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 structural rearrangements.
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…
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…
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…
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.
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 …
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）
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.
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…
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…
We report a significant change in friction of a $\rm La_{0.55}Ca_{0.45}MnO_3$ thin film measured as a function of the materials resistive state under ultrahigh vacuum conditions at room temperature by friction force microscopy. While friction is high in the insulating state, it clearly changes to lower values if the probed local region is switched to the conducting state via nanoscale resistance switching. Thus we demonstrate active control of friction without having to change the temperature or pressure. Upon switching back to an insulating state the friction increases again. The results are …
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…
In order to determine the key parameters that control the resistive switching mechanism in metal-complex oxides interfaces, we have studied the electrical properties of metal / YBa2Cu3O7-d (YBCO) interfaces using metals with different oxidation energy and work function (Au, Pt, Ag) deposited by sputtering on the surface of a YBCO ceramic sample. By analyzing the IV characteristics of the contact interfaces and the temperature dependence of their resistance, we inferred that ion migration may generate or cancel conducting filaments, which modify the resistance near the interface, in accordance …
A possible mechanism for the resistive switching observed experimentally in Fe/MgO/V/Fe junctions is presented. Ab initio total energy calculations within the local density approximation and pseudopotential theory shows that by moving the oxygen ions across the MgO/V interface one obtains a metastable state. It is argued that this state can be reached by applying an electric field across the interface. In addition, the ground state and the metastable state show different electric conductances. The latter results are discussed in terms of the changes of the density of states at the Fermi level …
We report giant resistive switching of an order of 104, long-time charge retention characteristics up to 104 s, non-overlapping SET and RESET voltages, ohmic in low resistance state (LRS) and space charge limited current (SCLC) mechanism in high resistance state (HRS) properties in polycrystalline perovskite Cobalt Titanate (CoTiO3 ~ CTO) thin films. Impedance spectroscopy study was carried out for both LRS and HRS states which illustrates that only bulk resistance changes after resistance switching, however, there is a small change (<10% which is in pF range) in the bulk capacitance value in …
BiFeO3 thin films are deposited on FTO coated glass substrates using a simple sol-gel deposition technique, limiting thickness about 70 nm and Ag/BiFeO3/FTO RRAM devices are prepared. The devices showed low-voltage bipolar switching with the maximum Ion/Ioff ~ 450, and low set and reset voltages ~ 1.1 V and -1.5 V, respectively. The devices are stable against on-off cycles with ~ 104 s retention time without any significant degradation. The variations in the set and reset voltages are 0.4 V and 0.6 V, respectively. We found that ohmic and trap-controlled space charge limited conductions are re…
Using metal-ferroelectric junctions as switchable diodes was proposed several decades ago. This was shown to actually work in PbZr(1-x)TixO3 (PZT) by Blom et al. [P.W. M. Blom et al., Phys. Rev. Lett. 73, 2107 (1994)], who reported switching in the rectification direction and changes of the current of about 2 orders of magnitude upon switching the polarization direction of the ferroelectric layer. This form of resistive switching enables the read out of a ferroelectric memory state at higher speed compared to the capacitive design, without destroying the information in each reading cycle. Rece…
The development prospects of memristive elements for non-volatile memory with use of the metal-dielectric-metal sandwich structures with a thin oxide layer are due to the possibility of reliable forming the sustained functional states with quantized resistance. In the paper we study the properties of fabricated memristors based on the non-stoichiometric $ZrO_2$ nanotubes in different resistive switching modes. Anodic oxidation of the $Zr$ foil has been used to synthesize a zirconia layer of $1.7$ $μ$$m$ thickness, consisting of an ordered array of vertically oriented nanotubes with outer diame…
We propose a tunneling heterostructure by replacing one of the metal electrodes in a metal/ferroelectric/metal ferroelectric tunnel junction with a heavily doped semiconductor. In this metal/ferroelectric/semiconductor tunnel diode, both the height and the width of the tunneling barrier can be electrically modulated due to the ferroelectric field effect, leading to a colossal tunneling electroresistance. This idea is implemented in Pt/BaTiO3/Nb:SrTiO3 heterostructures, in which an ON/OFF conductance ratio above 10$^4$ can be readily achieved at room temperature. The colossal tunneling electror…
Functional oxides based resistive memories are recognized as potential candidate for the next-generation high density data storage and neuromorphic applications. Fundamental understanding of the compositional changes in the functional oxides is required to tune the resistive switching characteristics for enhanced memory performance. Herein, we present the micro/nano-structural and compositional changes induced in a resistive oxide memory during resistive switching. Oxygen deficient amorphous chromium doped strontium titanate (Cr:$a$-SrTiO$_{3-x}$) based resistance change memories are fabricate…
Recent research demonstrated the electrical switching of antiferromagnets via intrinsic spin-orbit torque or the spin Hall effect of an adjacent heavy metal layer. The electrical readout is typically realized by measuring the transverse anisotropic magnetoresistance at planar cross- or star-shaped devices with four or eight arms, respectively. Depending on the material, the current density necessary to switch the magnetic state can be large, often close to the destruction threshold of the device. We demonstrate that the resulting electrical stress changes the film resistivity locally and there…
High-performance non-volatile resistive random access memories (ReRAM) and their small stimuli control are of immense interest for high-speed computation and big-data processing in the emergent Internet of Things (IOT) arena. Here, we examine the resistive switching (RS) behavior in growth controlled HfO2/La0.67Sr0.33MnO3 heterostructures and their tunability under low magnetic field. It is demonstrated that oxygen-deficient HfO2 films show bipolar switching with high on/off ratio, stable retention, as well as good endurance owing to the orthorhombic-rich phase constitution and charge (de)-tra…
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.
