Forming-Free, Low-Voltage, and High-Speed Resistive Switching in Ag/Oxygen-Deficient Vanadium Oxide(VOx)/Pt Device through Two-Step Resistance Change by Ag Filament Formation.

Forming-free, low-voltage, and high-speed resistive switching is demonstrated in an Ag/oxygen-deficient vanadium oxide (VOx)/Pt device via the facilitated formation and rupture of Ag filaments. Direct current (DC) voltage sweep measurements exhibit forming-free switching from a high-resistance state (HRS) to a low-resistance state (LRS), called SET, at an average VSET of +0.23 V. The reverse RESET transition occurs at an average VRESET of -0.07 V with a low RESET current of <1 mA. Reversible switching operations are stable with an HRS/LRS resistance ratio >103 during repeated measurements for thousands of cycles. In pulse measurements, switching occurs within 100 ns at an amplitude of +1.5 V. Notably, a two-step resistance change is observed in the SET operation, where the resistance first partially decreases due to Ag+ ion accumulation in VOx and then further decreases to the LRS after hundreds of nanoseconds upon complete filament formation. The VOx layer deposited to be mostly amorphous with oxygen deficiency from V2O5 has abundant vacancies and expedites Ag+ ion migration, thus realizing forming-free, high-speed, and low-voltage switching. These characteristics of the facilitated Ag filament formation using the substoichiometric VOx layer are highly beneficial for use as stand-alone nonvolatile memory and in-memory computing elements.

Enhanced linear and symmetric synaptic weight update characteristics in a Pt/p-LiCoOx/p-NiO/Pt memristor through interface energy barrier modulation by Li ion redistribution.

Artificial synaptic devices have been extensively investigated for neuromorphic computing systems, which require synaptic behaviors mimicking the biological ones. In particular, a highly linear and symmetric weight update with a conductance (or resistance) change for potentiation and depression operation is one of the essential requirements for energy-efficient neuromorphic computing; however, it is not sufficiently met. In this study, a memristor with a Pt/p-LiCoOx/p-NiO/Pt structure is investigated, where a low interface energy barrier between the Pt electrode and the NiO layer makes for a more linear and symmetric conductance change. In addition, the use of voltage-driven Li+ ion redistribution in the NiO layer facilitates the analog conductance change at a low voltage. Besides the linear and symmetric potentiation and depression weight updates, the memristor exhibits various synaptic characteristics such as the dependence of weight update on the pulse amplitude and number, paired pulse facilitation, and short-term and long-term plasticity. The conductance modulation is thought to be induced by a tunable interface energy barrier at the NiO layer and Pt bottom electrode, as a result of Li+ ion diffusion in NiO supplied from the LiCoOx layer and their redistribution. Thanks to the use of Li+ ion redistribution, the conductance change could be achieved at a voltage <4 V within the time of µs range. These results verify the potential of artificial synapses with the Pt/LiCoOx/NiO/Pt memristor operated by voltage-driven Li+ ion redistribution under the low interface energy barrier conditions, realizing a highly linear and symmetric weight update at a low voltage with a high speed for energy-efficient neuromorphic computing systems.

Nanoscale Vertical Resolution in Optical Printing of Inorganic Nanoparticles.

Direct optical printing of functional inorganics shows tremendous potential as it enables the creation of intricate two-dimensional (2D) patterns and affordable design and production of various devices. Although there have been recent advancements in printing processes using short-wavelength light or pulsed lasers, the precise control of the vertical thickness in printed 3D structures has received little attention. This control is vital to the diverse functionalities of inorganic thin films and their devices, as they rely heavily on their thicknesses. This lack of research is attributed to the technical intricacy and complexity involved in the lithographic processes. Herein, we present a generalized optical 3D printing process for inorganic nanoparticles using maskless digital light processing. We develop a range of photocurable inorganic nanoparticle inks encompassing metals, semiconductors, and oxides, combined with photolinkable ligands and photoacid generators, enabling the direct solidification of nanoparticles in the ink medium. Our process creates complex and large-area patterns with a vertical resolution of ∼50 nm, producing 50-nm-thick 2D films and several micrometer-thick 3D architectures with no layer height difference via layer-by-layer deposition. Through fabrication and operation of multilayered switching devices with Au electrodes and Ag-organic resistive layers, the feasibility of our process for cost-effective manufacturing of multilayered devices is demonstrated.

