For the clear understanding of the role of interface reaction between top metal electrode and titanium oxide layer, we investigated the effects of various top metals on the resistive switching in Metal/a-TiO2/Al devices. The top Al device with the highest oxygen affinity showed the best memory performance, which is attributed to the fast formation of interfacial layer (Al-Ti-O), as confirmed by high resolution transmission electron microscopy and electron dispersive spectroscopy. Hence, we concluded that the interface layer, created by the redox reaction between top metal electrode and TiO2 layer, plays a crucial role in bipolar resistive switching behaviors of metal/TiO2/Al systems.
Bipolar resistive switching (BRS) phenomenon has been demonstrated in Mn3O4 using Al (Aluminum)/Mn3O4/FTO (Fluorine doped Tin Oxide) Resistive Random Access Memory (RRAM) device. The fabricated RRAM device shows good retention, non volatile behavior and forming free BRS. The Current-Voltage (I-V) characteristics and the temperature dependence of the resistance (R-T) measurements were used to explore conduction mechanisms and the thermal activation energy (Ea). The resistance ratio of high resistance state (HRS) to low resistance state (LRS) is ~102. The fabricated RRAM device shows different c…
In this paper, we report the effect of filament radius and filament resistivity on the saturated temperature of ZnO, TiO2, WO3 and HfO2 Resistive Random Access Memory (RRAM) devices. We resort to the thermal reaction model of RRAM for the present analysis. The results substantiate decrease in saturated temperature with increase in the radius and resistivity of filament for the investigated RRAM devices. Moreover, a sudden change in the saturated temperature at a lower value of filament radius and resistivity is observed as against the steady change at the medium and higher value of the filamen…
In this study, we proposed and demonstrated a self-rectifying property of silicon nitride (Si3N4)-based resistive random access memory device by employing p-type silicon (p-Si) as bottom electrode. The RRAM devices consisted of Al/Si3N4/p-Si are fabricated by a low presure chemical vapor deposition and exhibited an intrinsic diode property with non-linear current-voltage (I-V) behavior. In addition, compared to conventional metal/insulator/metal (MIM) structure of Al/Si3N4/Ti RRAM cells, operating current in whole bias regions for proposed metal/insulator/semiconductor (MIS) cells has been dra…
Much effort has been devoted to device and materials engineering to realize nanoscale resistance random access memory (RRAM) for practical applications, but there still lacks a rational physical basis to be relied on to design scalable devices spanning many length scales. In particular, the critical switching criterion is not clear for RRAM devices in which resistance changes are limited to localized nanoscale filaments that experience concentrated heat, electric current and field. Here, we demonstrate voltage-controlled resistance switching for macro and nano devices in both filamentary RRAM …
Resistance Random Access Memory (RRAMTM) device, with its electrically induced nanoscale resistive switching capacity, has been gaining considerable attention as future non-volatile memory device. Here, we propose a mechanism of switching based on oxygen vacancy migration-driven change in electronic properties of the transition metal oxide (TMO) film stimulated by set pulse voltages. We used density functional theory (DFT)-based calculations to account for the effect of oxygen vacancy and its migration on the electronic properties of HfO2 and Ta/HfO2 systems, and thereby create the entire stor…
The fundamental building blocks of modern silicon-based microelectronics, such as double gate transistors in non-volatile Flash memories, are based on the control of electrical resistance by electrostatic charging. Flash memories could soon reach their miniaturization limits mostly because reliably keeping enough electrons in an always smaller cell size will become increasingly difficult . The control of electrical resistance at the nanometer scale therefore requires new concepts, and the ultimate resistance-change device is believed to exploit a purely electronic phase change such as the Mott…
Reduction in metal-oxide thin films has been suggested as the key mechanism responsible for forming conductive nanofilaments within solid-state memory devices, enabling their resistive switching capacity. The quantitative spatial identification of such filaments is a daunting task, particularly for metal-oxides capable of exhibiting multiple phases as in the case of TiOx. Here, we spatially resolve and chemically characterize distinct TiOx phases in localized regions of a TiOx-based memristive device by combining full-field transmission X-ray microscopy with soft X-ray spectroscopic analysis t…
Memory has always been a building block element for information technology. Emerging technologies such as artificial intelligence, big data, the internet of things, etc., require a novel kind of memory technology that can be energy efficient and have an exception data retention period. Among several existing memory technologies, resistive random-access memory (RRAM) is an answer to the above question as it is necessary to possess the combination of speed of RAM and nonvolatility, thus proving to be one of the most promising candidates to replace flash memory in next-generation non-volatile RAM…