Films of Hf0.5Z0.5O2 (HZO) contain a network of grain boundaries. In (111) HZO epitaxial films on (001) SrTiO3, for instance, twinned orthorhombic (o-HZO) ferroelectric crystallites coexist with grain boundaries between o-HZO and a residual paraelectric monoclinic (m-HZO) phase. These grain boundaries contribute to the resistive switching response in addition to the genuine ferroelectric polarization switching and have detrimental effects on device performance. Here, it is shown that, by using suitable nanometric capping layers deposited on HZO film, a radical improvement of the operation wind…
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…
We report on the electric-field-induced reversible metal-insulator transition (MIT) of the insulating LaAlO3 thin films observed in metal/LaAlO3/Nb-SrTiO3 heterostructures. The switching voltage depends strongly on the thickness of the LaAlO3 thin film which indicates that a minimum thickness is required for the MIT. A constant opposing voltage is required to deplete the charges from the defect states. Our experimental results exclude the possibility of diffusion of the metal electrodes or oxygen vacancies into the LaAlO3 layer. Instead, the phenomenon is attributed to the formation of a quasi…
We have studied the effects of accumulating cyclic electrical pulses of increasing amplitude on the non-volatile resistance state of interfaces made by sputtering a metal (Au, Pt) on top of the surface of a cuprate superconductor YBa$_2$Cu$_3$O$_{7-δ}$ (YBCO). We have analyzed the influence of the number of applied pulses $N$ on the relative amplitude of the remnant resistance change between the high ($R_H$) and the low ($R_L$) state [$α=(R_{H}-R_{L})/R_{L}$] at different temperatures ($T$). We show that the critical voltage ($V_c$) needed to produce a resistive switching (RS, i.e. $α>0$) decr…
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…
Copper oxide thin film based metal-insulator-metal structures were subjected to white light irradiation.The top electrodes included Al, Cr and Ni while the bottom electrode was either Au or Pt. A white light pulse controls the set process and this light induced set (LIS) can be performed at very low voltages (tens of milli volts) which is not possible in the normal set process. The LIS is initiated at the positive edge of the pulse and there is no effect of the falling edge of the light. In most cases the high resistance state (HRS) to low resistance state (LRS) transition is irreversible i.e.…
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…
A detailed understanding of quantization conductance (QC), their correlation with resistive switching phenomena and controlled manipulation of quantized states is crucial for realizing atomic-scale multilevel memory elements. Here, we demonstrate highly stable and reproducible quantized conductance states (QC-states) in Al/Niobium oxide/Pt resistive switching devices. Three levels of control over the QC-states, required for multilevel quantized state memories, like, switching ON to different quantized states, switching OFF from quantized states, and controlled inter-state switching among one Q…
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…
We have synthesized Ga-doped Cr2O3 system with compositions Cr1.45Ga0.55O3 and Cr1.17Ga0.83O3 by chemical co-precipitation route and post annealing at 800^C. The samples have been stabilized in rhombohedral crystal structure with space group R3C. The present work focuses on the study of non-linear current-voltage (I-V) characteristics of the samples, which exhibited many interesting electronic properties, e.g., I-V loop, resistive switching, bi-stable electronic states, and negative differential resistance. The non-equilibrium character of the I-V characteristics has been studied by measuremen…
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.
