Probing resistive switching in HfO2/Al2O3 bilayer oxides using in-situ transmission electron microscopy

In this work, we investigate the resistive switching in hafnium dioxide (HfO2) and aluminum oxide (Al2O3) bilayered stacks using in-situ transmission electron microscopy and X-ray energy dispersive spectroscopy. Conductance of the HfO2/Al2O3 stack changes gradually upon electrical stressing which is related to the formation of extended nanoscale physical defects at the HfO2/Al2O3 interface and the migration and re-crystallization of Al into the oxide bulk. The results suggest two competing physical mechanisms including the redistribution of oxygen ions and the migration of Al species from the Al electrode during the switching process. While the HfO2/Al2O3 bilayered stack appears to be a good candidate for RRAM technology, the low diffusion barrier of the active Al electrode causes severe Al migration in the bi-layered oxides leading to the device to fail in resetting, and thereby, largely limiting the overall switching performance and material reliability

Resistive switching in ALD metal-oxides with engineered interfaces

L'abstract è presente nell'allegato / the abstract is in the attachmen

SiOx-based resistive switching memory integrated in nanopillar structure fabricated by nanosphere lithography

textA highly compact, one diode-one resistor (1D-1R) SiOx-based resistive switching memory device with nano-pillar architecture has been achieved for the first time using nano-sphere lithography. The average nano-pillar height and diameter are 1.3 μm and 130 nm, respectively. Low-voltage electroforming using DC bias and AC pulse response in the 50ns regime demonstrate good potential for high-speed, low-energy nonvolatile memory. Nano-sphere deposition, oxygen-plasma isolation, and nano-pillar formation by deep-Si-etching are studied and optimized for the 1D-1R configurations. Excellent electrical performance, data retention and the potential for wafer-scale integration are promising for future non-volatile memory applications.Materials Science and Engineerin

Growth and Oxidation of Graphene and Two-Dimensional Materials for Flexible Electronic Applications

The non-volatile storage of information is becoming increasingly important in our data-driven society. Limitations in conventional devices are driving the research and development of incorporating new materials into conventional device architectures to improve performance, as well as developing an array of emerging memory technologies based on entirely new physical processes. The discovery of graphene allowed for developing new approaches to these problems, both itself and as part of the larger, and ever-expanding family of 2D materials. In this thesis the growth and oxidation of these materials is investigated for implementing into such devices, exploiting some of the unique properties of 2D materials including atomic thinness, mechanical flexibility and tune-ability through chemical modification - to meet some challenges facing the community. This begins with the growth of graphene by chemical vapour deposition for a high quality flexible electrode material, followed by oxidation of graphene for use in resistive memory devices. The theme of oxidation is then extended to another 2D material, HfS2, which is selectively oxidised for use as high-k dielectric in Van der Waals heterostructures for FETs and resistive memory devices. Lastly, a technique for fabrication of graphene-based devices directly on the copper growth substrate is demonstrated for use in flexible devices for sensing touch and humidity

Processos de condução eletrónica em células de memória ReRAM do tipo VCM com óxidos metálicos

