Solution-processed Amorphous Oxide Semiconductor Research Articles

Bilayer channel structure to improve the stability of solution-processed metal oxide transistors under AC stress

In this work, we report solution-processed bilayer channel thin film transistors (TFTs) based on solution-processed amorphous oxide semiconductors (AOSs) that fulfill both superb electrical performance and device stability against applied alternating current (AC) drain bias stress. Acceptor-like states generation via hot carrier effect (HCE) is a representative device degradation mechanism suggested for AOS-based TFTs when subjected to AC bias stress, featuring threshold voltage (Vth) shift and on-current (Ion) lowering. As excess electric field and accumulated carriers in the AOS channel cause HCE, alleviating carrier accumulation is a key solution for mitigating HCE. Bilayer channel TFTs comprising two different AOSs could work as a countermeasure to overcome HCE since proper energy band alignment of two channels creates a conduction band difference that act as the energy barrier for carriers. In this regard, we employed amorphous indium-gallium-zinc oxide (IGZO) and zinc-tin oxide (ZTO) as bottom and top layer, respectively, for bilayer channel TFT. Designed bilayer channel showed a conduction band difference of 0.18 eV, and fabricated TFT based on this architecture exhibited high mobility over to 5.9 cm2/Vs with slight Vth shift of 0.1 V and Ion lowering of 1.7% for 1000 s against applied AC stress, demonstrating device stability under AC drain bias stress.

Low-Temperature Solution-Processed ZnSnO Ozone Gas Sensors Using UV-Assisted Thermal Annealing

Ultraviolet-assisted thermal annealing (UVTA) has been widely used to fabricate solution-processed amorphous oxide semiconductor (AOS)-based transistors and photodetectors. However, this method has not been used for AOS-based gas sensors, even though AOS is a good gas sensing material. This study determines the effect of UVTA on the electrical properties of In-free amorphous ZnSnO (ZTO) thin films and their ozone (O3) gas sensing characteristics. UV light from a Mercury lamp has sufficient energy to decompose the organic- and hydrogen-based impurities completely, which promotes the formation of metal oxide networks, so the quality of ZTO films is greatly increased by increasing treatment time. A relatively high gas response of 1.42 with a fast response/recovery time (124/78 s) is achieved. This strategy allows the fabrication of ZTO gas sensors at low temperature (150 °C) and is applicable to flexible electronics.

In-Plane Amorphous Oxide Ionotronic Devices and Circuits with Photochemically Enabled Favorable Interfaces.

Here, we demonstrate a side-gated in-plane structure of solution-processed amorphous oxide semiconductor ionotronic devices and logic circuits enabled by ion gel gate dielectrics with a monolithically integrated nanoscale passivation architecture. The large capacitance of the electric double layer (EDL) in the ion gel allows a device structure to be a side gate geometry, forming an in-plane structured amorphous In-Ga-Zn-O (a-IGZO) ionotronic transistor, which can be translated into a simplified logic gate configuration with a low operation voltage. Particularly, the monolithic passivation of the coplanar electrodes offers advantages over conventional inhomogeneous passivation, mitigating unintentional parasitic leakage current through the ion gel dielectric layer. More importantly, the monolithically integrated passivation over electrodes was readily obtained with a complementary metal-oxide semiconductor-compatible photochemical process by employing a controlled ultraviolet light manipulation under ozone ambient, which introduced not only much enhanced electrical characteristics but also a scalable device architecture. We investigated various electrical behaviors of the side-gated a-IGZO ionotronic transistor based on EDL, which is called an electric double layer transistor (EDLT), and logic circuits enabled by photochemically realized monolithic aluminum oxide (AlOX) passivation comparing to the native or polymerized passivation layer, which reveals that the photoassisted AlOX secures high-performance a-IGZO EDLTs with a low off current (<5.23 × 10-8 A), high on/off ratio (>1.87 × 105), and exceptional high carrier mobility (>14.5 cm2 V-1 s-1). Owing to the significantly improved electrical characteristics, an inverter circuit was successfully achieved with broad operation voltages from an ultralow VDD of 1 mV to 1.5 V, showing a fully logical voltage transfer characteristic with a gain of more than 4 V V-1.

