Amorphous Indium Oxide Research Articles

The Electronic Impact of X-Ray on Atomically-Thin Oxide Semiconductor Devices

In the past few years, there has been a significant emphasis on atomically-thin metal oxide semiconductors (OS), driven by their adjustable electrical properties that open up a range of electronic applications [1.2]. However, the mechanisms of transport and electronic tunability in OS remain unclear [3]. X-ray characterization techniques, i.e. X-ray photoelectron spectroscopy (XPS) and X-ray diffractometer (XRD), are considered as non-destructive and are widely used to quantify the chemical and electronic state of OS. In this work, we discovered that X-ray has significant impact on the electronic properties of OS. We observed that low energy X-ray (<2 keV) induces a negative V T offset in OS devices [4]. The variation in V T primarily originates from the chemical interaction of oxygen molecules on the channel surface. OS devices absorb the low-energy X-ray, generating the holes, and they subsequently react with O2 - on the channel surface, resulting in the production of oxygen and its removal from the channel surface, as shown in Fig 1a. The V T shift caused by low energy X-ray will recover in air over time, as illustrated in Fig 1b. We incorporated the post low-energy X-ray devices into a vacuum environment with a pressure of 10-6 torr, and the V T of the device exhibited no recovery over time, providing additional support for oxygen absorption mechanism. Time-resolved electrical measurements conducted in different atmospheric conditions reveal that the variations in V T arise from the oxygen absorption mechanism. The research highlights the effect of X-ray on OS and analyzes the mechanism behind the increase in OS carrier concentration induced by the X-ray exposure.[1] Si, M. et al. Scaled indium oxide transistors fabricated using atomic layer deposition. Nat. Electron. 5, 164–170 (2022).[2] Charnas, Adam, et al. Extremely Thin Amorphous Indium Oxide Transistors. Adv. Mater. 2304044 (2023).[3] Conley, J. F. Instabilities in amorphous oxide semiconductor thin-film transistors. IEEE Trans. Device Mater. Rel. 10, 460–475 (2010).[4] Tseng, R., Wang, ST., Ahmed, T. et al. Wide-range and area-selective threshold voltage tunability in ultrathin indium oxide transistors. Nat. Commun. 14, 5243 (2023). Figure 1

Trio strategy of harmonizing electronic structure, interface, and microenvironment on amorphous indium oxide nanofiber for selective electrochemical ammonia synthesis

Suppressing parasitic hydrogen evolution reaction (HER) remains a dilemma in developing aqueous electrochemical nitrogen reduction reaction (NRR). Nevertheless, previous studies have revealed the significant challenge of relying solely on electrocatalyst design to pursue selective NRR. Herein, we present a ‘Trio’ strategy to harmonize electronic structures of electrocatalysts, properties of interfaces, and configurations of microenvironments, thereby governing the intricate proton behaviors throughout the reaction, to suppress HER while boosting NRR. As proof-of-concept demonstration, the first designed amorphous In2O3-based nanofiber electrocatalyst, with optimized electronic state by oxygen vacancy and anchoring Mo species, is in conjunction with low-surface-energy monolayer interface and molecular-crowding microenvironment. Such rational synergy creates an advantageous catalytic configuration with decelerated proton diffusion and restricted proton transfer to active sites, thus achieving NH3 yield of 59.72 μg h−1 mg−1 and a FE of 30.60 %. We expect these findings will inspire “collaborative combat” strategies and desirable systems of NRR in the future.

Nucleation and grain growth in low-temperature rapid solid-phase crystallization of hydrogen-doped indium oxide

Nucleation and grain growth are discussed as a means of clarifying the mechanism of the rapid solid-phase crystallization (SPC) process of H2-doped amorphous indium oxide (InO x :H) films. H2-doping in InO x :H films reduced nucleation density at 250 °C from 4.1 to 1.1 μm−2, resulting in an increase in grain size and Hall mobility of the polycrystalline (poly)-InO x :H films. Lateral growth rate from the nucleus was estimated to be 220 nm min−1 for the InO x :H film at 250 °C. Thus, an amorphous InO x :H film could be converted to a poly-InO x :H film within 3 min owing to a fast lateral growth rate from the nucleus. Almost the same grain size, Hall mobility, and carrier density could be obtained from the poly-InO x :H films after annealing at 250 °C for only 3 min irrespective of the ramp rate. The results demonstrated the wide range of the processing window for SPC for poly-InO x :H films.