New applications, such as neuromorphic computing, and the limitations of current semiconductor technologies demand a revolution in electronic devices. As one of the key enablers of a new electronics paradigm, redox-based resistive switching random access memory (ReRAM) has been the focus of much research and development. Among the ReRAM research community, Ta2O5 has emerged as one of the most popular materials, for enabling high endurance and high switching speed. Ta2O5-based ReRAM rely on the nonvolatile change of the resistance via the modulation of the oxygen content in conductive filaments, as it is described in the valence change mechanism. However, the filaments’ structure and exact composition are currently under intense debate, which hinders the development of better device design rules. The two current models in the literature consider filaments composed of oxygen vacancies and those containing metallic Ta. This work attempts to solve this dispute by reporting a detailed study of the electrical transport through the conductive filaments inside Ta2O5-based ReRAM. In parallel, the electrical transport and structure of substoichiometric TaOx thin films, grown to try and match the material of the filaments, was studied in detail. A strong correlation between the transport mechanisms in the conductive filaments inside the Ta2O5 ReRAM and in the TaOx thin films with x 1 was found. This clearly links the physical properties of the materials composing the filaments and the substoichiometric TaOx thin films. Structural analysis performed on the TaOx films reveals the presence of Ta clusters inside the films. Moreover, the electrical transport of metallic Ta films shows the same transport mechanism as TaOx with x 1, for most of the measured temperature range, from 2 K to 300 K. Beyond the transport mechanisms, both cases share a carrier concentration on the order of 1022 cm−3 and a positive magnetoresistance associated with weak antilocalization at T < 30 K. Therefore, it is concluded that the transport in the TaOx films with x 1 is dominated by a percolation chain of Ta clusters embedded in an insulating Ta2O5 matrix. These clusters exhibit disordered metal-like behaviour, where quantum corrections to the Boltzmann transport dominate the conduction. In conclusion, the electrical transport in the conductive filaments inside Ta2O5-based ReRAM devices is determined by percolation through Ta clusters, which is in line with independent observations of metallic Ta in the filaments. This work strongly supports the metallic Ta filament model.Novas aplicações, tais como computação neuromórfica, e as limitações da tecnologia de semicondutores atual exigem uma revolução nos dispositivos eletrónicos. Sendo uma peça chave para um novo paradigma da eletrónica, a memória ReRAM (redox-based resistive switching random access memory) tem sido alvo de muita investigação e desenvolvimento. O Ta2O5 é um dos materiais mais populares para usar em dispositivos ReRAM, permitindo alta durabilidade e velocidades de comutação elevadas. As ReRAM com Ta2O5 baseiam-se na mudança não volátil da resistência elétrica através da modulação da quantidade de oxigénio em filamentos condutores, como é descrito no mecanismo de alteração de valência (valence change mechanism). No entanto, a estrutura dos filamentos e a sua composição química exata, são ainda alvo de intenso debate, limitando o desenvolvimento de melhores receitas de fabricação de dispositivos. Os dois modelos atuais na literatura consideram filamentos compostos por lacunas de oxigénio e filamentos com Ta metálico. Este trabalho procura resolver esta disputa ao reportar um estudo detalhado do transporte elétrico através de filamentos condutores em dispositivos ReRAM de Ta2O5. Paralelamente, foi estudado em detalhe o transporte elétrico e a estrutura de filmes finos de TaOx subestequiométrico, depositados de forma a emular o material dos filamentos. Foi encontrada uma forte correlação entre os mecanismos de transporte nos filamentos condutores dentro dos dispositivos ReRAM de Ta2O5 e nos filmes finos de TaOx com x 1. Isto estabelece uma ligação clara entre as propriedades físicas dos materiais que compõem tanto os filamentos como os filmes finos de TaOx. A análise estrutural efetuada nos filmes de TaOx revela a presença de aglomerados de Ta. Por outro lado, o transporte elétrico em filmes finos de Ta é dominado pelos mesmos mecanismos de condução observados nos filmes de TaOx com x 1, para a maior parte da gama de temperatura de 2 K a 300 K. Ambos os casos partilham ainda uma concentração de portadores da ordem de 1022 cm−3 e uma magnetoresistência positiva associada a anti-localização fraca para T < 30 K. Portanto, é concluído que o transporte em filmes de TaOx com x 1 é dominado por uma cadeia de percolação de aglomerados de Ta embutidos numa matriz isoladora de Ta2O5. Estes aglomerados exibem um comportamento típico de metais desordenados, para os quais a condução é dominada por correções quânticas ao transporte de Boltzmann. Em conclusão, o transporte elétrico em filamentos condutores dentro de dispositivos ReRAM baseados em Ta2O5 é dominado pela percolação de aglomerados de Ta, o que corrobora observações independentes de Ta metálico nos filamentos. Assim, este trabalho suporta o modelo baseado no filamento metálico de Ta.Programa Doutoral em Engenharia Físic

Effect of Surface Variations on Resistive Switching

In this chapter, we study factors that dominate the interfacial resistive switching (RS) in memristive devices. We have also given the basic understanding of different type of RS devices which are predominantly interfacial in nature. In case of resistive random access memory (RRAM), the effect of surface properties on the bulk cannot be neglected as thickness of the film is generally below 100 nm. Surface properties are effected by redox reactions, interfacial layer formation, and presence of tunneling barrier. Surface morphology affects the band structure in the vicinity of interface, which in turn effects the movements of charge carriers. The effect of grain boundaries (GBs) and grain surfaces (GSs) on RS have also been discussed. The concentration of vacancies (Ov)/traps/defects is comparatively higher at GBs which leads to leakage current flow through the GBs predominantly. Such huge presence of charge carriers causes current flow through grain boundaries