Metallic oxides encased within Metal-Insulator-Metal (MIM) structures can demonstrate both unipolar and bipolar switching mechanisms, rendering them the capability to exhibit a multitude of resistive states and ultimately function as memory elements. Identifying the vital physical mechanisms behind resistive switching can enable these devices to be utilized more efficiently, reliably and in the long-term. In this paper, we present a new approach for analysing resistive switching by modelling the active core of two terminal devices as 2D and 3D grid circuit breaker networks. This model is emplo…
Earlier, the DC hole-current modeling of PCMO RRAM by drift-diffusion (DD) including self-heating (SH) in TCAD (but without ionic transport) was able to explain the experimentally observed SCLC characteristics, prior to resistive switching. Further, transient analysis using DD+SH model was able to reproduce the experimentally observed fast current increase at ~100ns timescale followed by saturation increases, prior to resistive switching. However, resistive switching requires the inclusion of ionic transport. We propose a Reaction-Drift (RD) model of oxide ions, which is combined with the DD+S…
Voltage-controlled resistive switching is demonstrated in various gap systems on SiO2 substrate. The nanosized gaps are made by different means using different materials including metal, semiconductor, and metallic nonmetal. The switching site is further reduced by using multi-walled carbon nanotubes and single-walled carbon nanotubes. The switching in all the gap systems shares the same characteristics. This independence of switching on the material compositions of the electrodes, accompanied by observable damage to the SiO2 substrate at the gap region, bespeaks the intrinsic switching from p…
We report on resistive switching of memristive electrochemical metallization devices using 3D kinetic Monte Carlo simulations describing the transport of ions through a solid state electrolyte of an Ag/TiO$_{\text{x}}$/Pt thin layer system. The ion transport model is consistently coupled with solvers for the electric field and thermal diffusion. We show that the model is able to describe not only the formation of conducting filaments but also its dissolution. Furthermore, we calculate realistic current-voltage characteristics and resistive switching kinetics. Finally, we discuss in detail the …
Using isothermal and temperature-dependent electrical measurements, we investigated the resistive switching mechanism of amorphous titanium oxide thin films deposited by a plasma-enhanced atomic layer deposition method between two aluminum electrodes. We found a bipolar resistive switching behavior in the high temperature region (> 140 K), and two activation energies of shallow traps, 0.055 eV and 0.126 eV in the ohmic current regime. We also proposed that the bipolar resistive switching of amorphous TiO2 thin films is governed by the transition of conduction mode from a bulk-limited SCLC mode…
We report a direct observation of the microscopic origin of the bipolar resistive switching behavior in nanoscale titanium oxide films. Through a high-resolution transmission electron microscopy, an analytical TEM technique using energy-filtering transmission electron microscopy and an in situ x-ray photoelectron spectroscopy, we demonstrated that the oxygen ions piled up at top interface by an oxidation-reduction reaction between the titanium oxide layer and the top Al metal electrode. We also found that the drift of oxygen ions during the on/off switching induced the bipolar resistive switch…
Nanometallic devices based on amorphous insulator-metal thin films are developed to provide a novel non-volatile resistance-switching random-access memory (RRAM). In these devices, data recording is controlled by a bipolar voltage, which tunes electron localization length, thus resistivity, through electron trapping/detrapping. The low-resistance state is a metallic state while the high-resistance state is an insulating state, as established by conductivity studies from 2K to 300K. The material is exemplified by a Si3N4 thin film with randomly dispersed Pt or Cr. It has been extended to other …
Nonvolatile bipolar resistive switching has been observed in an Au/BiFeO3/Pt structure, where a Schottky contact and a quasi-Ohmic contact were formed at the Au/BiFeO3 and BiFeO3/Pt interface, respectively. By changing the polarity of the external voltage, the Au/BiFeO3/Pt is switched between two stable resistance states without an electroforming process. The resistance ratio is larger than two orders of magnitude. The resistive switching is understood by the electric field - induced carriers trapping and detrapping, which changes the depletion layer thickness at the Au/BiFeO3 interface.
Reverse and stable bipolar resistive switching effect was observed in planar NdCeCuO - NdCeO - Ag heterostructures. It was shown that the current voltage charactereriscs of the BRSE observed has a diode character. Simulations were used to consider the influence of the nonuniform distribution of an electric field at the interface of a heterojunction on the effect of bipolar resistive switching in investigated structures. The inhomogeneous distribution of the electric field near the contact edge creates regions of higher electric field strength which, in turn, stimulates motion and redistributio…
Two-dimensional materials have been discovered to exhibit non-volatile resistive switching (NVRS) phenomenon. In our work, we reported the universal NVRS behavior in a dozen metal dichalcogenides, featuring low switching voltage, large on/off ratio, fast switching speed and forming free characteristics. A unique conductive-point random access memory (CPRAM) effect is used to explain the switching mechanisms, supported by experimental results from current-sweep measurements.