1/f Noise During Thermal Treatment of Amorphous Films

Flicker noise is a sensitive tool for probing the dynamics of two‐level systems. Herein, this technique is employed to study the dependence of conductance noise on disorder for two versions of amorphous indium oxide films. The disorder in these substances may be tuned by thermal treatment that is manifested by enhanced conductivity. Structural studies reveal that this is mainly due to densification of the material. A similar reduction of volume has been achieved in glasses when subjected to high pressures. Both protocols, pressure and heat treatment, initiate nonequilibrium state that slowly relaxes. This relaxation is reflected in the sample conductivity and its optical transmission as a monotonic change. The magnitude of 1/f noise during these events turns out to fluctuate appreciably following changes in the sample conductance caused by thermal treatment. This may overshadow the tendency of the noise level to increase with disorder. Possible reasons for the fluctuations of noise levels in highly disordered systems are discussed.

Excess noise in the anomalous metallic phase in amorphous indium oxide

Excess noise in the anomalous metallic phase in amorphous indium oxide

Atomically Thin Amorphous Indium-Oxide Semiconductor Film Developed Using a Solution Process for High-Performance Oxide Transistors.

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.

Role of morphology in defect formation and photo-induced carrier instabilities in amorphous indium oxide

Ab initio molecular dynamics liquid-quench simulations and hybrid density functional calculations are performed to model the effects of room-temperature atomic fluctuations and photo-illumination on the structural and electronic properties of amorphous sub-stoichiometric In2O2.96. A large configurational ensemble is employed to reliably predict the distribution of localized defects as well as their response to the thermal and light activation. The results reveal that the illumination effects on the carrier concentration are greater in amorphous configurations with shorter In–O bond length and reduced polyhedral sharing as compared to the structures with a more uniform morphology. The obtained correlation between the photo-induced carrier density and the reduction in the number of fully coordinated In-atoms implies that metal oxides with a significant fraction of crystalline/amorphous interfaces would show a more pronounced response to illumination. Photo-excitation also produces In–O2–In defects that have not been previously found in sub-stoichiometric amorphous oxides; these defects are responsible for carrier instabilities due to overdoping.

Fluoride Doping in Crystalline and Amorphous Indium Oxide Semiconductors

Fluoride Doping in Crystalline and Amorphous Indium Oxide Semiconductors

High mobility silicon indium oxide thin-film transistor fabrication by sputtering process

Amorphous silicon indium oxide (a-ISO) thin-films were deposited by sputtering process at room temperature for thin-film transistor (TFT) active channel applications. The amorphous nature of the deposited ISO thin films was confirmed by structural analysis and the films had an average surface roughness of ∼0.11 nm. The oxygen partial pressure was varied from 0 to 20% to deposit ISO active channel layers which showed a transition from conducting to semiconducting behaviour. The a-ISO TFT deposited with 5% oxygen partial pressure and post annealed at 100 °C exhibits a saturation mobility of 31.7 cm2/V.s, on-off current ratio of 2.3 × 1010, turn-on voltage of −5 V and sub-threshold swing of 0.25 V/dec. Bias stress analysis further confirms the stable operation of the ISO TFT devices. Silicon dopant acts as a strong carrier suppressor and enhances performance of a-ISO TFT devices.

Metallic networks and hydrogen compensation in highly nonstoichiometric amorphous In2O3−x

The unique response of amorphous ionic oxides to changes in oxygen stoichiometry is investigated using computationally intensive ab initio molecular dynamics simulations, comprehensive structural analysis, and hybrid density-functional calculations for the oxygen defect formation energy and electronic properties of amorphous ${\mathrm{In}}_{2}{\mathrm{O}}_{3\ensuremath{-}x}$ with $x=0$--0.185. In marked contrast to nonstoichiometric crystalline nanocomposites with clusters of metallic inclusions inside an insulating matrix, the lack of oxygen in amorphous indium oxide is distributed between a large fraction of undercoordinated In atoms, leading to an extended shallow state for $x&lt;0.037$, a variety of weakly and strongly localized states for $0.074&lt;x&lt;0.148$, and a percolation-like network of single-atom chains of metallic In-In bonds for $x&gt;0.185$. The calculated carrier concentration increases from $3.3\ifmmode\times\else\texttimes\fi{}{10}^{20}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$ at $x=0.037$ to $6.6\ifmmode\times\else\texttimes\fi{}{10}^{20}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$ at $x=0.074$ and decreases only slightly at lower oxygen content. At the same time, the density of deep defects located between 1 and 2.5 eV below the Fermi level increases from $0.4\ifmmode\times\else\texttimes\fi{}{10}^{21}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$ at $x=0.074$ to $2.2\ifmmode\times\else\texttimes\fi{}{10}^{21}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}3}$ at $x=0.185$. The wide range of localized gap states associated with various spatial distributions and individual structural characteristics of undercoordinated In is passivated by hydrogen that helps enhance electron velocity from $7.6\ifmmode\times\else\texttimes\fi{}{10}^{4}$ to $9.7\ifmmode\times\else\texttimes\fi{}{10}^{4}$ m/s and restore optical transparency within the visible range; H doping is also expected to improve the material's stability under thermal and bias stress.

