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High-performance oxide transistors have recently attracted significant attention for use in various electronic applications, such as displays, sensors, and back-end-of-line transistors. In this study, we demonstrate atomically thin indium-oxide (InOx) semiconductors using a solution process for high-performance thin-film transistors (TFTs). To achieve superior field-effect mobility and switching characteristics in TFTs, the bandgap and thickness of the InOx were tuned by controlling the InOx solution molarity. As a result, a high field-effect mobility and on/off-current ratio of 13.95 cm2 V-1 s-1 and 1.42 × 1010, respectively, were achieved using 3.12-nanometer-thick InOx. Our results showed that the charge transport of optimized InOx with a thickness of 3.12 nm is dominated by percolation conduction due to its low surface roughness and appropriate carrier concentration. Furthermore, the atomically thin InOx TFTs showed superior positive and negative gate bias stress stabilities, which are important in electronic applications. The proposed oxide TFTs could provide an effective means of the fabrication of scalable, high-throughput, and high-performance transistors for next-generation electronic applications.

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Neuromorphic computing, which mimics brain function, can address the shortcomings of the "von Neumann" system and is one of the critical components of next-generation computing. The use of light to stimulate artificial synapses has the advantages of low power consumption, low latency, and high stability. We demonstrate amorphous InAlZnO-based light-stimulated artificial synaptic devices with a thin-film transistor structure. The devices exhibit fundamental synaptic properties, including excitatory postsynaptic current, paired-pulse facilitation (PPF), and short-term plasticity to long-term plasticity conversion under light stimulation. The PPF index stimulated by 375 nm light is 155.9% when the time interval is 0.1 s. The energy consumption of each synaptic event is 2.3 pJ, much lower than that of ordinary MOS devices and other optical-controlled synaptic devices. The relaxation time constant reaches 277 s after only 10 light spikes, which shows the great synaptic plasticity of the device. In addition, we simulated the learning-forgetting-relearning-forgetting behavior and learning efficiency of human beings under different moods by changing the gate voltage. This work is expected to promote the development of high-performance optoelectronic synaptic devices for neuromorphic computing.

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In this study, we propose tunable pH sensors based on the electric-double-layer transistor (EDLT) with time-dependent sensitivity characteristics. The EDLT is able to modulate the drain current by using the mobile ions inside the electrolytic gate dielectric. This property allows the implementation of a device with sensitivity characteristics that are simply adjusted according to the measurement time. An extended gate-type, ion-sensitive, field-effect transistor consisting of a chitosan/Ta2O5 hybrid dielectric EDLT transducer, and an SnO2 sensing membrane, were fabricated to evaluate the sensing behavior at different buffer pH levels. As a result, we were able to achieve tunable sensitivity by only adjusting the measurement time by using a single EDLT and without additional gate electrodes. In addition, to demonstrate the unique sensing behavior of the time-dependent tunable pH sensors based on organic−inorganic hybrid EDLT, comparative sensors consisting of a normal FET with a SiO2 gate dielectric were prepared. It was found that the proposed pH sensors exhibit repeatable and stable sensing operations with drain current deviations <1%. Therefore, pH sensors using a chitosan electrolytic EDLT are suitable for biosensor platforms, possessing tunable sensitivity and high-reliability characteristics.

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To utilize continuous ultralow intensity signals from oxide synaptic transistors as artificial synapses that mimic human visual perception, we propose strategic oxide channels that optimally utilize their advantageous functions by stacking two oxide semiconductors with different conductivities. The bottom amorphous indium-gallium-zinc oxide (a-IGZO) layer with a relatively low conductivity was designed for an extremely low initial postsynaptic current (PSCi) by achieving full depletion at a low negative gate voltage, and the stacked top amorphous indium-zinc oxide (a-IZO) layer improved the amplitude of the synaptic current and memory retention owing to the enhancement in the persistent photoconductivity characteristics. We demonstrated an excellent photonic synapse thin-film transistor (TFT) with a precise synaptic weight change even in the range of ultralow light intensity by adapting this stacking IGZO/IZO channel. The proposed device exhibited distinct ∆PSC values of 3.1 and 18.1 nA under ultralow ultraviolet light (350 nm, 50 ms) of 1.6 and 8.0 µW/cm2. In addition, while the lowest light input exhibited short-term plasticity characteristics similar to the "volatile-like" behavior of the human brain with a current recovery close to the initial value, the increase in light intensity caused long-term plasticity characteristics, thus achieving synaptic memory transition in the IGZO/IZO TFTs.