Superlattices may play an important role in next generation electronic and spintronic devices if the key-challenge of the reading and writing data can be solved. This challenge emerges from the coupling of low dimensional individual layers with macroscopic world. Here we report the study of the resistive switching characteristics of a of hybrid structure made out of a superlattice with ultrathin layers of two ferromagnetic metallic oxides, La0.7Sr0.3MnO3 (LSMO) and SrRuO3 (SRO). Bipolar resistive switching memory effects are measured on these LSMO/SRO superlattices, and the observed switching …
We demonstrate the feasibility of multilevel recording in Pt/Bi(1-d)FeO3/SrRuO3 capacitors using the ferroelectric resistive switching phenomenon exhibited by the Pt/Bi(1-d)FeO3 interface. A tunable population of up and down ferroelectric domains able to modulate the Schottky barrier height at the Pt/Bi(1-d)FeO3 interface can be achieved by means of either a collection of SET/RESET voltages or current compliances. This programming scheme gives rise to well defined resistance states, which form the basis for a multilevel storage nonvolatile memory.
The non-Markov processes widely exist in thermodymanic processes, while it usually requires packing of many transistors and memories with great system complexity in traditional device architecture to minic such functions. Two-dimensional (2D) material-based resistive random access memory (RRAM) devices show potential for next-generation computing systems with much-reduced complexity. Here, we achieve the non-Markov chain in an individual RRAM device based on 2D mica with a vertical metal/mica/metal structure. We find that the internal potassium ions (K+) in 2D mica gradually move along the dir…
The resistive switching phenomena of HfO2 films grown by metalorganic chemical vapor deposition was studied for the application of ReRAM devices. In the fabricated Pt/HfO2/TiN memory cells, the bipolar resistive switching characteristics were observed, and the set and reset states were measured to be as low as 7 uA and 4 uA, respectively, at VREAD = 1 V. Regarding the resistive switching performance, the stable RS performance was observed under 40 repetitive dc cycling test with the small variations of set/reset voltages and currents, and good retention characteristics over 105 s in both LRS a…
Complementary resistive switches (CRS) are considered as a potential solution for the sneak path problem in large-scale integration of passive crossbar resistive memory arrays. A typical CRS is composed of two bipolar memory cells that are connected anti-serially. Here we report a tantalum-oxide based resistive memory that achieves the complementary switching functionality within a single memory cell. The complementary switching effect is accompanied by switching polarity reversal in different voltage bias regimes. These effects were explained by the redistribution of oxygen vacancies inside t…
We studied the resistive memory switching in pulsed laser deposited amorphous LaHoO3 (LHO) thin films for non-volatile resistive random access memory (RRAM) applications. Nonpolar resistive switching (RS) was achieved in PtLHOPt memory cells with all four possible RS modes ( positive unipolar, positive bipolar, negative unipolar, and negative bipolar) having high RON and ROFF ratios (in the range of 104 to 105) and non-overlapping switching voltages (set voltage, VON 3.6 to 4.2 V and reset voltage, VOFF 1.3 to 1.6 V) with a small variation of about 5 to 8 percent. X ray photoelectron spectrosc…
The operation of resistive and phase-change memory (RRAM and PCM) is controlled by highly localized self-heating effects, yet detailed studies of their temperature are rare due to challenges of nanoscale thermometry. Here we show that the combination of Raman thermometry and scanning thermal microscopy (SThM) can enable such measurements with high spatial resolution. We report temperature-dependent Raman spectra of HfO$_2$, TiO$_2$ and Ge$_2$Sb$_2$Te$_5$ (GST) films, and demonstrate direct measurements of temperature profiles in lateral PCM devices. Our measurements reveal that electrical and …
Materials exhibiting reversible resistive switching in electrical fields are highly demanded for functional elements in oxide electronics. In particular, multilevel switching effects allow for advanced applications like neuromorphic circuits. Here we report on a structurally driven switching mechanism involving the so-called `dead layers' of perovskite manganite surfaces. Forming a tunnel barrier whose thickness can be changed in monolayer steps by electrical fields, the switching effect exhibits well-defined and robust resistive states.