Electron glass signatures up to room temperature in disordered insulators

This paper describes the observation of non-equilibrium field effects at room temperature in four disordered insulating systems: granular Al, discontinuous Au, amorphous NbSi and amorphous indium oxide thin films. The use of wide enough gate voltage ranges and a cautious analysis of the data allow us to uncover memory dips (MDs), the advocated hallmark of the electron glass, in the four systems. These MDs are found to relax slowly over days of measurements under gate voltage changes, reflecting the impossibility for the systems to reach an equilibrium state within experimentally accessible times. Our findings demonstrate that these electrical glassy effects, so far essentially reported at cryogenic temperatures, actually extend up to room temperature.

Superconductor–insulator transitions in three-dimensional indium-oxide at high pressures

Experiments investigating magnetic-field-tuned superconductor–insulator transition (HSIT) mostly focus on two-dimensional material systems where the transition and its proximate ground-state phases, often exhibit features that are seemingly at odds with the expected behavior. Here we present a complementary study of a three-dimensional pressure-packed amorphous indium-oxide (InOx) powder where granularity controls the HSIT. Above a low threshold pressure of ∼0.2 GPa, vestiges of superconductivity are detected, although neither a true superconducting transition nor insulating behavior are observed. Instead, a saturation at very high resistivity at low pressure is followed by saturation at very low resistivity at higher pressure. We identify both as different manifestations of anomalous metallic phases dominated by superconducting fluctuations. By analogy with previous identification of the low resistance saturation as a ‘failed superconductor’, our data suggests that the very high resistance saturation is a manifestation of a ‘failed insulator’. Above a threshold pressure of ∼6 GPa, the sample becomes fully packed, and superconductivity is robust, with T C tunable with pressure. A quantum critical point at P C ∼ 25 GPa marks the complete suppression of superconductivity. For a finite pressure below P C, a magnetic field is shown to induce a HSIT from a true zero-resistance superconducting state to a weakly insulating behavior. Determining the critical field, H C, we show that similar to the 2D behavior, the insulating-like state maintains a superconducting character, which is quenched at higher field, above which the magnetoresistance decreases to its fermionic normal state value.

Electron glass effects in amorphous NbSi films

We report on non equilibrium field effect in insulating amorphous NbSi thin films having different Nb contents and thicknesses. The hallmark of an electron glass, namely the logarithmic growth of a memory dip in conductance versus gate voltage curves, is observed in all the films after a cooling from room temperature to 4.2~K. A very rich phenomenology is demonstrated. While the memory dip width is found to strongly vary with the film parameters, as was also observed in amorphous indium oxide films, screening lengths and temperature dependence of the dynamics are closer to what is observed in granular Al films. Our results demonstrate that the differentiation between continuous and discontinuous systems is not relevant to understand the discrepancies reported between various systems in the electron glass features. We suggest instead that they are not of fundamental nature and stem from differences in the protocols used and in the electrical inhomogeneity length scales within each material.

0.7-GHz Solution-Processed Indium Oxide Rectifying Diodes

Solution-based deposition, with its simplicity and possibility for upscaling through printing, is a promising process for low-cost electronics. Metal oxide semiconductor devices, especially indium oxide with its excellent electrical properties, offer high performance compared to amorphous Si-based rivals, and with a form factor conducive to flexible and wearable electronics. Here, rectifying diodes based on an amorphous spin-coated indium oxide are fabricated for high-speed applications. We report a solution-processed diode approaching the UHF range, based on indium oxide, with aluminum and gold as the electrodes. The device was spin-coated from a precursor material and configured into a half-wave rectifier. The J-V and frequency behavior of the diodes were studied, and the material composition of the diode was investigated by X-ray photoemission spectroscopy (XPS). The 3-dB point was found to be over 700 MHz. The results are promising for the development of autonomously powered wireless Internetof-Things systems based on scalable, low-cost processes.

Structural Dynamics in Thermal Treatment of Amorphous Indium Oxide Films

Thermal treatment of amorphous indium oxide (InxO) films is used in various basic studies as a means of tuning the disorder perceived by the electronic system. In this process, the resistance of a given sample decreases, whereas its amorphous structure and chemical composition is preserved. The main effect of the process is an increase in the system density, which, in turn, leads to improved interatomic overlap manifested as improved conductivity. A similar effect has been observed in studies of other amorphous systems that were subjected to pressure. Herein, the Raman spectra of amorphous InxO change in response to thermal treatment in a similar way as in pressure experiments performed on other disordered and amorphous systems. A study of how thermal treatment changes the system dynamics is presented by monitoring the resistance versus time of InxO films following various stages of thermal treatment. The time dependence of the sample resistance fits the stretched exponential law with parameters that change systematically with repeated thermal treatment cycles. The implications of these results to slow dynamics phenomena that are governed by the Kohlrausch's law are discussed.

