Photo-induced Reactive Oxygen Species Activation for Amorphous Indium-Gallium-Zinc Oxide Thin-Film Transistors Using Sodium Hypochlorite.

We proposed a novel material named sodium hypochlorite (NaClO) solution as a source of activation for amorphous indium-gallium-zinc oxide (a-IGZO) thin-film transistors (TFTs). We reduced the activation temperature from 300 to 150 °C using NaClO solution (concentration: 50%) and obtained satisfactory electrical characteristics of a-IGZO TFTs. The field-effect mobility, threshold voltage, on/off ratio, subthreshold swing, and threshold voltage (Vth) shift under negative bias illumination stress (VG = -20 V and VD = 10.1 V for 10,000 s) of NaClO (50%)-activated a-IGZO TFTs were 10.41 cm2/V·s, 1.51 V, 2.78 × 108, 0.37 V/dec, and -5.43 V, respectively. Also, the Vth shifts of the NaClO (50%)-activated a-IGZO TFTs (150 °C) under the positive bias stress test decreased from 5.01 to 1.87 V (VG = 20 V and VD = 10.1 V for 10,000 s) compared with that of only-annealed (300 °C) a-IGZO TFTs. Also, the mechanism of NaClO activation for a-IGZO TFTs is clarified through photo-assisted oxygen radical (POR) and heat-driven oxygen radical (HOR) effects. The POR and HOR effects generated the reactive oxygen species (ROS) from NaClO solution (50%), which activated a-IGZO TFTs at a low temperature (150 °C). When the NaClO solution (50%) was exposed to external energy, it generated ROS such as hydroxyl radicals (OH•), hydroperoxyl radicals (HO2•), and oxygen radicals (O•), which promoted the formation of strong metal-oxide bonds in a-IGZO TFTs. Furthermore, NaClO solution (50%) was applied to a-IGZO TFTs on a flexible polyimide substrate and electrohydrodynamic printing process for selective deposition.

Mechanochemical and Thermal Treatment for Surface Functionalization to Reduce the Activation Temperature of In-Ga-Zn-O Thin-film Transistors.

Amorphous indium-gallium-zinc oxide (a-IGZO) films, which are widely regarded as a promising material for the channel layer in thin-film transistors (TFTs), require a relatively high thermal annealing temperature to achieve switching characteristics through the formation of metal-oxygen (M-O) bonding (i.e., the activation process). The activation process is usually carried out at a temperature above 300 °C; however, achieving activation at lower temperatures is essential for realizing flexible display technologies. Here, a facile, low-cost, and novel technique using cellophane tape for the activation of a-IGZO films at a low annealing temperature is reported. In terms of mechanochemistry, mechanical pulling of the cellophane tape induces reactive radicals on the a-IGZO film surface, which can give rise to improvements in the properties of the a-IGZO films, leading to an increase in the number of M-O bonds and the carrier concentration via radical reactions, even at 200 °C. As a result, the a-IGZO TFTs, compared to conventionally annealed a-IGZO TFTs, exhibited improved electrical performances, such as mobility, on/off current ratio, and threshold voltage shift (under positive bias temperature and negative bias temperature stress for 10,000 s at 50 °C) from 8.25 to 12.81 cm2/(V·s), 2.85 × 107 to 1.21 × 108, 6.81 to 3.24 V, and -6.68 to -4.93 V, respectively.

Multifunctional, Room-Temperature Processable, Heterogeneous Organic Passivation Layer for Oxide Semiconductor Thin-Film Transistors.

In recent decades, oxide thin-film transistors (TFTs) have attracted a great deal of attention as a promising technology in terms of next-generation electronics due to their outstanding electrical performance. However, achieving robust electrical characteristics under various environments is a crucial challenge for successful realization of oxide-based electronic applications. To resolve the limitation, we propose a highly flexible and reliable heterogeneous organic passivation layer composed of stacked parylene-C and diketopyrrolopyrrole-polymer films for improving stability of oxide TFTs under various environments and mechanical stress. The presented multifunctional heterogeneous organic (MHO) passivation leads to high-performance oxide TFTs by: (1) improving their electrical characteristics, (2) protecting them from external reactive molecules, and (3) blocking light exposure to the oxide layer. As a result, oxide TFTs with MHO passivation exhibit outstanding stability in ambient air as well as under light illumination: the threshold voltage shift of the device is almost 0 V under severe negative bias illumination stress condition (white light of 5700 lx, gate voltage of -20 V, and drain voltage of 10.1 V for 20 000 s). Furthermore, since the MHO passivation layer exhibits high mechanical stability at a bending radius of ≤5 mm and can be deposited at room temperature, this technique is expected to be useful in the fabrication of flexible/wearable devices.