Linear and symmetric synaptic weight update characteristics by controlling filament geometry in oxide/suboxide HfOx bilayer memristive device for neuromorphic computing.

Memristive devices have been explored as electronic synaptic devices to mimic biological synapses for developing hardware-based neuromorphic computing systems. However, typical oxide memristive devices suffered from abrupt switching between high and low resistance states, which limits access to achieve various conductance states for analog synaptic devices. Here, we proposed an oxide/suboxide hafnium oxide bilayer memristive device by altering oxygen stoichiometry to demonstrate analog filamentary switching behavior. The bilayer device with Ti/HfO2/HfO2-x(oxygen-deficient)/Pt structure exhibited analog conductance states under a low voltage operation through controlling filament geometry as well as superior retention and endurance characteristics thanks to the robust nature of filament. A narrow cycle-to-cycle and device-to-device distribution were also demonstrated by the filament confinement in a limited region. The different concentrations of oxygen vacancies at each layer played a significant role in switching phenomena, as confirmed through X-ray photoelectron spectroscopy analysis. The analog weight update characteristics were found to strongly depend on the various conditions of voltage pulse parameters including its amplitude, width, and interval time. In particular, linear and symmetric weight updates for accurate learning and pattern recognition could be achieved by adopting incremental step pulse programming (ISPP) operation scheme which rendered a high-resolution dynamic range with linear and symmetry weight updates as a consequence of precisely controlled filament geometry. A two-layer perceptron neural network simulation with HfO2/HfO2-x synapses provided an 80% recognition accuracy for handwritten digits. The development of oxide/suboxide hafnium oxide memristive devices has the capacity to drive forward the development of efficient neuromorphic computing systems.

Electroforming-free threshold switching of NbO x -based selector devices by controlling conducting phases in the NbO x layer for the application to crossbar array architectures.

Bipolar threshold switching characteristics, featuring volatile transition between the high-resistance state (HRS) at lower voltage than threshold voltage (V th) and the low-resistance state (LRS) at higher voltage irrespective of the voltage polarity, are investigated in the Nb(O)/NbO x /Nb(O) devices with respect to deposition and post-annealing conditions of NbO x layers. The device with NbO x deposited by reactive sputtering with 12% of O2 gas mixed in Ar shows threshold switching behaviors after electroforming operation at around +4 V of forming voltage (V f). On the other hand, electroforming-free threshold switching is achieved from the device with NbO x deposited in the reduced fraction of 7% of O2 gas and subsequently annealed at 250 °C in vacuum, thanks to the increase of the amount of conducting phases within the NbO x layer. Threshold switching is thought to be driven by the formation of a temporally percolated filament composed of conducting NbO and NbO2 phases in the NbO x layer, which were formed as a result of the interaction with Nb electrodes such as oxygen ion migration either by annealing or electrical biasing. The presence of a substantial amount of oxygen in the Nb electrodes up to ∼40 at%, named Nb(O) herein, would alleviate excessive migration of oxygen and consequent overgrowth of the filament during operation, thus enabling reliable threshold switching. These results demonstrate a viable route to realize electroforming-free threshold switching in the Nb(O)/NbO x /Nb(O) devices by controlling the contents of conducting phases in the NbO x layer for the application to selector devices in high-density crossbar memory and synapse array architectures.

Wide range modulation of synaptic weight in thin-film transistors with hafnium oxide gate insulator and indium-zinc oxide channel layer for artificial synapse application.

Wide range synaptic weight modulation with a tunable drain current was demonstrated in thin-film transistors (TFTs) with a hafnium oxide (HfO2-x) gate insulator and an indium-zinc oxide (IZO) channel layer for application to artificial synapses in neuromorphic systems. The drain current in these TFTs was reduced significantly by four orders of magnitude on application of a negative gate bias, then could be restored to its original value by applying a positive bias. The reduced drain current under negative biasing is interpreted as being caused by voltage-driven oxygen ion migration from the HfO2-x gate insulator to the IZO channel, which reduces the oxygen vacancy concentration in the IZO channel. In addition to emulating the analog-type potentiation and depression motions in artificial synapses, the tunable drain current presents paired-pulse facilitation and short-term and long-term plasticity behaviors. These wide-ranging and nonvolatile synaptic behaviors with tunable drain currents are indicative of the potential of the proposed TFTs for artificial synapse applications.

Analog Memristive Characteristics of Square Shaped Lanthanum Oxide Nanoplates Layered Device.