An electro-thermal computational study of conducting channels in dielectric thin films using self-consistent phase-field methodology: A view toward the physical origins of resistive switching
In the present work, multi-level resistive switching (RS) in W/Co:TiO2/FTO structures induced by a multi-mixed mechanism was studied. It was found that the devices could be reproducibly programmed into three nonvolatile resistance states. And the directly switching between any resistance states was realized. This increases the operation speed and lowers the complexity of control circuit of multi-state nonvolatile memory.
We introduce a model that accounts for the bipolar resistive switching phenomenom observed in transition metal oxides. It qualitatively describes the electric field-enhanced migration of oxygen vacancies at the nano-scale. The numerical study of the model predicts that strong electric fields develop in the highly resistive dielectric-electrode interfaces, leading to a spatially inhomogeneous oxygen vacancies distribution and a concomitant resistive switching effect. The theoretical results qualitatively reproduce non-trivial resistance hysteresis experiments that we also report, providing key …
Films produced by assembling bare gold clusters well beyond the electrical percolation threshold show a resistive switching behavior whose investigation has started only recently. Here we address the challenge to charaterize the resistance of a nanogranular film starting from limited information on the structure at the microscopic scale by the means of Bruggeman's approach to multicomponent media, within the framework of Effective Medium Approximations. The approach is used to build a model that proves that the observed resistive switching can be explained by thermally regulated local structur…
We investigated electroforming-free bipolar resistive switching behavior in Pt/Ti/Al2O3/Al tunnel junctions where the Al2O3 tunnel barrier was naturally formed on Al in air. Various compliance current values for the junction's set switching successfully lead to various resistance values in its low resistance state, suggesting the possibility for multi-level-operation. A mechanism for the bipolar switching is qualitatively discussed in terms of the modulation of the tunnel barrier by the reactive Ti layer on top of the barrier.
BiFeO3 thin films have been grown on Pt/Ti/SiO2/Si substrates with pulsed laser deposition using Au as the top electrode. The resistive switching property of the Au/BiFeO3/Pt stack has been significantly improved by carefully tuning the oxygen pressure during the growth, and a large switching ratio of ~4500 has been achieved. The deposition pressure modifies the concentration of oxygen vacancies and the rectifying behavior of the Au/BiFeO3 junction, and consequently influences the resistive switching behavior of the whole stack. The switching takes place homogeneously over the entire electrode…
Decoupling effects of the resistive-switching behavior on the polarization reversal in ultrathin ferroelectric Hf0.5Zr0.5O2 films
Harbin Institute of Technology, Shenzhen（哈尔滨工业大学（深圳））；Quantum Science Center of Guangdong-Hong Kong-Macao Greater Bay Area（粤港澳大湾区量子科学中心）；Westlake University（西湖大学）；Indian Institute of Science（印度科学学院）；University of Science and Technology Beijing（北京科技大学）
Organic electronics is very promising due to the flexibility, modifiability as well as variety of the available organic molecules. Efforts are going on to use organic materials for the realization of memory devices. In this regard resistive switching devices surely will play a key role. In this paper an effort has been made to illustrate the general information about resistive switching devices as well as switching mechanisms involving organic materials. As a whole a general overview of the emerging topic resistive switching has been given.
We demonstrated an electric field controlled exchange bias (EB) effect accompanied with unipolar resistive switching behavior in the Si/SiO2/Pt/Co/NiO/Pt device. By applying certain voltages, the device displays obvious EB in high-resistance-state while negligible EB in low-resistance-state. Conductive filaments forming and rupture in the NiO layer but near the Co-NiO interface are considered to play dominant roles in determining the combined resistive switching and EB phenomena. This work paves a new way for designing multifunctional and nonvolatile magnetic-electrical random access memory de…
BiFeO3 thin films have been deposited on Pt/sapphire and Pt/Ti/SiO2/Si substrates with pulsed laser deposition using the same growth conditions, respectively. Au was sputtered as the top electrode. The microscopic structure of the thin film varies by changing the underlying substrate. Thin films on Pt/sapphire are not resistively switchable due to the formation of Schottky contacts at both the top and the bottom interface. However, thin films on Pt/Ti/SiO2/Si exhibit an obvious resistive switching behavior under forward bias. The conduction mechanisms in BiFeO3 thin films on Pt/sapphire and Pt…
Controlled bipolar resistive switching (BRS) has been observed in nanostructured CoFe2O4 films using Al(aluminum)/CoFe2O4/FTO(fluorine-doped tin oxide) device. The fabricated device shows electroforming-free uniform BRS with two clearly distinguished and stable resistance states without any application of compliance current (CC), with a resistance ratio of high resistance state (HRS) and low resistance state (LRS) > 102. Small switching voltage (< 1 volt) and lower current in both the resistance states confirms the fabrication of low power consumption device. In the LRS, the conduction mechani…
We study the resistive switching triggered by an applied electrical bias in antiferromagnetic Mott insulator Sr(3)Ir(2)O(7). The switching was previously associated with an electric-field driven structural transition. Here we use time-resolved measurements of the switching to probe the energy barrier associated with the transition. We quantify the changes in the energy barrier height with respect to the applied bias and find a linear decrease of the barrier with increasing bias. Our observations support the potential of antiferromagnetic transition metal oxides for spintronic applications.
