Nonvolatile Resistive Switching Research Articles

Nonvolatile ferroelectric resistive switching in α-In2Se3(2H) ferroelectric semiconductor junctions

Emerging two-dimensional van der Waals (vdW) based ferroelectric semiconductor junctions (FSJs) are promising for low-power and high-density applications. In this work, we report the vdW α-In2Se3(2H) based FSJs of different metal-In2Se3 interfaces. All vertical devices emerge with the nonvolatile ferroelectric resistive switching behavior. The Cr/α-In2Se3(2H)/Au FSJs show a typical ferroelectric resistive switching behavior under ∼1.0 V applied voltage. The switching voltage of the Ag/α-In2Se3(2H)/Au FSJs could be further decreased from 1.0 V to 0.8 V because of Ag migrations and ferroelectric reversal. Further, by optimizing the metal-In2Se3 interfaces, the Ag/α-In2Se3(2H)/Pt FSJs exhibit the ultralow switching voltage (∼0.3 V), excellent endurance (>225 cycles) and retention (>1 × 104 s). The results suggest that vdW α-In2Se3(2H) ferroelectric has great potential for low-power memristive devices.

Modified Donor End Caps for Binary-to-Ternary WORM Memory Conversion in N-Heteroaromatic Systems.

A series of novel D-π-A type organic small molecules have been designed, synthesized, and demonstrated for non-volatile resistive switching WORM memory application. The electron-deficient phenazine and quinoxaline units were coupled with various functionalized triphenylamine end caps to explore the structure-property correlations. The photophysical investigations displayed considerable intramolecular charge transfer, and the electrochemical analysis revealed an optimum band gap of 2.44 to 2.83 eV. These factors and the thin film morphological studies suggest the feasibility of the compounds as better resistive memory devices. All the compounds indicated potent non-volatile resistive switching memory capabilities with ON/OFF ratios ranging from 103 to 104, and the lowest threshold voltage recorded stands at -0.74 V. A longer retention time of 103 s marks the substantial stability of the devices. The phenazine-based compounds outperformed the others in terms of memory performance. Exceptionally, the compound with -CHO substituted triphenylamine exhibited ternary memory performance owing to its multiple traps. The resistive switching mechanism for the devices was validated using density functional theory calculations, which revealed that the integrated effect of charge transfer and charge trapping contributes significantly to the resistive switching phenomena.

Study on multifunctional resistive switching and UV light detection characteristics in p-PEDOT:PSS/i-BFO/n-ZnO hybrid structures

The present research work based on the newly prepared organic-inorganic hybrid heterostructure will be exploited to develop a multifunctional device including non-volatile resistance switching memory devices, and ultraviolet (UV) light detection behavior for the first time based on p-PEDOT:PSS/i-BFO/n-ZnO junctions. Using a spray pyrolysis technique, n-type zinc oxide (ZnO) and i-type bismuth ferrite (BiFeO3) thin film layers were prepared on the clean glass substrates at temperature 673 K. Using a spin coater method, the p-PEDOT:PSS were grown upon a bismuth ferrite (BiFeO3) thin film with a constant spin velocity of 2000 rpm and heated at 363 K. The current (I)–voltage (V), photoresponse characteristics and resistive switching (RS) behavior of the fabricated p-PEDOT:PSS/i-BFO/n-ZnO hybrid devices were carried out. The device shows high photoresponsivity (R) of 0.001 285 A W−1 and fast photoresponse switching speed with the measured rise and fall time of 493 and 970 ms respectively. Based on the electrical properties, a conductive filament formation/rupture mechanism is proposed to explain the observed RS characteristics.

Building Uniformly Structured Polymer Memristors via a 2D Conjugation Strategy for Neuromorphic Computing.