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In this paper, we present an empirical modeling procedure to capture gate bias dependency of amorphous oxide semiconductor (AOS) thin-film transistors (TFTs) while considering contact resistance and disorder effects at room temperature. From the measured transfer characteristics of a pair of TFTs where the channel layer is an amorphous In-Ga-Zn-O (IGZO) AOS, the gate voltage-dependent contact resistance is retrieved with a respective expression derived from the current-voltage relation, which follows a power law as a function of a gate voltage. This additionally allows the accurate extraction of intrinsic channel conductance, in which a disorder effect in the IGZO channel layer is embedded. From the intrinsic channel conductance, the characteristic energy of the band tail states, which represents the degree of channel disorder, can be deduced using the proposed modeling. Finally, the obtained results are also useful for development of an accurate compact TFT model, for which a gate bias-dependent contact resistance and disorder effects are essential.

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The integration of 4 nm thick amorphous indium tungsten oxide (a-IWO) and a hafnium oxide (HfO2) high-κ gate dielectric has been demonstrated previously as one of promising amorphous oxide semiconductor (AOS) thin-film transistors (TFTs). In this study, the more positive threshold voltage shift (∆VTH) and reduced ION were observed when increasing the oxygen ratio during a-IWO deposition. Through simple material measurements and Technology Computer Aided Design (TCAD) analysis, the distinct correlation between different chemical species and the corresponding bulk and interface density of states (DOS) parameters were systematically deduced, validating the proposed physical mechanisms with a quantum model for a-IWO nanosheet TFT. The effects of oxygen flow on oxygen interstitial (Oi) defects were numerically proved for modulating bulk dopant concentration Nd and interface density of Gaussian acceptor trap NGA at the front channel, significantly dominating the transfer characteristics of a-IWO TFT. Furthermore, based on the studies of density functional theory (DFT) for the correlation between formation energy Ef of Oi defect and Fermi level (EF) position, we propose a numerical methodology for monitoring the possible concentration distribution of Oi as a function of a bias condition for AOS TFTs.

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Neuromorphic engineering, a methodology for emulating synaptic functions or neural systems, has attracted tremendous attention for achieving next-generation artificial intelligence technologies in the field of electronics and photonics. However, to emulate human visual memory, an active pixel sensor array for neuromorphic photonics has yet to be demonstrated, even though it can implement an artificial neuron array in hardware because individual pixels can act as artificial neurons. Here, we present a neuromorphic active pixel image sensor array (NAPISA) chip based on an amorphous oxide semiconductor heterostructure, emulating the human visual memory. In the 8 × 8 NAPISA chip, each pixel with a select transistor and a neuromorphic phototransistor is based on a solution-processed indium zinc oxide back channel layer and sputtered indium gallium zinc oxide front channel layer. These materials are used as a triggering layer for persistent photoconductivity and a high-performance channel layer with outstanding uniformity. The phototransistors in the pixels exhibit both photonic potentiation and depression characteristics by a constant negative and positive gate bias due to charge trapping/detrapping. The visual memory and forgetting behaviors of the NAPISA can be successfully demonstrated by using the pulsed light stencil method without any software or simulation. This study provides valuable information to other neuromorphic devices and systems for next-generation artificial intelligence technologies.