Suppression of persistent photo-conductance in solution-processed amorphous oxide thin-film transistors

This study offers a combinatorial approach for suppressing the persistent photo-conductance (PPC) characteristic in solution-processed amorphous oxide semiconductor (AOS) thin-film transistors (TFTs) in order to achieve rapid photo-recovery. Various analyses were used to examine the photo-instability of indium-gallium-zinc-oxide (IGZO) TFTs including negative-bias-illumination-stress (NBIS) and transient photo-response behaviors. It was found that the indium ratio in metallic components had a significant impact on their PPC and photo-recovery characteristics. In particular, when the indium ratio was low (51.5%), the PPC characteristic was significantly suppressed and achieving rapid photo-recovery was possible without significantly affecting the electrical performance of AOSs. These results imply that the optimization of the indium composition ratio may allow achieving highly photo-stable and near PPC-free characteristics while maintaining high electrical performance of AOSs. It is considered that the negligible PPC behavior and rapid photo-recovery observed in IGZO TFTs with a lower indium composition are attributed to the less activation energy required for the neutralization of ionized oxygen vacancies.

Multifunctional Organic-Semiconductor Interfacial Layers for Solution-Processed Oxide-Semiconductor Thin-Film Transistor.

The stabilization and control of the electrical properties in solution-processed amorphous-oxide semiconductors (AOSs) is crucial for the realization of cost-effective, high-performance, large-area electronics. In particular, impurity diffusion, electrical instability, and the lack of a general substitutional doping strategy for the active layer hinder the industrial implementation of copper electrodes and the fine tuning of the electrical parameters of AOS-based thin-film transistors (TFTs). In this study, the authors employ a multifunctional organic-semiconductor (OSC) interlayer as a solution-processed thin-film passivation layer and a charge-transfer dopant. As an electrically active impurity blocking layer, the OSC interlayer enhances the electrical stability of AOS TFTs by suppressing the adsorption of environmental gas species and copper-ion diffusion. Moreover, charge transfer between the organic interlayer and the AOS allows the fine tuning of the electrical properties and the passivation of the electrical defects in the AOS TFTs. The development of a multifunctional solution-processed organic interlayer enables the production of low-cost, high-performance oxide semiconductor-based circuits.

Ion-gel gated field-effect transistors with solution-processed oxide semiconductors for bioinspired artificial synapses

With the development of sciences and technologies of artificial intelligence in recent years, more and more attention is focused on the research of the synaptic devices inspired by human brain. In this paper, ion-gel coupled synaptic transistors with solution-possessed amorphous indium-zinc-oxide (In-Zn-O) thin films were demonstrated. Ion-gel dielectric provides a strong ionic/electronic coupling on the solution-processed In-Zn-O thin films, which is due to the very large electric-double-layer (EDL) capacitances (∼4.87 μF/cm2). The surface morphology, chemical composition/stoichiometry and electrical performances of In-Zn-O field-effect transistors (FETs) were analyzed as a function of annealing temperature. Most importantly, the ion-gel gated In-Zn-O FETs were used for synaptic functions simulations. The in-plane gate is used as the presynaptic input terminal and the In-Zn-O channel with source/drain electrodes is used as the postsynaptic output terminal. Mobile ions in ion-gel are regarded as neurotransmitters. Gate pluses were applied on the in-plane electrodes which is analogous to presynaptic spikes onto presynaptic membrane. Fundamental synaptic functions including excitatory postsynaptic current (EPSC), spike time-dependent EPSC, paired-pulse facilitation (PPF), and dynamic synaptic behaviors are mimicked. These results may provide a new opportunity and strategy to develop of highly functional electronic synapses and next-generation neuromorphic systems by using ion-gel gated devices with solution-processed amorphous oxide semiconductors.

A review of multi-stacked active-layer structures for solution-processed oxide semiconductor thin-film transistors

ABSTRACTIn this review, the multi-stacked active-layer (MSAL) structures for the solution-processed amorphous oxide semiconductor (AOS) thin-film transistors (TFTs) are summarized to improve their electrical characteristics and stabilities based on the authors’ previous researches. The MSAL structures can overcome an inherent weakness of the solution-processed AOS TFTs, which is the creation of porosities from solvent volatilization. Furthermore, by modifying each layer, the performance and reliability of the solution-processed AOS TFTs could be improved more. Here, the fundamental studies of MSAL structures with homo-stacked active-layer TFTs are presented, and the various modulations of active layers in hetero-stacked active-layer TFTs are covered. In addition, the effect of the interface between the stacked layers is also discussed.

High-Performance Inkjet-Printed Indium-Gallium-Zinc-Oxide Transistors Enabled by Embedded, Chemically Stable Graphene Electrodes.

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.

Transparent megahertz circuits from solution-processed composite thin films.