Polymer memristors represent a highly promising avenue for the advancement of next-generation computing systems. However, the intrinsic structural heterogeneity characteristic of most polymers often results in organic polymer memristors displaying erratic resistive switching phenomena, which in turn lead to diminished production yields and compromised reliability. In this study, a 2D conjugated polymer, named PBDTT-BPQTPA, is synthesized by integrating the coplanar bis(thiophene)-4,8-dihydrobenzo[1,2-b:4,5-b]dithiophene (BDTT) as an electron-donating unit with a quinoxaline derivative serving as an electron-accepting unit. The incorporation of triphenylamine groups at the quinoxaline termini significantly enhances the polymer's conjugation and planarity, thereby facilitating more efficient charge transport. The fabricated polymer memristor with the structure of Al/PBDTT-BPQTPA/ITO exhibits typical non-volatile resistive switching behavior under high voltage conditions, along with history-dependent memristive properties at lower voltages. The unique memristive behavior of the device enables the simulation of synaptic enhancement/inhibition, learning algorithms, and memory operations. Additionally, the memristor demonstrates its capability for executing logical operations and handling decimal calculations. This study offers a promising and innovative approach for the development of artificial neuromorphic computing systems.

High-performance memristor for energy-efficient artificial optoelectronic synapse based on BiVO4 nanosheets

Artificial optoelectronic synapses have drawn extensive attention owing to their ability to combine the optical and electrical responses. Those photosensitive materials that has been reported in memristors have the potential to be adopted in such optoelectronic synapses. Herein, optoelectronic synapses can be achieved based on two-terminal memristors by using two-dimensional (2D) BiVO4 with monoclinic scheelite (m-BiVO4) structure as the memristive layer. The fabricated memristors exhibit bipolar resistive switching (RS) characteristics with stable retention and reliable endurance performance. Furthermore, both electrical and optical synaptic functions can be achieved based on the memristors, such as long-term potentiation (LTP) and depression (LTD) stimulated by the voltages pulses as well as short-term and long-term memory under the light stimulation. More importantly, owing to the LTP and LTD functions with high symmetry, linearity and good repeatability of the LTP/LTD cycles, the artificial neural network can be simulated to achieve image recognition with a high accuracy for handwritten digits. Moreover, both the electrical and optical synapses can be used to emulate the “learning-forgetting” behaviors of human brain. Remarkably, the energy consumption per synaptic event in the optical and electrical modes can be calculated, indicating potential applications in energy-efficient synaptic devices. The m-BiVO4 nanosheets not only demonstrate good non-volatile RS behaviors but also implement energy-efficient optoelectronic synaptic functions, providing a promising strategy for applications in future neuromorphic computing.

Versatile Cu2ZnSnS4-based synaptic memristor for multi-field-regulated neuromorphic applications.

Integrating both electrical and light-modulated multi-type neuromorphic functions in a single synaptic memristive device holds the most potential for realizing next-generation neuromorphic systems, but is still challenging yet achievable. Herein, a simple bi-terminal optoelectronic synaptic memristor is newly proposed based on kesterite Cu2ZnSnS4, exhibiting stable nonvolatile resistive switching with excellent spatial uniformity and unique optoelectronic synaptic behaviors. The device demonstrates not only low switching voltage (-0.39 ± 0.08V), concentrated Set/Reset voltage distribution (<0.08/0.15V), and long retention time (>104s) but also continuously modulable conductance by both electric (different width/interval/amplitude) and light (470-808nm with different intensity) stimulus. These advantages make the device good electrically and optically simulated synaptic functions, including excitatory and inhibitory, paired-pulsed facilitation, short-/long-term plasticity, spike-timing-dependent plasticity, and "memory-forgetting" behavior. Significantly, decimal arithmetic calculation (addition, subtraction, and commutative law) is realized based on the linear conductance regulation, and high precision pattern recognition (>88%) is well achieved with an artificial neural network constructed by 5 × 5 × 4 memristor array. Predictably, such kesterite-based optoelectronic memristors can greatly open the possibility of realizing multi-functional neuromorphic systems.