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This paper presents a fully transparent and sensitivity-programmable biosensor based on an amorphous-indium-gallium-zinc-oxide (a-IGZO) thin-film transistor (TFT) with embedded resistive switching memories (ReRAMs). The sensor comprises a control gate (CG) and a sensing gate (SG), each with a resistive switching (RS) memory connected, and a floating gate (FG) that modulates the channel conductance of the a-IGZO TFT. The resistive coupling between the RS memories connected to the CG and SG produces sensitivity properties that considerably exceed the limit of conventional ion-sensitive field-effect transistor (ISFET)-based sensors. The resistances of the embedded RS memories were determined by applying a voltage to the CG-FG and SG-FG structures independently and adjusting the compliance current. Sensors constructed using RS memories with different resistance ratios yielded a pH sensitivity of 50.5 mV/pH (RCG:RSG = 1:1), 105.2 mV/pH (RCG:RSG = 2:1), and 161.9 mV/pH (RCG:RSG = 3:1). Moreover, when the RCG:RSG = 3:1, the hysteresis voltage width (VH) and drift rate were 54.4 mV and 32.9 mV/h, respectively. As the increases in VH and drift rate are lower than the amplified sensitivity, the sensor performs capably. The proposed device is viable as a versatile sensing device capable of detecting various substances, such as cells, antigens, DNA, and gases.

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Low-temperature solution-processed oxide semiconductor and dielectric films typically possess a substantial number of defects and impurities due to incomplete metal-oxygen bond formation, causing poor electrical performance and stability. Here, we exploit a facile route to improve the film quality and the interfacial property of low-temperature solution-processed oxide thin films via elemental diffusion between metallic ion-doped InOx (M:InOx) ternary oxide semiconductor and AlOx gate dielectric layers. Particularly, it was revealed that metallic dopants such as magnesium (Mg) and hafnium (Hf) having a small ionic radius, a high Gibbs energy of oxidation, and bonding dissociation energy could successfully diffuse into the low-quality AlOx gate dielectric layer and effectively reduce the structural defects and residual impurities present in the bulk and at the semiconductor/dielectric interface. Through an extensive investigation on the compositional, structural, and electrical properties of M:InOx/AlOx thin-film transistors (TFTs), we provide direct evidences of elemental diffusion occurred between M:InOx and AlOx layers as well as its contribution to the electrical performance and operational stability. Using the elemental diffusion process, we demonstrate solution-processed Hf:InOx TFTs using a low-temperature (180 °C) AlOx gate dielectric having a field-effect mobility of 2.83 cm2 V-1·s-1 and improved bias stability. Based on these results, it is concluded that the elemental diffusion between oxide semiconductor and gate dielectric layers can play a crucial role in realizing oxide TFTs with enhanced structural and interfacial integrity.

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Transparent conductive oxides (TCOs) are important materials for a wide range of optoelectronic devices. Amorphous zinc tin oxide (a-ZTO) is a TCO and one of the best nontoxic, low-cost replacements for more expensive amorphous indium-gallium-zinc oxide. Here, we employ spray pyrolysis (SP), an inexpensive and versatile chemical vapor deposition-based technique, to synthesize a-ZTO with an as-deposited conductivity of ≈300 S/cm-the highest value hitherto among the reported solution-processed films. Compositional analysis via X-ray photoelectron spectroscopy reveals a nonstoichiometric transfer of Zn and Sn from the dissolved precursors into the film, with the best electrical properties achieved at a film composition of xfilm = 0.38 ± 0.04 ((ZnO)x(SnO2)1-x (0 < x < 1)). The morphology of these films is compared to films synthesized by physical vapor deposition (PVD), and a strong correlation between morphology and electrical properties is revealed. The granular nature of the SP-grown films, which seems like a drawback at first glance, brings about the prospect of using a-ZTO in ink-jet-printed films from a nanoparticle suspension for the room-temperature deposition. Brief post-anneal cycles in N2 gas improve the conductivity of the films by means of grain boundary (GB) passivation.