Artificially Fabricated Subgap States for Visible-Light Absorption in Indium-Gallium-Zinc Oxide Phototransistor with Solution-Processed Oxide Absorption Layer.

We present a solution-processed oxide absorption layer (SAL) for detecting visible light of long wavelengths (635 and 532 nm) for indium-gallium-zinc oxide (IGZO) phototransistors. The SALs were deposited onto sputtered IGZO using precursor solutions composed of IGZO, which have the same atomic configuration as that of the channel layer, resulting in superior interface characteristics. We artificially generated subgap states in the SAL using a low annealing temperature (200 °C), minimizing the degradation of the electrical characteristics of thin-film transistor. These subgap states improved the photoelectron generation in SALs under visible light of long wavelength despite the wide band gap of IGZO (∼3.7 eV). As a result, IGZO phototransistors with SALs have both high optical transparency and superior optoelectronic characteristics such as a high photoresponsivity of 206 A/W and photosensitivity of ∼106 under the influence of a green (532 nm) laser. Furthermore, endurance tests proved that the IGZO phototransistor with SALs can operate stably under red laser illumination switched on and off at 0.05 Hz for 7200 s.

High-Throughput Open-Air Plasma Activation of Metal-Oxide Thin Films with Low Thermal Budget.

Sputter-processed oxide films are typically annealed at high temperature (activation process) to achieve stable electrical characteristics through the formation of strong metal-oxide chemical bonds. For instance, indium-gallium-zinc oxide (IGZO) films typically need a thermal treatment at 300 °C for ≥1 h as an activation process. We propose an open-air plasma treatment (OPT) to rapidly and effectively activate sputter-processed IGZO films. The OPT effectively induces metal-oxide chemical bonds in IGZO films at temperatures as low as 240 °C, with a dwell time on the order of a second. Furthermore, by controlling the plasma-processing conditions (scan speed, distance a between plasma nozzle and samples, and gas flow rate), the electrical characteristics and the microstructure of the IGZO films can be easily tuned. Finally, OPT can be utilized to implement a selective activation process. Plasma-treated IGZO thin-film transistors (TFTs) exhibit comparable electrical characteristics to those of conventionally thermal treated IGZO TFTs. Through in-depth optical, chemical, and physical characterizations, we confirm that OPT simultaneously dissociates weak chemical bonds by UV radiation and ion bombardment and re-establishes the metal-oxide network by radical reaction and OPT-induced heat.

Analysis of the Bipolar Resistive Switching Behavior of a Biocompatible Glucose Film for Resistive Random Access Memory.

Resistive random access memory (RRAM) devices are fabricated through a simple solution process using glucose, which is a natural biomaterial for the switching layer of RRAM. The fabricated glucose-based RRAM device shows nonvolatile bipolar resistive switching behavior, with a switching window of 103 . In addition, the endurance and data retention capability of glucose-based RRAM exhibit stable characteristics up to 100 consecutive cycles and 104 s under constant voltage stress at 0.3 V. The interface between the top electrode and the glucose film is carefully investigated to demonstrate the bipolar switching mechanism of the glucose-based RRAM device. The glucose based-RRAM is also evaluated on a polyimide film to verify the possibility of a flexible platform. Additionally, a cross-bar array structure with a magnesium electrode is prepared on various substrates to assess the degradability and biocompatibility for the implantable bioelectronic devices, which are harmless and nontoxic to the human body. It is expected that this research can provide meaningful insights for developing the future bioelectronic devices.

Effect of Static and Rotating Magnetic Fields on Low-Temperature Fabrication of InGaZnO Thin-Film Transistors.

We suggest thermal treatment with static magnetic fields (SMFs) or rotating magnetic fields (RMFs) as a new technique for the activation of indium-gallium-zinc oxide thin-film transistors (IGZO TFTs). Magnetic interactions between metal atoms in IGZO films and oxygen atoms in air by SMFs or RMFs can be expected to enhance metal-oxide (M-O) bonds, even at low temperature (150 °C), through attraction of metal and oxygen atoms having their magnetic moments aligned in the same direction. Compared to IGZO TFTs with only thermal treatment at 300 °C, IGZO TFTs under an RMF (1150 rpm) at 150 °C show superior or comparable characteristics: field-effect mobility of 12.68 cm2 V-1 s-1, subthreshold swing of 0.37 V dec-1, and on/off ratio of 1.86 × 108. Although IGZO TFTs under an SMF (0 rpm) can be activated at 150 °C, the electrical performance is further improved in IGZO TFTs under an RMF (1150 rpm). These improvements of IGZO TFTs under an RMF (1150 rpm) are induced by increases in the number of M-O bonds due to enhancement of the magnetic interaction per unit time as the rpm value increases. We suggest that this new process of activating IGZO TFTs at low temperature widens the choice of substrates in flexible or transparent devices.