Square-shaped or rectangular nanoparticles (NPs) of lanthanum oxide (LaOx) were synthesized and layered by convective self-assembly to demonstrate an analog memristive device in this study. Along with non-volatile analog memory effect, selection diode property could be co-existent without any implementation of heterogeneous multiple stacks with ~1 µm thick LaOx NPs layer. Current-voltage (I-V) behavior of the LaOx NPs resistive switching (RS) device has shown an evolved current level with memristive behavior and additional rectification functionality with threshold voltage. The concurrent memristor and diode type selector characteristics were examined with electrical stimuli or spikes for the duration of 10-50 ms pulse biases. The pulsed spike increased current levels at a read voltage of +0.2 V sequentially along with ±7 V biases, which have emulated neuromorphic operation of long-term potentiation (LTP). This study can open a new application of rare-earth LaOx NPs as a component of neuromorphic synaptic device.

Effect of the Bilayer Period of Atomic Layer Deposition on the Growth Behavior and Electrical Properties of the Amorphous In-Zn-O Film.

This study reports on the effect of a bilayer period on the growth behavior, microstructure evolution, and electrical properties of atomic layer deposition (ALD) deposited In-Zn-O (IZO) films, fixing the ALD cycle ratio of In-O/Zn-O as 9:1. Here, the bilayer period is defined as the total number of ALD cycles in one supercycle of In-O and Zn-O by alternately stacking Zn-O and In-O layers at a temperature of 220 °C. IZO films with a bilayer period from 10 to 40 cycles, namely, IZO[In-O/Zn-O = 9:1] to IZO[36:4], result to form an amorphous phase with a resistivity of 4.94 × 10-4 Ω·cm. However, by increasing the bilayer period above 100 cycles, the IZO films begin to form a mixed amorphous-nanocrystalline microstructure, resulting from the limited intermixing at the interfaces. Concomitantly, the overall film resistivity is considerably increased with a simultaneous decrease in both the carrier mobility and the concentration. These results not only reveal the importance of the bilayer period in designing the ALD stacking sequence in the ALD-IZO, but also provide the possibility of forming various multilayered materials with different electrical properties.

Enhancement of cortisol measurement sensitivity by laser illumination for AlGaN/GaN transistor biosensor.

In this study, high electron mobility transistor (HEMT) device was used as an immuno biosensor to measure concentration of a stress hormone, cortisol, by using selective binding on cortisol monoclonal antibody (c-Mab). Also, the HEMT sensor was enhanced in its sensitivity through light illumination to generate photocurrent. The optical pumping could assist the biosensor to discriminate more detailed change, which could result in an increment of limit of detection (LOD) to 1.0 pM cortisol level. It was the lowest level of detection with semiconductor device-based cortisol biosensors and the enhancement of surface potential sensitivity was induced by laser light (532 nm). Output current amplificated by photocurrent was higher than dark original current at about 3.39% when gate voltage is applied with -3 V. Since the device could be applied to not only standard cortisol solution but also real human salivary sample, it is expected to apply for in vitro direct diagnosis of point-of-care test (POCT).

Effect of nitrogen-doping on drain current modulation characteristics of an indium-gallium-zinc oxide thin-film transistor.

The effect of nitrogen-doping (N-doping) in an indium-gallium-zinc oxide (IGZO) channel layer on the analog, linear, and reversible drain current modulation in thin-film transistors (TFTs) with Al-top-gate/SiOx/TaOx/IGZO stack is investigated for potential application to artificial synaptic devices. The N-doped devices exhibit a more linear increase of drain current upon repeating positive gate biasing, corresponding to synaptic potentiation, while the undoped device shows a highly non-linear and abrupt increase of drain current. Distinct from the increase of drain current at positive biasing for potentiation, the decrease of drain current for depression behavior at negative biasing is found to be the same. Whereas the increase of drain current becomes more linear, the channel conductance, the magnitude of its change, and its changing speed are decreased by the N-doping. The partial replacement of oxygen with nitrogen, having higher binding energy with metal-cations, suppresses oxygen vacancy formation, then decreases the channel conductance. It also retards the migration of oxygen ions, then leads to a linear increase of drain current. These results reveal that the characteristics of tunable drain current such as its linearity, dynamic range, and speed could be controlled by altering the internal state of the IGZO channel, which is crucial for application to an artificial synapse in a neuromorphic system.