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The trade-off between performance and stability in amorphous oxide semiconductor-based thin-film transistors (TFTs) has been a critical challenge, meaning that it is difficult to simultaneously achieve high mobility and stability under bias and light stresses. Here, an amorphous mixture of two indium-free BaSnO3 and ZnSnO3 compounds, a-(Zn,Ba)SnO3, is proposed as a feasible strategy to achieve high mobility and stability at the same time. The choice of BaSnO3 as a counterpart to ZnSnO3, a well-known In-free candidate in amorphous oxide semiconductors, is to improve structural order and oxygen stoichiometry due to the large heat of formation and to preserve electron mobility due to the same kind of octahedral Sn-O network. Our first-principles calculations indeed show that compared to pure a-ZnSnO3, BaSnO3 plays a crucial role in restoring structural order in both stoichiometric and O-deficient supercells without seriously damaging the conduction band minimum. The resulting features of a-(Zn,Ba)SnO3 reduce O-deficiency and the valence band tail states, which are known to be critically associated with instability. It is experimentally demonstrated that a-(Zn,Ba)SnO3-based TFTs simultaneously exhibit high mobility (>20 cm2 V-1 s-1) and remarkable stability against negative bias illumination stress (ΔVth: <0.9 V). Our results suggest that a-(Zn,Ba)SnO3 would be a strong In-free candidate for next-generation TFT display, replacing the conventional a-InGaZnO4.

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The limited choice of materials for large area electronics limits the expansion of applications. Polycrystalline silicon (poly-Si) and indium gallium zinc oxide (IGZO) lead to thin-film transistors (TFTs) with high field-effect mobilities (>10 cm2/Vs) and high current ON/OFF ratios (IOn/IOff > ~107). But they both require vacuum processing that needs high investments and maintenance costs. Also, IGZO is prone to the scarcity and price of Ga and In. Other oxide semiconductors require the use of at least two cations (commonly chosen among Ga, Sn, Zn, and In) in order to obtain the amorphous phase. To solve these problems, we demonstrated an amorphous oxide material made using one earth-abundant metal: amorphous tin oxide (a-SnOx). Through XPS, AFM, optical analysis, and Hall effect, we determined that a-SnOx is a transparent n-type oxide semiconductor, where the SnO2 phase is predominant over the SnO phase. Used as the active material in TFTs having a bottom-gate, top-contact structure, a high field-effect mobility of ~100 cm2/Vs and an IOn/IOff ratio of ~108 were achieved. The stability under 1 h of negative positive gate bias stress revealed a Vth shift smaller than 1 V.

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In this report, reactive and nonreactive sputtering of amorphous ZnSnOy (a-ZnSnOy) was investigated, and extensive composition maps have been measured by X-ray photoelectron spectroscopy. The comprehensive analysis of the ((ZnO)x(SnO2)1-x) composition reveals that the best Zn/Sn ratio for high conductivity of the material can vary depending on the deposition technique utilized. Best conductivities of 225 S/cm were found to occur at x = 0.32 for reactive sputtering of a Sn target and x = 0.27 for nonreactive sputtering of a SnO2 target. These values correspond to unstable polymorphs of a-ZnSnOy, ZnSn2O5, and ZnSn3O7. Distinct local bonding arrangements have been confirmed by Raman spectroscopy.