Facile fabrication of wire-type indium gallium zinc oxide thin-film transistors applicable to ultrasensitive flexible sensors.

We fabricated wire-type indium gallium zinc oxide (IGZO) thin-film transistors (TFTs) using a self-formed cracked template based on a lift-off process. The electrical characteristics of wire-type IGZO TFTs could be controlled by changing the width and density of IGZO wires through varying the coating conditions of template solution or multi-stacking additional layers. The fabricated wire-type devices were applied to sensors after functionalizing the surface. The wire-type pH sensor showed a sensitivity of 45.4 mV/pH, and this value was an improved sensitivity compared with that of the film-type device (27.6 mV/pH). Similarly, when the wire-type device was used as a glucose sensor, it showed more variation in electrical characteristics than the film-type device. The improved sensing properties resulted from the large surface area of the wire-type device compared with that of the film-type device. In addition, we fabricated wire-type IGZO TFTs on flexible substrates and confirmed that such structures were very resistant to mechanical stresses at a bending radius of 10 mm.

Boosting Visible Light Absorption of Metal-Oxide-Based Phototransistors via Heterogeneous In-Ga-Zn-O and CH3NH3PbI3 Films.

To broaden the availability and application of metal-oxide (M-O)-based optoelectronic devices, we suggest heterogeneous phototransistors composed of In-Ga-Zn-O (IGZO) and methylammonium lead iodide (CH3NH3PbI3) layers, which act as the amplifier layer (channel layer) and absorption layer, respectively. These heterogeneous phototransistors showed low persistence photocurrent compared with IGZO-only phototransistors and exhibited high photoresponsivity of 61 A/W, photosensitivity of 3.48 × 106, detectivity of 9.42 × 1010 Jones, external quantum efficiency of 154% in an optimized structure, and high photoresponsivity under water exposure via the deposition of silicon dioxide as a passivation layer. On the basis of these electrical results and various analyses, we determined that CH3NH3PbI3 could be activated as a light absorption layer, current barrier, and plasma damage blocking layer, which would serve to widen the range of applications of M-O-based optoelectronic devices with high photoresponsivity and reliability under visible light illumination.

The self-activated radical doping effects on the catalyzed surface of amorphous metal oxide films.

In this study, we propose a self-activated radical doping (SRD) method on the catalyzed surface of amorphous oxide film that can improve both the electrical characteristics and the stability of amorphous oxide films through oxidizing oxygen vacancy using hydroxyl radical which is a strong oxidizer. This SRD method, which uses UV irradiation and thermal hydrogen peroxide solution treatment, effectively decreased the amount of oxygen vacancies and facilitated self-passivation and doping effect by radical reaction with photo-activated oxygen defects. As a result, the SRD-treated amorphous indium-gallium-zinc oxide (a-IGZO) thin film transistors (TFTs) showed superior electrical performances compared with non-treated a-IGZO TFTs. The mobility increased from 9.1 to 17.5 cm2/Vs, on-off ratio increased from 8.9 × 107 to 7.96 × 109, and the threshold voltage shift of negative bias-illumination stress for 3600 secs under 5700 lux of white LED and negative bias-temperature stress at 50 °C decreased from 9.6 V to 4.6 V and from 2.4 V to 0.4 V, respectively.

Structural Engineering of Metal-Mesh Structure Applicable for Transparent Electrodes Fabricated by Self-Formable Cracked Template.