Atomic Layer Deposition Films for Resistive Random‐Access Memories

AbstractResistive random‐access memory (RRAM) stands out as a promising memory technology due to its ease of operation, high speed, affordability, exceptional stability, and potential to enable smaller memory devices with sizes under 10 nm. This has drawn significant attention, with atomic layer deposition (ALD) emerging as an ideal technology to tackle the challenges of nanoscale fabrication in the micro‐ and nanomanufacturing industry. ALD offers technological advantages such as functional multiple‐layer stacking, doping capabilities, and incorporating oxygen reservoirs or reactive layers. These factors contribute to achieving more intriguing, stable, and reliable nonvolatile resistance switching behaviors in RRAM. Specifically, ALD greatly benefits RRAM, that relies on the valence change mechanism, where high‐k transition metal oxides are commonly used as switching materials, and precise control over oxygen vacancies is achievable. This review provides a comprehensive overview of ALD films used in RRAM, delves into resistive switching properties and microscopic mechanisms in binary and ternary oxides and nitrides, and explores the impact of ALD‐prepared electrodes. Furthermore, the current status and future prospects of ALD‐based RRAM are highlighted, which is poised to catalyze further advancements in the fields of information storage and neural networks.

Versatile Titanium Carbide MXene Thin-Film Memristors with Adaptive Learning Behavior.

With the advent of the modern era, there is a huge demand for memristor-based neuromorphic computing hardware to overcome the von Neumann bottleneck in traditional computers. Here, we have prepared two-dimensional titanium carbide (Ti3C2Tx) MXene following the conventional HF etching technique in solution. After confirmation of Ti3C2Tx properties by Raman scattering and crystallinity measurements, high-quality thin-film deposition is realized using an immiscible liquid-liquid interfacial growth technique. Following this, the memristor is fabricated by sandwiching a Ti3C2Tx layer with a thickness of 70 nm between two electrodes. Subsequently, current-voltage (I-V) characteristics are measured, revealing a nonvolatile resistive switching property characterized by a swift switching speed of 30 ns and an impressive current On/Off ratio of approximately 103. Furthermore, it exhibits endurance through 500 cycles and retains the states for at least 1 × 104 s without observable degradation. Additionally, it maintains a current On/Off ratio of about 102 while consuming only femtojoules (fJ) of electrical energy per reading. Systematic I-V results and conductive AFM-based current mapping image analysis are converged to support the electroforming mediated filamentary conduction mechanism. Furthermore, our Ti3C2Tx memristor was found to be truly versatile as an all-in-one device for demonstrating edge computation, logic gate operation, and classical conditioning of learning by the brain in Psychology.

Reconfigurable Resistive Switching in VO2/La0.7Sr0.3MnO3/Al2O3 (0001) Memristive Devices for Neuromorphic Computing.

The coexistence of nonvolatile and volatile switching modes in a single memristive device provides flexibility to emulate both neuronal and synaptic functions in the brain. Furthermore, such a device structure may eliminate the need for additional circuit elements such as transistor-based selectors, enabling low-power consumption and high-density device integration in fully memristive spiking neural networks. In this work, we report dual resistive switching (RS) modes in VO2/La0.7Sr0.3MnO3 (LSMO) bilayer memristive devices. Specifically, the nonvolatile RS is driven by the movement of oxygen vacancies (Vo) at the VO2/LSMO interface and requires a higher biasing voltage, whereas the volatile RS is controlled by the metal-insulator transition (MIT) of VO2 under a lower biasing voltage. The simple device structure is electrically driven between the two RS modes and thus can operate as a one selector-one resistor (1S1R) cell, which is a desirable feature in memristive crossbar arrays to avoid the sneak-path current issue. The RS modes are found to be stable and repeatable and can be reconfigured by exploiting the interfacial and phase transition properties, and thus, they hold great promise for applications in memristive neural networks and neuromorphic computing.

Ferroelectric polarization and conductance filament coupling for large window and high-reliability resistive memory and energy-efficient synaptic devices

Ferroelectric capacitors hold great promise for non-volatile memory applications. However, the challenge lies in fabricating resistive switching devices with a high on/off ratio, excellent non-volatility, and a simple manufacturing process. Here, a novel approach is introduced by demonstrating the efficacy of the coupling effect between ferroelectric polarization and oxygen vacancy-based conductive filaments in Hf0.5Zr0.5O2 (HZO) films for the creation of non-volatile resistive switching memory devices, achieving an impressive on/off ratio of 6.8 × 103 at +1.8 V. An in-depth exploration of the resistive switching mechanism is provided and subsequently the outstanding durability and retention characteristics of these devices for resistive switching is validated. Furthermore, the device’s capacity to emulate non-volatile synaptic functionalities is assessed. Our results reveal that under pulsed conditions of 1 V/–2 V with 1 µs pulses spaced 50 ms apart, the device can robustly achieve potentiation/depression synaptic plasticity, while exhibiting energy consumption (0.16 fJ for potentiation, 0.12 fJ for depression) reduced by 1–2 orders of magnitude compared to biological synapses. This work holds significant value as a reference for the fabrication of energy-efficient, non-volatile memory and synaptic devices.

