Quantum transport properties of tantalum-oxide resistive switching filaments
Budapest University of Technology and Economics（布达佩斯技术与经济大学）；Institute of Technical Physics and Materials Science, Centre for Energy Research（技术物理与材料科学研究所，能源研究中心）；MTA-BME Correlated van der Waals Structures Momentum Research Group（匈牙利科学院-布达佩斯技术与经济大学关联范德华结构动力学研究组）；ELKH-BME Condensed Matter Research Group（匈牙利研究与创新院-布达佩斯技术与经济大学凝聚态研究组）；Institute of Electromagnetic Fields, ETH Zurich（苏黎世联邦理工学院电磁场研究所）
Tímea Nóra Török, Péter Makk, Zoltán Balogh, Miklós Csontos, András Halbritter
Filamentary resistive switching devices are not only considered as promising building blocks for brain-inspired computing architectures, but they also realize an unprecedented operation regime, where the active device volume reaches truly atomic dimensions. Such atomic-sized resistive switching filaments represent the quantum transport regime, where the transmission eigenvalues of the conductance channels are considered as a specific device fingerprint. Here, we gain insight into the quantum transmission properties of close-to-atomic-sized resistive switching filaments formed across an insulating Ta$_2$O$_5$ layer through superconducting subgap spectroscopy. This method reveals the transmission density function of the open conduction channels contributing to the device conductance. Our analysis confirms the formation of truly atomic-sized filaments composed of 3-8 Ta atoms at their narrowest cross-section. We find that this diameter remains unchanged upon resistive switching. Instead, the switching is governed by the redistribution of oxygen vacancies within the filamentary volume. The set/reset process results in the reduction/formation of an extended barrier at the bottleneck of the filament which enhances/reduces the transmission of the highly open conduction channels.
We present a phenomenological theory of filamentary resistive random access memory (RRAM) describing the commonly observed features of their current-voltage characteristics. Our approach follows the approach of thermodynamic theory developed earlier for chalcogenide memory and threshold switches and largely independent of their microscopic details. It explains, without adjustable parameters, such features as the domains of filament formation and switching, voltage independent current in SET and current independent voltage in RESET regimes, the relation between the set and reset voltages, filam…
The nature of the conducting filaments in many resistive switching systems has been elusive. Through in situ transmission electron microscopy, we image the real-time formation and evolution of the filament in a silicon oxide resistive switch. The electroforming process is revealed to involve the local enrichment of silicon from the silicon oxide matrix. Semi-metallic silicon nanocrystals with structural variations from the conventional diamond cubic form of silicon are observed, which likely accounts for the conduction in the filament. The growth and shrinkage of the silicon nanocrystals in re…
Memristors are among the most promising elements for modern microelectronics, having unique properties such as quasi-continuous change of conductance and long-term storage of resistive states. However, identifying the physical mechanisms of resistive switching and evolution of conductive filaments in such structures still remains a major challenge. In this work, aiming at a better understanding of these phenomena, we experimentally investigate an unusual effect of enhanced conductive filament stability in memristors with copper filaments under the applied voltage and present a simplified theor…
We report the fabrication and performance of all-metallic three-terminal devices with tantalum diselenide thin-film conducting channels. For this proof-of-concept demonstration, the layers of 2H-TaSe2 were exfoliated mechanically from single crystals grown by the chemical vapor transport method. Devices with nanometer-scale thicknesses exhibit strongly non-linear current-voltage characteristics, unusual optical response, and electrical gating at room temperature. We have found that the drain-source current in thin-film 2H-TaSe2-Ti/Au devices reproducibly shows an abrupt transition from a highl…
We show that, in tantalum oxide resistive memories, activation power provides a multi-level variable for information storage that can be set and read separately from the resistance. These two state variables (resistance and activation power) can be precisely controlled in two steps: (1) the possible activation power states are selected by partially reducing resistance, then (2) a subsequent partial increase in resistance specifies the resistance state and the final activation power state. We show that these states can be precisely written and read electrically, making this approach potentially…
Critical temperature regions for resistive switching were found based on HfAlO resistive switching memory. From 5 K to 300 K, the resistive switching appears at 60 K, and then a reversible bipolar switching between the two states is observed at above 150 K. It is suggested that the resistive switching characteristics of the binary transitional metal oxides are governed by thermal assisted percolating conductive paths. The process of charge trap/de-trapping under the external electrical field plays a dominated role with the assumption of the same Joule heating generated by internal conductive f…
Some correlated materials display an insulator-to-metal transition as the temperature is increased. In most cases this transition can also be induced electrically, resulting in volatile resistive switching due to the formation of a conducting filament. While this phenomenon has attracted much attention due to potential applications, many fundamental questions remain unaddressed. One of them is its characteristic lengths: what sets the size of these filaments, and how does this impact resistive switching properties. Here we use a combination of wide-field and scattering-type scanning near-field…
Prevailing models of resistive switching arising from electrochemical formation of conducting filaments across solid state ionic conductors commonly attribute the observed polarity of the voltage-biased switching to the sequence of the active and inert electrodes confining the resistive switching memory cell. Here we demonstrate equivalent, stable switching behavior in metallic Ag-Ag$_{2}$S-Ag nanojunctions at room temperature. Our experimental results and numerical simulations reveal that the polarity of the switchings is solely determined by the geometrical asymmetry of the electrode surface…