Flexible and transparent conducting electrodes are essential for future electronic devices. In this study, we successfully fabricated a highly-interconnected metal-mesh structure (MMS) using a self-formable cracked template. The template-fabricated from colloidal silica-can be easily formed and removed, presenting a simple and cost-effective way to construct a randomly and uniformly networked MMS. The structure of the MMS can be controlled by varying the spin-coating speed during the coating of the template solution or by stacking of metal-mesh layers. Through these techniques, the optical transparency and sheet resistance of the MMS can be designed for a specific purpose. A double-layered Al MMS showed high optical transparency (~80%) in the visible region, low sheet resistance (~20 Ω/sq), and good flexibility under bending test compared with a single-layered MMS, because of its highly-interconnected wire structure. Additionally, we identified the applicability of the MMS in the case of practical devices by applying it to electrodes of thin-film transistors (TFTs). The TFTs with MMS electrodes showed comparable electrical characteristics to those with conventional film-type electrodes. The cracked template can be used for the fabrication of a mesh structure consisting of any material, so it can be used for not only transparent electrodes, but also various applications such as solar cells, sensors, etc.

Improvement of Electrical Characteristics and Stability of Amorphous Indium Gallium Zinc Oxide Thin Film Transistors Using Nitrocellulose Passivation Layer.

In this research, nitrocellulose is proposed as a new material for the passivation layers of amorphous indium gallium zinc oxide thin film transistors (a-IGZO TFTs). The a-IGZO TFTs with nitrocellulose passivation layers (NC-PVLs) demonstrate improved electrical characteristics and stability. The a-IGZO TFTs with NC-PVLs exhibit improvements in field-effect mobility (µFE) from 11.72 ± 1.14 to 20.68 ± 1.94 cm2/(V s), threshold voltage (Vth) from 1.85 ± 1.19 to 0.56 ± 0.35 V, and on/off current ratio (Ion/off) from (5.31 ± 2.19) × 107 to (4.79 ± 1.54) × 108 compared to a-IGZO TFTs without PVLs, respectively. The Vth shifts of a-IGZO TFTs without PVLs, with poly(methyl methacrylate) (PMMA) PVLs, and with NC-PVLs under positive bias stress (PBS) test for 10,000 s represented 5.08, 3.94, and 2.35 V, respectively. These improvements were induced by nitrogen diffusion from NC-PVLs to a-IGZO TFTs. The lone-pair electrons of diffused nitrogen attract weakly bonded oxygen serving as defect sites in a-IGZO TFTs. Consequently, the electrical characteristics are improved by an increase of carrier concentration in a-IGZO TFTs, and a decrease of defects in the back channel layer. Also, NC-PVLs have an excellent property as a barrier against ambient gases. Therefore, the NC-PVL is a promising passivation layer for next-generation display devices that simultaneously can improve electrical characteristics and stability against ambient gases.

A solution-processed quaternary oxide system obtained at low-temperature using a vertical diffusion technique.

We report a method for fabricating solution-processed quaternary In-Ga-Zn-O (IGZO) thin-film transistors (TFTs) at low annealing temperatures using a vertical diffusion technique (VDT). The VDT is a deposition process for spin-coating binary and ternary oxide layers consecutively and annealing at once. With the VDT, uniform and dense quaternary oxide layers were fabricated at lower temperatures (280 °C). Compared to conventional IGZO and ternary In-Zn-O (IZO) thin films, VDT IGZO thin film had higher density of the metal-oxide bonds and lower density of the oxygen vacancies. The field-effect mobility of VDT IGZO TFT increased three times with an improved stability under positive bias stress than IZO TFT due to the reduction in oxygen vacancies. Therefore, the VDT process is a simple method that reduces the processing temperature without any additional treatment for quaternary oxide semiconductors with uniform layers.

Electric Field-aided Selective Activation for Indium-Gallium-Zinc-Oxide Thin Film Transistors.

A new technique is proposed for the activation of low temperature amorphous InGaZnO thin film transistor (a-IGZO TFT) backplanes through application of a bias voltage and annealing at 130 °C simultaneously. In this 'electrical activation', the effects of annealing under bias are selectively focused in the channel region. Therefore, electrical activation can be an effective method for lower backplane processing temperatures from 280 °C to 130 °C. Devices fabricated with this method exhibit equivalent electrical properties to those of conventionally-fabricated samples. These results are analyzed electrically and thermodynamically using infrared microthermography. Various bias voltages are applied to the gate, source, and drain electrodes while samples are annealed at 130 °C for 1 hour. Without conventional high temperature annealing or electrical activation, current-voltage curves do not show transfer characteristics. However, electrically activated a-IGZO TFTs show superior electrical characteristics, comparable to the reference TFTs annealed at 280 °C for 1 hour. This effect is a result of the lower activation energy, and efficient transfer of electrical and thermal energy to a-IGZO TFTs. With this approach, superior low-temperature a-IGZO TFTs are fabricated successfully.

High-pressure Gas Activation for Amorphous Indium-Gallium-Zinc-Oxide Thin-Film Transistors at 100 °C.