Nanophotonic resistive switch based on tapered copper-silicon structure with low power and high extinction ratio

A non-volatile nanophotonic resistive switch in tapered copper-on-silicon structure is proposed with a potential of electrical writing and optical readout. Incorporating tapered hybrid plasmonic structure in the device enables variable areas of the density of conduction filaments in the direction of optical propagation causing enhanced interaction of light with the lossy metal filaments. The tapered Cu-SiO2-Si is shown to have large optical extinction ratio where high mobility of copper ions in thin SiO2 leads to the low power operation. Optical readout of the resistive switching is demonstrated in the 10 nm thin ion conducting layer (SiO2) at a 1550 nm wavelength with well-defined hysteresis curve. Switching between off and on states is attained by voltage induced annihilation/formation of the nanoscale metal filament inside a thin layer of SiO2 sandwiched between copper and silicon. An optical extinction ratio of 18 dB is reported for a 30 μm long device. In addition, the proposed nanophotonic switch exhibits an intrinsic stochastic property of set voltage reduction in each set-reset cycle. High extinction ratio, reduced set voltage, low power consumption, and non-volatility make the device excellent choice for applications in realizing ultra-compact on-chip devices for optical switching, modulation, and neuromorphic computing.

An analytical approach to engineer multistability in the oscillatory response of a pulse-driven ReRAM

A nonlinear system, exhibiting a unique asymptotic behaviour, while being continuously subject to a stimulus from a certain class, is said to suffer from fading memory. This interesting phenomenon was first uncovered in a non-volatile tantalum oxide-based memristor from Hewlett Packard Labs back in 2016 out of a deep numerical investigation of a predictive mathematical description, known as the Strachan model, later corroborated by experimental validation. It was then found out that fading memory is ubiquitous in non-volatile resistance switching memories. A nonlinear system may however also exhibit a local form of fading memory, in case, under an excitation from a given family, it may approach one of a number of distinct attractors, depending upon the initial condition. A recent bifurcation study of the Strachan model revealed how, under specific train stimuli, composed of two square pulses of opposite polarity per cycle, the simplest form of local fading memory affects the transient dynamics of the aforementioned Resistive Random Access Memory cell, which, would asymptotically act as a bistable oscillator. In this manuscript we propose an analytical methodology, based on the application of analysis tools from Nonlinear System Theory to the Strachan model, to craft the properties of a generalised pulse train stimulus in such a way to induce the emergence of complex local fading memory effects in the nano-device, which would consequently display an interesting tuneable multistable oscillatory response, around desired resistance states. The last part of the manuscript discusses a case study, shedding light on a potential application of the local history erase effects, induced in the device via pulse train stimulation, for compensating the unwanted yet unavoidable drifts in its resistance state under power off conditions.

Hyperbranched polyimide with triazole core structure for nonvolatile resistive switching memory

AbstractHyperbranched polyimides (HBPIs) possess a unique branched structure, which can make the lowest unoccupied molecular orbitals (LUMOs) degenerate and reduce the bandgap between the highest occupied molecular orbital (HOMO) and LUMO energy levels. The triazole group can facilitate the charge transfer process. Thus, a novel hyperbranched polyimide (HBPI‐TZA‐6FDA) has been prepared from new triazole derivative triamine monomer (TZA) and 4,4′‐(hexafluoroisopropylidene)diphthalic anhydride (6FDA) for memory device. The memory device with the structure ITO/HBPI‐TZA‐6FDA/Al exhibits a low‐threshold voltage of −2.2 V and a high ON/OFF current ratio of about 105. Meanwhile, the memory device shows nonvolatile write once read many times (WORM) type memory behavior and excellent stability with an operation time of 104 at a continuous applied voltage of −1 V. Optical, electrochemical experiments, and molecular simulation have been carried out to illustrate the memory performance. The memory performance is governed by the charge transfer between TZA and 6FDA units. The branched structure and triazole unit can reduce the band gap between HOMO and LUMO energy levels effectively, which is favorable for improving charge transfer and reducing threshold voltage. The HBPI‐TZA‐6FDA‐based memory device is favorable for memory device applications due to its relatively low‐power consumption and high‐operation stability.