Effect of Zinc Oxide Modification by Indium Oxide on Microstructure, Adsorbed Surface Species, and Sensitivity to CO

Additives in semiconductor metal oxides are commonly used to improve sensing behavior of gas sensors. Due to complicated effects of additives on the materials microstructure, adsorption sites and reactivity to target gases the sensing mechanism with modified metal oxides is a matter of thorough research. Herein, we establish the promoting effect of nanocrystalline zinc oxide modification by 1 – 7 at.% of indium on the sensitivity to CO gas due to improved nanostructure dispersion and concentration of active sites. The sensing materials were synthesized via an aqueous coprecipitation route. Materials composition, particle size and BET area were evaluated using X-ray diffraction, nitrogen adsorption isotherms, high-resolution electron microscopy techniques and EDX-mapping. Surface species of chemisorbed oxygen, OH-groups and acid sites were characterized by probe molecule techniques and infrared spectroscopy. Zinc oxide particle size was found to decrease and the BET area to increase with the amount of indium. The additive was observed in the form of amorphous indium oxide segregated on agglomerated crystalline ZnO nanoparticles. The concentration of surface species was found to be higher on In-modified zinc oxide. With the increase of indium content, the sensor response of ZnO(In) to CO was improved. Using in situ infrared spectroscopy, it was shown that oxidation of CO molecules was enhanced on the modified zinc oxide surface. The effect of modifier was attributed to promotion of surface OH-groups and enhancement of CO oxidation on the segregated indium ions, as suggested by DFT in previous work.

Infinite-randomness fixed point of the quantum superconductor-metal transitions in amorphous thin films

The magnetic-field-tuned quantum superconductor-insulator transitions of disordered amorphous indium oxide films are a paradigm in the study of quantum phase transitions, and exhibit power-law scaling behavior. For superconducting indium oxide films with low disorder, such as the ones reported on here, the high-field state appears to be a quantum-corrected metal. Resistance data across the superconductor-metal transition in these films are shown here to obey an activated scaling form appropriate to a quantum phase transition controlled by an infinite randomness fixed point in the universality class of the random transverse-field Ising model. Collapse of the field-dependent resistance vs. temperature data is obtained using an activated scaling form appropriate to this universality class, using values determined through a modified form of power-law scaling analysis. This exotic behavior of films exhibiting a superconductor-metal transition is caused by the dissipative dynamics of superconducting rare regions immersed in a metallic matrix, as predicted by a recent renormalization group theory. The smeared crossing points of isotherms observed are due to corrections to scaling which are expected near an infinite randomness critical point, where the inverse disorder strength acts as an irrelevant scaling variable.

Synergistic combination of amorphous indium oxide with tantalum pentoxide for efficient electron transport in low-power electronics

High-quality amorphous indium oxide thin films are obtained by exploiting a synergistic interaction with an underlying tantalum pentoxide layer.

Collective energy gap of preformed Cooper pairs in disordered superconductors

In most superconductors the transition to the superconducting state is driven by the binding of electrons into Cooper-pairs. The condensation of these pairs into a single, phase coherent, quantum state takes place concomitantly with their formation at the transition temperature, $T_c$. A different scenario occurs in some disordered, amorphous, superconductors: Instead of a pairing-driven transition, incoherent Cooper pairs first pre-form above $T_c$, causing the opening of a pseudogap, and then, at $T_c$, condense into the phase coherent superconducting state. Such a two-step scenario implies the existence of a new energy scale, $\Delta_{c}$, driving the collective superconducting transition of the preformed pairs. Here we unveil this energy scale by means of Andreev spectroscopy in superconducting thin films of amorphous indium oxide. We observe two Andreev conductance peaks at $\pm \Delta_{c}$ that develop only below $T_c$ and for highly disordered films on the verge of the transition to insulator. Our findings demonstrate that amorphous superconducting films provide prototypical disordered quantum systems to explore the collective superfluid transition of preformed Cooper-pairs pairs.

Low-temperature anomaly in disordered superconductors near B c2 as a vortex-glass property.

Strongly disordered superconductors in a magnetic field display many characteristic properties of type-II superconductivity—except at low temperatures, where an anomalous linear temperature dependence of the resistive critical field Bc2 is routinely observed. This behavior violates the conventional theory of superconductivity, and its origin has posed a long-standing puzzle. Here we report systematic measurements of the critical magnetic field and current on amorphous indium oxide films with various levels of disorder. Surprisingly, our measurements show that the Bc2 anomaly is accompanied by mean-field-like scaling of the critical current. Based on a comprehensive theoretical study we argue that these observations are a consequence of the vortex-glass ground state and its thermal fluctuations. Our theory further predicts that the linear-temperature anomaly occurs more generally in both films and disordered bulk superconductors, with a slope that depends on the normal-state sheet resistance, which we confirm experimentally.