Resistive Switching (RS) is the change in resistance of a dielectric under the influence of an external current or electric field. This change is non-volatile, and the basis of both the memristor and resistive random access memory. In the latter, high integration densities favor the anti-serial combination of two RS-elements to a single cell, termed the complementary resistive switch (CRS). Motivated by the irregular shape of the filament protruding into the device, we suggest a nonlinearity in the resistance-interpolation function, and thereby expand the original HP-memristor. We numerically …
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 …
In this work we report on kinetic Monte-Carlo calculations of resistive switching and the underlying growth dynamics of filaments in an electrochemical metallization device consisting of an Ag/TiO2/Pt sandwich-like thin film system. The developed model is not limited to i) fast time scale dynamics and ii) only one growth and dissolution cycle of metallic filaments. In particular, we present results from the simulation of consecutive cycles. We find that the numerical results are in excellent agreement with experimentally obtained data. Additionally, we observe an unexpected filament growth mod…
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…
The equilibrium ON and OFF states of resistive random access memory (RRAM) are due to formation and destruction of a conducting filament. The laws of thermodynamics dictate that these states correspond to the minimum of free energy. Here, we develop a numerical model that, through the minimization of free energy at a given voltage, determines the filament parameters and thus the electric current. Overall, it simulates the current-voltage (I-V) characteristics of RRAM. The model describes mutual transformations of RRAM states through SET (ON to OFF) and RESET (OFF to ON) processes. From the mod…
Resistive switching devices, important for emerging memory and neuromorphic applications, face significant challenges related to control of delicate filamentary states in the oxide material. As a device switches, its rapid conductivity change is involved in a positive feedback process that would lead to runaway destruction of the cell without current, voltage, or energy limitation. Typically, cells are directly patterned on MOS transistors to limit the current, but this approach is very restrictive as the necessary integration limits the materials available as well as the fabrication cycle tim…
Memristive switching devices, candidates for resistive random access memory technology, have been shown to switch off through a progression of states with quantized conductance and subsequent non-integer conductance (in terms of conductance quantum $G_0$). We have performed calculations based on density functional theory to model the switching process for a Pt-HfO$_2$-Pt structure, involving the movement of one or two oxygen atoms. Oxygen atoms moving within a conductive oxygen vacancy filament act as tunneling barriers, and partition the filament into weakly coupled quantum wells. We show tha…
Budapest University of Technology and Economics（布达佩斯技术与经济大学）；MTA-BME Condensed Matter Research Group（MTA-BME凝聚态研究组）；Empa, Swiss Federal Laboratories for Materials Science and Technology（瑞士联邦材料科技研究所）
Usually, resistive switching (RS) devices show digital RS memory (sharp SET and RESET process), which is most suitable for digital data storage applications. Some RS devices also manifest ideal memristive behavior or analog memory characteristics (gradual change in resistance states). The analog RS properties of memristive devices widen their application domain to a much broader field of neuromorphic computing. The tunability of memristive devices to digital or analog memory applications greatly depends upon the switching medium. In this work, we report a comparative study on RS properties of …
In this study, direct-current reactive sputtered ZnO and ZnO1-x based thin film (30 nm and 300 nm in thickness) memristor devices were produced and the effects of oxygen vacancies and thickness on the memristive characteristics were investigated. The oxygen deficiency of the ZnO1-x structure was confirmed by SIMS analyses. The memristive characteristics of both the ZnO and ZnO1-x devices were determined by time dependent current-voltage (I-V-t) measurements. The distinctive pinched hysteresis I-V loops of memristors were observed in all the fabricated devices. The typical homogeneous interface…
Tuning the memristive response of TaO$_x$-based devices with Ag Nanoparticles
Centro Atómico Bariloche, Instituto Balseiro (UNCuyo), CONICET（巴里洛切原子中心，巴尔塞罗研究所）；Zernike Institute for Advanced Materials, University of Groningen（格罗宁根大学泽尔尼克先进材料研究所）；CogniGron Center, University of Groningen（格罗宁根大学认知格罗宁根中心）；Instituto de Nanociencia y Materiales de Aragón (INMA-Unizar)（阿拉贡纳米科学与材料研究所）；Departamento de Física de la Materia Condensada, UNIZAR（萨拉戈萨大学凝聚态物理系）；Laboratorio de Microscopías Avanzadas, UNIZAR-CSIC（萨拉戈萨大学-西班牙国家研究委员会先进显微镜实验室）；Laboratorio de Ablación Láser (INN-CONICET-CNEA), Centro Atómico Constituyentes（constituent 原子中心激光烧蚀实验室）
Like silicon-based semiconductor devices, van der Waals heterostructures will require integration with high-K oxides. This is needed to achieve suitable voltage scaling, improved performance as well as allowing for added functionalities. Unfortunately, commonly used high-k oxide deposition methods are not directly compatible with 2D materials. Here we demonstrate a method to embed a multi-functional few nm thick high-k oxide within van der Waals devices without degrading the properties of the neighbouring 2D materials. This is achieved by in-situ laser oxidation of embedded few layer HfS2 crys…
Rate Programmable Ionic-Redox Switching with Tunable Volatility in CuCrP2S6
CIC NanoGUNE BRTA（CIC纳米古恩BRTA）；Department of Physics and Astronomy, University of Bologna（博洛尼亚大学物理与天文学系）；University of the Basque Country (UPV/EHU)（巴斯克大学）；Donostia International Physics Center, DIPC（圣塞巴斯蒂安国际物理中心，DIPC）；Materials Physics Center CSIC-UPV/EHU（材料物理中心 CSIC-UPV/EHU）；IKERBASQUE, Basque Foundation for Science（伊卡巴斯基，巴斯克科学基金会）；INFN, Sezione di Bologna（意大利国家核物理研究所，博洛尼亚分部）