Volatile and Nonvolatile Resistive Switching Coexistence in Conductive Point Hexagonal Boron Nitride Monolayer.

Recently, we demonstrated the nonvolatile resistive switching effects of metal-insulator-metal (MIM) atomristor structures based on two-dimensional (2D) monolayers. However, there are many remaining combinations between 2D monolayers and metal electrodes; hence, there is a need to further explore 2D resistance switching devices from material selections to future perspectives. This study investigated the volatile and nonvolatile switching coexistence of monolayer hexagonal boron nitride (h-BN) atomristors using top and bottom silver (Ag) metal electrodes. Utilizing an h-BN monolayer and Ag electrodes, we found that the transition between volatile and nonvolatile switching is attributed to the thickness/stiffness of chain-like conductive bridges between h-BN and Ag surfaces based on the current compliance and atomristor area. Computations indicate a "weak" bridge is responsible for volatile switching, while a "strong" bridge is formed for nonvolatile switching. The current compliance determines the number of Ag atoms that undergo dissociation at the electrode, while the atomristor area determines the degree of electric field localization that forms more stable conductive bridges. The findings of this study suggest that the h-BN atomristor using Ag electrodes shows promise as a potential solution to integrate both volatile neurons and nonvolatile synapses in a single neuromorphic crossbar array structure through electrical and dimensional designs.

Giant tunnel resistance effect in (SrTiO3)2/(BaTiO3)4/(CaTiO3)2 asymmetric superlattice with enhanced polarization.

In this work, we report the effectively enhanced tunneling electroresistance effect in Au/(SrTiO3)2/(BaTiO3)4/(CaTiO3)2/Nb:SrTiO3 superlattice ferroelectric tunnel junction (FTJ). The stable polarization switching and enhanced ferroelectricity were achieved in the nanoscale thickness high-quality epitaxial superlattice. A high ON/OFF current ratio of more than 105 was obtained at room temperature, which is an order of magnitude larger than the BaTiO3 FTJ with the same structure. Nonvolatile resistance switching controlled by nonvolatile polarization switching was observed in the superlattice FTJ. Driven by increased polarization and intrinsic asymmetric ferroelectricity, a highly asymmetric depolarization field is generated compared with the Au/BaTiO3/Nb:SrTiO3 FTJ, resulting in an enhanced tunneling electroresistance effect. These results provide a potential way to construct FTJ memory devices by constructing asymmetric three-component ferroelectric superlattices.

LTP–LTD transformation of unipolar pulse voltage-driven zinc oxide memristors via TiO2 thin layer incorporation

ZnO-based memristors are considered to be promising candidates in neuromorphic computing because of their nonvolatile resistive switching characteristics.

Solution-Processed Robust Multifunctional Memristor of 2D Layered Material Thin Film.

Memristors have gained significant attention recently due to their unique ability to exhibit functionalities for brain-inspired neuromorphic computing. Here, we demonstrate a high-performance multifunctional memristor using a thin film of liquid-phase exfoliated (LPE) 2D MoS2 pinched between two electrodes. Nanoscale inspection of a solution-processed MoS2 thin film using scanning electron and scanning probe microscopies revealed the high-quality and defect-free nature. Systematic current-voltage (I-V) characterizations depict a facile, nonvolatile resistive switching behavior of our 2D MoS2 thin film device with a current On/Off ratio of 103 and energy cost of only a few picojoules. Excellent performance metrics, including at least 103 cycle endurance, 104 s retention, and switching speed down to a few nanoseconds, reflect robust high-performance data storage capability. Charge carriers trapping and detrapping at the sulfur vacancy defect sites in MoS2 nanosheets mainly display the resistive switching property, supported by the impedance analysis and theoretical fitting results. Multifunctionality is leveraged through implementing two-input logic gate operations, edge computation, and crucial adaptive learning via a Pavlov's dogs experiment. Overall, our solution-processed MoS2 memristor has the potential for tremendous future opportunities in integrated circuits and different computing paradigms, including energy-efficient neuromorphic computing hardware in artificial intelligence.

