, mechanical flexibility, stretchability and disposability, meaning that the fabricated OFET could open up a new approach for low-cost electronic devices toward on-site detection of nitrate in aqueous media., (Copyright © 2016 Elsevier B.V. All rights reserved.)

The realization of wearable electronic devices with extremely thin and flexible form factors has been a major technological challenge. While substrates typically limit the thickness of thin-film electronic devices, they are usually necessary for their fabrication and functionality. Here we report on ultra-thin organic transistors and integrated circuits using device components whose substrates that have been removed. The fabricated organic circuits with total device thicknesses down to 350 nm have electrical performance levels close to those fabricated on conventional flexible substrates. Moreover, they exhibit excellent mechanical robustness, whereby their static and dynamic electrical characteristics do not change even under 50% compressive strain. Tests using systematically applied compressive strains reveal that these free-standing organic transistors possess anisotropic mechanical stability, and a strain model for a multilayer stack can be used to describe the strain in this sort of ultra-thin device. These results show the feasibility of ultimate-thin organic electronic devices using free-standing constructions.

Ultrathin electronic circuits that can be manufactured by using conventional printing technologies are key elements necessary to realize wearable health sensors and next-generation flexible electronic devices. Due to their low level of power consumption, complementary (CMOS) circuits using both types of semiconductors can be easily employed in wireless devices. Here, we describe ultrathin CMOS logic circuits, for which not only the source/drain electrodes but also the semiconductor layers were printed. Both p-type and n-type organic thin film transistor devices were employed in a D-flip flop circuit in the newly developed stacked structure and exhibited excellent electrical characteristics, including good carrier mobilities of 0.34 and 0.21 cm(2) V(-1) sec(-1), and threshold voltages of nearly 0 V with low operating voltages. These printed organic CMOS D-flip flop circuits exhibit operating frequencies of 75 Hz and demonstrate great potential for flexible and printed electronics technology, particularly for wearable sensor applications with wireless connectivity.

An antibody- and label-free detection of a phosphoprotein (α-casein) has been achieved using an organic field-effect transistor (OFET)-based sensor. The fabricated OFET device possesses an extended-gate electrode functionalized with an artificial phosphoprotein receptor (Zn(II)-dipicolylamine complex, Zn(II)-DPA). It is shown that the OFET responds to the molecular recognition processes involving the Zn(II)-DPA at the extended-gate electrode. The binding of α-casein to the receptor in a HEPES solution results in an analyte-specific changes of the drain current of the OFET. The successful demonstration of the antibody- and label-free detection using the OFET could pave the way to the development of low-cost, disposable, and portable electronic sensor devices.

Herein, we report an organic field effect transistor (OFET) with an extended-gate modified by an artificial receptor for the detection of mercury(II) ions (Hg(2+)) in water. The sensor device is easy to fabricate, reusable, disposable, and portable. Thus OFET sensors could be applied for low-cost on-site detection of Hg(2+).

Biosensors based on organic field effect transistors (OFETs) are one of the more promising device applications in organic electronics. However, OFET-based biosensors are still in their early stages of development compared to other electrochemical biosensors. This study is the first to report on an extended-gate type organic field effect transistor (OFET) for lactate detection in aqueous media. Here, the extended-gate electrode of the OFET was modified with layers of a lactate oxidase and a horseradish peroxidase osmium-redox polymer on a flexible plastic film substrate for an enzymatic redox reaction of lactate. The device exhibited both high selectivity and sensitivity. The limit of detection (LOD) and the limit of quantification (LOQ) were estimated to be 66 nM and 220 nM, respectively, which are the sufficient detection limit for practical sensor applications. The obtained results confirm that extended-gate type OFET devices are applicable to enzyme-based biosensors for detecting lactate levels., (Copyright © 2015 Elsevier B.V. All rights reserved.)

We have characterized mechanisms to improve the adhesion between printed electrodes prepared from silver nanoparticle inks and underlying polymer layers. Adhesion strength was significantly improved by sintering the inks above the glass transition temperature of the polymer underlayers, whereby enhanced adhesion was realized through interfacial fusion between the silver electrode layer and the underlying polymer layer. The surface energy of the underlayer was found to be an important factor in the improvement of adhesive strength, in that larger and thicker interfused regions between layers were observed for underlayers that had higher surface energies.

We propose an organic field effect transistor (OFET)-based sensor design as a new and innovative platform for anion detection. OFETs could be fabricated on low-cost plastic film substrates using printing technologies, suggesting that OFETs can potentially be applied to practical supramolecular anion sensor devices in the near future.