Solution-processed amorphous oxide semiconductors have attracted considerable interest in large-area transparent electronics. However, due to its relative low carrier mobility (∼10 cm(2) V(-1) s(-1)), the demonstrated circuit performance has been limited to 800 kHz or less. Herein, we report solution-processed high-speed thin-film transistors (TFTs) and integrated circuits with an operation frequency beyond the megahertz region on 4 inch glass. The TFTs can be fabricated from an amorphous indium gallium zinc oxide/single-walled carbon nanotube (a-IGZO/SWNT) composite thin film with high yield and high carrier mobility of >70 cm(2) V(-1) s(-1). On-chip microwave measurements demonstrate that these TFTs can deliver an unprecedented operation frequency in solution-processed semiconductors, including an extrinsic cut-off frequency (f(T) = 102 MHz) and a maximum oscillation frequency (f(max) = 122 MHz). Ring oscillators further demonstrated an oscillation frequency of 4.13 MHz, for the first time, realizing megahertz circuit operation from solution-processed semiconductors. Our studies represent an important step toward high-speed solution-processed thin film electronics.

Amorphous oxide alloys as interfacial layers with broadly tunable electronic structures for organic photovoltaic cells

In diverse classes of organic optoelectronic devices, controlling charge injection, extraction, and blocking across organic semiconductor-inorganic electrode interfaces is crucial for enhancing quantum efficiency and output voltage. To this end, the strategy of inserting engineered interfacial layers (IFLs) between electrical contacts and organic semiconductors has significantly advanced organic light-emitting diode and organic thin film transistor performance. For organic photovoltaic (OPV) devices, an electronically flexible IFL design strategy to incrementally tune energy level matching between the inorganic electrode system and the organic photoactive components without varying the surface chemistry would permit OPV cells to adapt to ever-changing generations of photoactive materials. Here we report the implementation of chemically/environmentally robust, low-temperature solution-processed amorphous transparent semiconducting oxide alloys, In-Ga-O and Ga-Zn-Sn-O, as IFLs for inverted OPVs. Continuous variation of the IFL compositions tunes the conduction band minima over a broad range, affording optimized OPV power conversion efficiencies for multiple classes of organic active layer materials and establishing clear correlations between IFL/photoactive layer energetics and device performance.

Photoresist-Free Fully Self-Patterned Transparent Amorphous Oxide Thin-Film Transistors Obtained by Sol-Gel Process

We demonstrated self-patterned solution-processed amorphous oxide semiconductor thin-film transistors (TFTs) using photosensitive sol-gels. The photosensitive sol-gels were synthesized by adding β-diketone compounds, i.e., benzoylacetone and acetylacetone, to sol-gels. The chemically modified photosensitive sol-gels showed a high optical absorption at specific wavelengths due to the formation of metal chelate bonds. Photoreactions of the modified solutions enabled a photoresist-free process. Moreover, Zn–Sn–O with a high Sn ratio, which is hard to wet-etch using conventional photolithography due to its chemical durability, was easily patterned via the self-patterning process. Finally, we fabricated a solution-processed oxide TFT that included fully self-patterned electrodes and an active layer.

Printed Indium Gallium Zinc Oxide Transistors. Self-Assembled Nanodielectric Effects on Low-Temperature Combustion Growth and Carrier Mobility

Solution-processed amorphous oxide semiconductors (AOSs) are emerging as important electronic materials for displays and transparent electronics. We report here on the fabrication, microstructure, and performance characteristics of inkjet-printed, low-temperature combustion-processed, amorphous indium gallium zinc oxide (a-IGZO) thin-film transistors (TFTs) grown on solution-processed hafnia self-assembled nanodielectrics (Hf-SANDs). TFT performance for devices processed below 300 °C includes >4× enhancement in electron mobility (μFE) on Hf-SAND versus SiO2 or ALD-HfO2 gate dielectrics, while other metrics such as subthreshold swing (SS), current on:off ratio (ION:IOFF), threshold voltage (Vth), and gate leakage current (Ig) are unchanged or enhanced. Thus, low voltage IGZO/SAND TFT operation (<2 V) is possible with ION:IOFF = 10(7), SS = 125 mV/dec, near-zero Vth, and large electron mobility, μFE(avg) = 20.6 ± 4.3 cm(2) V(-1) s(-1), μFE(max) = 50 cm(2) V(-1) s(-1). Furthermore, X-ray diffraction analysis indicates that the 300 °C IGZO combustion processing leaves the underlying Hf-SAND microstructure and capacitance intact. This work establishes the compatibility and advantages of all-solution, low-temperature fabrication of inkjet-printed, combustion-derived high-mobility IGZO TFTs integrated with self-assembled hybrid organic-inorganic nanodielectrics.