Record high room temperature resistance switching in ferroelectric-gated Mott transistors unlocked by interfacial charge engineering

The superior size and power scaling potential of ferroelectric-gated Mott transistors makes them promising building blocks for developing energy-efficient memory and logic applications in the post-Moore’s Law era. The close to metallic carrier density in the Mott channel, however, imposes the bottleneck for achieving substantial field effect modulation via a solid-state gate. Previous studies have focused on optimizing the thickness, charge mobility, and carrier density of single-layer correlated channels, which have only led to moderate resistance switching at room temperature. Here, we report a record high nonvolatile resistance switching ratio of 38,440% at 300 K in a prototype Mott transistor consisting of a ferroelectric PbZr0.2Ti0.8O3 gate and an RNiO3 (R: rare earth)/La0.67Sr0.33MnO3 composite channel. The ultrathin La0.67Sr0.33MnO3 buffer layer not only tailors the carrier density profile in RNiO3 through interfacial charge transfer, as corroborated by first-principles calculations, but also provides an extended screening layer that reduces the depolarization effect in the ferroelectric gate. Our study points to an effective material strategy for the functional design of complex oxide heterointerfaces that harnesses the competing roles of charge in field effect screening and ferroelectric depolarization effects.

Growth and characterization of sputter-deposited Ga2O3-based memristive devices

In the last few years, there has been significant interest in gallium oxide devices for resistive switching technologies due to its remarkable sensitivity to oxygen. In this study, we present the growth and resistive switching of a (2¯01) oriented (75 ± 3) nmβ-Ga2O3 thin film on a Ru/Al2O3 substrate using magnetron radio frequency sputtering. The observed resistive switching was attributed to the formation and rupture of conductive filaments constituted by oxygen vacancies in the β-Ga2O3 film as confirmed by x-ray photoelectron spectroscopy and energy-dispersive x-ray spectroscopy. The electrical conduction was found to be of Ohmic nature in the low-resistance ON state, while the high-resistance OFF state was governed by the Poole–Frenkel transport mechanism. Exhibiting stable endurance cycles, long retention times, and ON/OFF ratios of up to 104, the devices can be considered as promising prototypes for future nonvolatile resistive switching random access memory with respect to both switching performance and device stability.

Conversion from memory to threshold resistance switching behavior by modulating compliance current

The volatile and nonvolatile resistance switching (RS) characteristics can be, respectively, used for the selector and memristor, which have received much attention. Thus, it is essential to find a simple and effective method to control the specific RS behavior of NbOx materials due to the co-occurrence of memory RS and threshold RS behaviors. Here, the NbOx film with a thickness of 100 nm was prepared by magnetron sputtering at 80 °C. The tungsten steel tip/NbOx/Pt device exhibited the co-existence of memory RS and threshold RS behaviors. By properly regulating compliance current (Icc), the specified memory and threshold RS behaviors were observed: the memory RS behavior occurred with an Icc of 5 mA, the threshold RS behavior occurred with an Icc of 10 mA, and integrated one selector-one-RRAM (resistive random access memory) (1S1R) RS behavior occurred with an Icc of 50 mA. Moreover, individual RS behavior showed good performance, e.g., good stability of memory RS, good repeatability and concentrated voltage distribution of threshold RS. The memory RS behavior occurred mainly due to the formation and fracture of oxygen vacancy conductive filaments (CFs). Meanwhile, mediated by local Joule heating, thermally induced conductivity change was responsible for the threshold RS behavior. Under an Icc of 50 mA, the oxygen vacancy CFs and a thermally induced conductivity change triggered the 1S1R RS behavior, which significantly suppressed the leakage current in RRAM 3D integrated structures. This work provides an efficient and convenient method for modulating and obtaining the desired RS behavior and better understanding the conversion mechanism between them.