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Thin-film transistors (TFTs) with high electrical performances (mobility > 10 cm2/V s, Vth < 1 V, SS < 1 V/decade, on/off ratio ≈ 106) obtained from the silicon- and oxide-based single-crystalline semiconductor materials require high processing temperature and hence are not suitable for flexible electronics. Amorphous oxide-based transparent electronic devices are attractive to meet emerging technological demands where crystalline oxide-/silicon-based architectures cannot provide a solution. Here, we tackle this problem by using a novel amorphous oxide semiconducting material-namely, indium tungsten oxide (IWO)-as the active channel in flexible TFTs (FTFTs). Post-annealing temperature as low as 270 °C for amorphous IWO thin films deposited by radio frequency sputtering at room temperature could result in smooth morphology ( Rrms ≈ 0.42 nm), good adhesion, and high carrier density ( n ≈ 7.19 × 1018 cm-3). Excellent TFT characteristics of flexible devices could be achieved with linear field effect mobility µFE ≈ 25.86 cm2/V s, subthreshold swing SS ≈ 0.30 V/decade, threshold voltage Vth ≈ -1.5 V, and on/off ratio Ion/ Ioff ≈ 5.6 × 105 at 3 V and stable operation during bending of the FTFT. Additionally, IWO TFTs were implemented as synapses, the building block for neuromorphic computing. Paired-pulse facilitation up to 138% was observed and showed an exponential decay resembling chemical synapses. Utilizing this characteristic, a high-pass dynamic temporal filter was devised providing increased gain from 1.55 to 21 when frequency was raised from 22 to 62 Hz. The high performance and stability of flexible TFTs obtained with IWO films demonstrate their promise for low-voltage electronic applications.

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We suggest the use of a thin-film transistor (TFT) composed of amorphous InGaZnO (a-IGZO) as a channel and a sensing layer for low-concentration NO2 gas detection. Although amorphous oxide layers have a restricted surface area when reacting with NO2 gas, such TFT sensors have incomparable advantages in the aspects of electrical stability, large-scale uniformity, and the possibility of miniaturization. The a-IGZO thin films do not possess typical reactive sites and grain boundaries, so that the variation in drain current of the TFTs strictly originates from oxidation reaction between channel surface and NO2 gas. Especially, the sensing data obtained from the variation rate of drain current makes it possible to monitor efficiently and quickly the variation of the NO2 concentration. Interestingly, we found that enhancement-mode TFT (EM-TFT) allows discrimination of the drain current variation rate at NO2 concentrations ≤10 ppm, whereas a depletion-mode TFT is adequate for discriminating NO2 concentrations ≥10 ppm. This discrepancy is attributed to the ratio of charge carriers contributing to gas capture with respect to total carriers. This capacity for the excellent detection of low-concentration NO2 gas can be realized through (i) three-terminal TFT gas sensors using amorphous oxide, (ii) measurement of the drain current variation rate for high selectivity, and (iii) an EM mode driven by tuning the electrical conductivity of channel layers.

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For large-area, printable, and flexible electronic applications using advanced semiconductors, novel dielectric materials with excellent capacitance, insulating property, thermal stability, and mechanical flexibility need to be developed to achieve high-performance, ultralow-voltage operation of thin-film transistors (TFTs). In this work, we first report on the facile fabrication of multifunctional hybrid multilayer gate dielectrics with tunable surface energy via a low-temperature solution-process to produce ultralow-voltage organic and amorphous oxide TFTs. The hybrid multilayer dielectric materials are constructed by iteratively stacking bifunctional phosphonic acid-based self-assembled monolayers combined with ultrathin high-k oxide layers. The nanoscopic thickness-controllable hybrid dielectrics exhibit the superior capacitance (up to 970 nF/cm2), insulating property (leakage current densities <10-7 A/cm2), and thermal stability (up to 300 °C) as well as smooth surfaces (root-mean-square roughness <0.35 nm). In addition, the surface energy of the hybrid multilayer dielectrics are easily changed by switching between mono- and bifunctional phosphonic acid-based self-assembled monolayers for compatible fabrication with both organic and amorphous oxide semiconductors. Consequently, the hybrid multilayer dielectrics integrated into TFTs reveal their excellent dielectric functions to achieve high-performance, ultralow-voltage operation (< ± 2 V) for both organic and amorphous oxide TFTs. Because of the easily tunable surface energy, the multifunctional hybrid multilayer dielectrics can also be adapted for various organic and inorganic semiconductors, and metal gates in other device configurations, thus allowing diverse advanced electronic applications including ultralow-power and large-area electronic devices.