We investigated the use of high-pressure gases as an activation energy source for amorphous indium-gallium-zinc-oxide (a-IGZO) thin film transistors (TFTs). High-pressure annealing (HPA) in nitrogen (N2) and oxygen (O2) gases was applied to activate a-IGZO TFTs at 100 °C at pressures in the range from 0.5 to 4 MPa. Activation of the a-IGZO TFTs during HPA is attributed to the effect of the high-pressure environment, so that the activation energy is supplied from the kinetic energy of the gas molecules. We reduced the activation temperature from 300 °C to 100 °C via the use of HPA. The electrical characteristics of a-IGZO TFTs annealed in O2 at 2 MPa were superior to those annealed in N2 at 4 MPa, despite the lower pressure. For O2 HPA under 2 MPa at 100 °C, the field effect mobility and the threshold voltage shift under positive bias stress were improved by 9.00 to 10.58 cm(2)/V.s and 3.89 to 2.64 V, respectively. This is attributed to not only the effects of the pressurizing effect but also the metal-oxide construction effect which assists to facilitate the formation of channel layer and reduces oxygen vacancies, served as electron trap sites.

Activation of sputter-processed indium-gallium-zinc oxide films by simultaneous ultraviolet and thermal treatments.

Indium-gallium-zinc oxide (IGZO) films, deposited by sputtering at room temperature, still require activation to achieve satisfactory semiconductor characteristics. Thermal treatment is typically carried out at temperatures above 300 °C. Here, we propose activating sputter- processed IGZO films using simultaneous ultraviolet and thermal (SUT) treatments to decrease the required temperature and enhance their electrical characteristics and stability. SUT treatment effectively decreased the amount of carbon residues and the number of defect sites related to oxygen vacancies and increased the number of metal oxide (M-O) bonds through the decomposition-rearrangement of M-O bonds and oxygen radicals. Activation of IGZO TFTs using the SUT treatment reduced the processing temperature to 150 °C and improved various electrical performance metrics including mobility, on-off ratio, and threshold voltage shift (positive bias stress for 10,000 s) from 3.23 to 15.81 cm(2)/Vs, 3.96 × 10(7) to 1.03 × 10(8), and 11.2 to 7.2 V, respectively.

Highly reliable switching via phase transition using hydrogen peroxide in homogeneous and multi-layered GaZnO(x)-based resistive random access memory devices.

Here, we propose an effective method for improving the resistive switching characteristics of solution-processed gallium-doped zinc oxide (GaZnO(x)) resistive random access memory (RRAM) devices using hydrogen peroxide. Our results imply that solution processed GaZnO(x) RRAM devices could be one of the candidates for the development of low cost RRAM.

Study of nitrogen high-pressure annealing on InGaZnO thin-film transistors.

We studied the effects of high-pressure annealing (HPA) on InGaZnO (IGZO) thin-film transistors (TFTs). HPA was proceeded after TFT fabrication as a post process to improve electrical performance and stability. We used N2 as the pressurized gas. The applied pressures were 1 and 3 MPa at 200 °C. For N2 HPA under 3 MPa at 200 °C, field-effect mobility and the threshold voltage shift under a positive bias temperature stress were improved by 3.31 to 8.82 cm(2)/(V s) and 8.90 to 4.50 V, respectively. The improved electrical performance and stability were due to structural relaxation by HPA, which leads to increased carrier concentration and decreased oxygen vacancy.

Enhanced electrical characteristics and stability via simultaneous ultraviolet and thermal treatment of passivated amorphous In-Ga-Zn-O thin-film transistors.

We developed a method to improve the electrical performance and stability of passivated amorphous In-Ga-Zn-O thin-film transistors by simultaneous ultraviolet and thermal (SUT) treatment. SUT treatment was carried out on fully fabricated thin-film transistors, including deposited source/drain and passivation layers. Ultraviolet (UV) irradiation disassociated weak and diatomic chemical bonds and generated defects, and simultaneous thermal annealing rearranged the defects. The SUT treatment promoted densification and condensation of the channel layer by decreasing the concentration of oxygen-vacancy-related defects and increasing the concentration of metal-oxide bonds. The SUT-treated devices exhibited improved electrical properties compared to nontreated devices: field-effect mobility increased from 5.46 to 13.36 V·s, sub-threshold swing decreased from 0.49 to 0.32 V/decade, and threshold voltage shift (for positive bias temperature stress) was reduced from 5.1 to 1.9 V.