High performance and high stability low temperature aqueous solution-derived Li–Zr co-doped ZnO thin film transistors

Highly stable and high performance solution-processed amorphous oxide semiconductor thin film transistors (TFTs) were produced using a Li and Zr co-doped ZnO-based aqueous solution. Li and Zr co-doping at the appropriate amounts enhanced the oxide film quality in terms of enhanced oxygen bonding and reduced defect sites. The 0.5 mol% Li and 1.0 mol% Zr co-doped ZnO TFTs annealed at 320 °C exhibited noticeably lower threshold voltage shifts of 3.54 V under positive bias stress and −2.07 V under negative bias temperature stress than the non-doped ZnO TFTs. The transistors revealed a good device mobility performance of 5.39 cm2 V−1 s−1 and an on/off current ratio of 108 when annealed at 320 °C, compared to a mobility performance of 2.86 cm2 V−1 s−1 and an on/off current ratio of ∼107 when annealed at 270 °C. Our results suggest that Li and Zr co-doping can be a useful technique to produce more reliable and low temperature solution-processed oxide semiconductor TFTs.

High-Performance Solution-Processed Amorphous Zinc−Indium−Tin Oxide Thin-Film Transistors

Films of the high-performance solution-processed amorphous oxide semiconductor a-ZnIn(4)Sn(4)O(15), grown from 2-methoxyethanol/ethanolamine solutions, were used to fabricate thin-film transistors (TFTs) in combination with an organic self-assembled nanodielectric as the gate insulator. This structurally dense-packed semiconductor composition with minimal Zn(2+) incorporation strongly suppresses transistor off-currents without significant mobility degradation, and affords field-effect electron mobilities of approximately 90 cm(2) V(-1) s(-1) (104 cm(2) V(-1) s(-1) maximum obtained for patterned ZITO films), with I(on)/I(off) ratio approximately 10(5), a subthreshhold swing of approximately 0.2 V/dec, and operating voltage <2 V for patterned devices with W/L = 50. The microstructural and electronic properties of ZITO semiconductor film compositions in the range Zn(9-2x)In(x)Sn(x)O(9+1.5x) (x = 1-4) and ZnIn(8-x)Sn(x)O(13+0.5x) (x = 1-7) were systematically investigated to elucidate those factors which yield optimum mobility, I(on)/I(off), and threshold voltage parameters. It is shown that structural relaxation and densification by In(3+) and Sn(4+) mixing is effective in reducing carrier trap sites and in creating carrier-generating oxygen vacancies. In contrast to the above results for TFTs fabricated with the organic self-assembled nanodielectric, ZnIn(4)Sn(4)O(15) TFTs fabricated with SiO(2) gate insulators exhibit electron mobilities of only approximately 11 cm(2) V(-1) s(-1) with I(on)/I(off) ratios approximately 10(5), and a subthreshhold swing of approximately 9.5 V/dec.

Solution-processed zinc–tin oxide thin-film transistors with low interfacial trap density and improved performance

Solution-processed amorphous oxide semiconductors are attractive channel materials in thin-film transistors (TFTs) for low-cost electronics. We demonstrate improved performance and uniformity of solution-processed zinc–tin oxide (ZTO) TFTs by optimizing the prebake process for the ZTO precursor film. ZTO prebake process prearranges the dielectric/semiconductor interface and minimizes the performance variation caused by the uneven thermal distribution during annealing process. Prearranging the interface also reduces interfacial trap density and results in improved performance. A mobility of 27.3 cm2/V s, an on/off ratio of ∼107, and a subthreshold swing of 122 mV/decade have been obtained. Significant improvement in operational stability has also been observed.

Correction to Aging Dynamics of Solution-Processed Amorphous Oxide Semiconductor Field Effect Transistors

Correction to Aging Dynamics of Solution-Processed Amorphous Oxide Semiconductor Field Effect Transistors

Aging Dynamics of Solution-Processed Amorphous Oxide Semiconductor Field Effect Transistors

This study determined the aging characteristics of solution-processed amorphous In−Ga−Zn oxide (a-IGZO) layers as amorphous oxide semiconductors (AOSs) for transparent, flexible thin-film transistor (TFT) applications. The work function of a-IGZOs upon exposure to air immediately after vacuum annealing was monitored using Kelvin probe force microscopy (KPFM). An increase was observed in the work function with time. Additionally, X-ray photoelectron spectroscopy combined with the KPFM results revealed two competing factors responsible for the aging characteristics: adsorption of oxygen molecules on the nanopore surfaces within the films, and the creation of defects, including oxygen vacancies and zinc interstitials. Although the former was reversible by alteration of ambient conditions, the latter was irreversible. On the basis of modified band theory, we proposed an operative mechanism for solution-processed AOS TFTs based on both the nature of porous amorphous structures and the aging dynamics. The persp...