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Efficient electron transfer between a cathode and an active organic layer is one key to realizing high-performance organic devices, which require electron injection/transport materials with very low work functions. We developed two wide-bandgap amorphous (a-) oxide semiconductors, a-calcium aluminate electride (a-C12A7:e) and a-zinc silicate (a-ZSO). A-ZSO exhibits a low work function of 3.5 eV and high electron mobility of 1 cm2/(V · s); furthermore, it also forms an ohmic contact with not only conventional cathode materials but also anode materials. A-C12A7:e has an exceptionally low work function of 3.0 eV and is used to enhance the electron injection property from a-ZSO to an emission layer. The inverted electron-only and organic light-emitting diode (OLED) devices fabricated with these two materials exhibit excellent performance compared with the normal type with LiF/Al. This approach provides a solution to the problem of fabricating oxide thin-film transistor-driven OLEDs with both large size and high stability.

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An electro-thermal annealing (ETA) method, which uses an electrical pulse of less than 100 ns, was developed to improve the electrical performance of array-level amorphous-oxide-semiconductor (AOS) thin-film transistors (TFTs). The practicality of the ETA method was experimentally demonstrated with transparent amorphous In-Ga-Zn-O (a-IGZO) TFTs. The overall electrical performance metrics were boosted by the proposed method: up to 205% for the trans-conductance (gm), 158% for the linear current (Ilinear), and 206% for the subthreshold swing (SS). The performance enhancement were interpreted by X-ray photoelectron microscopy (XPS), showing a reduction of oxygen vacancies in a-IGZO after the ETA. Furthermore, by virtue of the extremely short operation time (80 ns) of ETA, which neither provokes a delay of the mandatory TFTs operation such as addressing operation for the display refresh nor demands extra physical treatment, the semipermanent use of displays can be realized.

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Recent developments in solution-processed amorphous oxide semiconductors have established indium-gallium-zinc-oxide (IGZO) as a promising candidate for printed electronics. A key challenge for this vision is the integration of IGZO thin-film transistor (TFT) channels with compatible source/drain electrodes using low-temperature, solution-phase patterning methods. Here we demonstrate the suitability of inkjet-printed graphene electrodes for this purpose. In contrast to common inkjet-printed silver-based conductive inks, graphene provides a chemically stable electrode-channel interface. Furthermore, by embedding the graphene electrode between two consecutive IGZO printing passes, high-performance IGZO TFTs are achieved with an electron mobility of ∼6 cm(2)/V·s and current on/off ratio of ∼10(5). The resulting printed devices exhibit robust stability to aging in ambient as well as excellent resilience to thermal stress, thereby offering a promising platform for future printed electronics applications.

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Recent advances in glucose sensing have focused on the integration of sensors into contact lenses to allow noninvasive continuous glucose monitoring. Current technologies focus primarily on enzyme-based electrochemical sensing which requires multiple nontransparent electrodes to be integrated. Herein, we leverage amorphous indium gallium zinc oxide (IGZO) field-effect transistors (FETs), which have found use in a wide range of display applications and can be made fully transparent. Bottom-gated IGZO-FETs can have significant changes in electrical characteristics when the back-channel is exposed to different environments. We have functionalized the back-channel of IGZO-FETs with aminosilane groups that are cross-linked to glucose oxidase and have demonstrated that these devices have high sensitivity to changes in glucose concentrations. Glucose sensing occurs through the decrease in pH during glucose oxidation, which modulates the positive charge of the aminosilane groups attached to the IGZO surface. The change in charge affects the number of acceptor-like surface states which can deplete electron density in the n-type IGZO semiconductor. Increasing glucose concentrations leads to an increase in acceptor states and a decrease in drain-source conductance due to a positive shift in the turn-on voltage. The functionalized IGZO-FET devices are effective in minimizing detection of interfering compounds including acetaminophen and ascorbic acid. These studies suggest that IGZO FETs can be effective for monitoring glucose concentrations in a variety of environments, including those where fully transparent sensing elements may be of interest.

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