Metallic nanogranular films display a complex dynamical response to a constant bias, showing up as atypical resistive switching mechanism which could be used to create electrical components for neuromorphic applications. To model such a phenomenon we use a multiscale approach blending together an ab initio treatment of the electric current at the nanoscale, a molecular dynamical approach dictating structural rearrangements, and a finite-element solution of the heat equation for heat propagation in the sample. We also consider structural changes due to electromigration which are modelled on the…
Resistive random access memories are promising for non-volatile memory and brain-inspired computing applications. High variability and low yield of these devices are key drawbacks hindering reliable training of physical neural networks. In this study, we show that doping an oxide electrolyte, Al2O3, with electronegative metals makes resistive switching significantly more reproducible, surpassing the reproducibility requirements for obtaining reliable hardware neuromorphic circuits. The underlying mechanism is the ease of creating oxygen vacancies in the vicinity of electronegative dopants, due…
Bipolar resistive switching using organic molecule is very promising for memory application owing to their advantages like simple device structure, low manufacturing cost, their stability and flexibility etc. Herein we report Langmuir-Blodgett and spin-coated film based bipolar resistive switching devices using organic material indole derivative. Pressure - area per molecule isotherm, Brewster Angle Microscopy, Atomic Force Microscopy and Scanning Electron Microscopy were used to have an idea about organization and morphology of the organic material onto thin film. Based on device structure an…
Resistive random-access memories, also known as memristors, whose resistance can be modulated by the electrically driven formation and disruption of conductive filaments within an insulator, are promising candidates for neuromorphic applications due to their scalability, low-power operation and diverse functional behaviours. However, understanding the dynamics of individual filaments, and the surrounding material, is challenging, owing to the typically very large cross-sectional areas of test devices relative to the nanometre scale of individual filaments. In the present work, conductive atomi…
Passing current at given threshold voltages through a metal/insulator/metal sandwich structure device may change its resistive state. Such resistive switching is unique to nanoscale devices, but its underlying physical mechanism remains unknown. We show that the different resistive states are due to different spontaneously charged states, characterized by different `band bending' solutions of Poisson's equation. For an insulator with mainly donor type defects, the low-resistivity state is characterized by a negatively charged insulator due to convex band bending, and the high-resistivity state…
Electrical characteristics of a Co/TiO_x/Co resistive memory device, fabricated by two different methods are reported. In addition to crystalline TiO_2 layers fabricated via conventional atomic layer deposition (ALD), an alternative method has been examined, where TiO_x nanoparticle layers were fabricated via sol-gel. The different devices have shown different hysteresis loops with a unique crossing point for the sol-gel devices. A simple qualitative model is introduced to describe the different current-voltage behaviours by suggesting only one active metal-oxide interface for the ALD devices …
Memory devices based on resistive switching (RS) have not been fully realised due to lack of understanding of the underlying switching mechanisms. Nature of ion transport responsible for switching and growth of conducting filament in transition metal oxide based RS devices is still in debate. Here, we investigated the mechanism in Niobium oxide based RS devices, which shows unipolar switching with high ON/OFF ratio, good endurance cycles and high retention times. We controlled the boundary conditions between low-conductance insulating and a high-conductance metallic state where conducting fila…
Metal oxide resistive switches are increasingly important as possible artificial synapses in next generation neuromorphic networks. Nevertheless, there is still no codified set of tools for studying properties of the devices. To this end, we demonstrate electron beam induced current measurements as a powerful method to monitor the development of local resistive switching in TiO2 based devices. By comparing beam-energy dependent electron beam induced currents with Monte Carlo simulations of the energy absorption in different device layers, it is possible to deconstruct the origins of filament i…
Application of an electric stimulus to a material with a metal-insulator transition can trigger a large resistance change. Resistive switching from an insulating into a metallic phase, which typically occurs by the formation of conducting filaments parallel to the current flow, has been an active research topic. Here we present the discovery of an opposite, metal-to-insulator switching that proceeds via nucleation and growth of an insulating barrier perpendicular to the driving current. The barrier formation leads to an unusual N-type negative differential resistance in the current-voltage cha…