Towards Oxide Electronics:a Roadmap

At the end of a rush lasting over half a century, in which CMOS technology has been experiencing a constant and breathtaking increase of device speed and density, Moore's law is approaching the insurmountable barrier given by the ultimate atomic nature of matter. A major challenge for 21st century scientists is finding novel strategies, concepts and materials for replacing silicon-based CMOS semiconductor technologies and guaranteeing a continued and steady technological progress in next decades. Among the materials classes candidate to contribute to this momentous challenge, oxide films and heterostructures are a particularly appealing hunting ground. The vastity, intended in pure chemical terms, of this class of compounds, the complexity of their correlated behaviour, and the wealth of functional properties they display, has already made these systems the subject of choice, worldwide, of a strongly networked, dynamic and interdisciplinary research community. Oxide science and technology has been the target of a wide four-year project, named Towards Oxide-Based Electronics (TO-BE), that has been recently running in Europe and has involved as participants several hundred scientists from 29 EU countries. In this review and perspective paper, published as a final deliverable of the TO-BE Action, the opportunities of oxides as future electronic materials for Information and Communication Technologies ICT and Energy are discussed. The paper is organized as a set of contributions, all selected and ordered as individual building blocks of a wider general scheme. After a brief preface by the editors and an introductory contribution, two sections follow. The first is mainly devoted to providing a perspective on the latest theoretical and experimental methods that are employed to investigate oxides and to produce oxide-based films, heterostructures and devices. In the second, all contributions are dedicated to different specific fields of applications of oxide thin films and heterostructures, in sectors as data storage and computing, optics and plasmonics, magnonics, energy conversion and harvesting, and power electronics

Nanoscale resistive switching memory devices: a review

In this review the different concepts of nanoscale resistive switching memory devices are described and classified according to their I–V behaviour and the underlying physical switching mechanisms. By means of the most important representative devices, the current state of electrical performance characteristics is illuminated in-depth. Moreover, the ability of resistive switching devices to be integrated into state-of-the-art CMOS circuits under the additional consideration with a suitable selector device for memory array operation is assessed. From this analysis, and by factoring in the maturity of the different concepts, a ranking methodology for application of the nanoscale resistive switching memory devices in the memory landscape is derived. Finally, the suitability of the different device concepts for beyond pure memory applications, such as brain inspired and neuromorphic computational or logic in memory applications that strive to overcome the vanNeumann bottleneck, is discussed

Low-temperature amorphous oxide semiconductors for thin-film transistors and memristors: physical insights and applications

While amorphous oxides semiconductors (AOS), namely InGaZnO (IGZO), have found market application in the display industry, their disruptive properties permit to envisage for more advanced concepts such as System-on-Panel (SoP) in which AOS devices could be used for addressing (and readout) of sensors and displays, for communication, and even for memory as oxide memristors are candidates for the next-generation memories. This work concerns the application of AOS for these applications considering the low thermal budgets (< 180 °C) required for flexible, low cost and alternative substrates. For maintaining low driving voltages, a sputtered multicomponent/multi-layered high-κ dielectric (Ta2O5+SiO2) was developed for low temperature IGZO TFTs which permitted high performance without sacrificing reliability and stability. Devices’ performance under temperature was investigated and the bias and temperature dependent mobility was modelled and included in TCAD simulation. Even for IGZO compositions yielding very high thermal activation, circuit topologies for counteracting both this and the bias stress effect were suggested. Channel length scaling of the devices was investigated, showing that operation for radio frequency identification (RFID) can be achieved without significant performance deterioration from short channel effects, which are attenuated by the high-κ dielectric, as is shown in TCAD simulation. The applicability of these devices in SoP is then exemplified by suggesting a large area flexible radiation sensing system with on-chip clock-generation, sensor matrix addressing and signal read-out, performed by the IGZO TFTs. Application for paper electronics was also shown, in which TCAD simulation was used to investigate on the unconventional floating gate structure. AOS memristors are also presented, with two distinct operation modes that could be envisaged for data storage or for synaptic applications. Employing typical TFT methodologies and materials, these are ease to integrate in oxide SoP architectures

Standards for the Characterization of Endurance in Resistive Switching Devices

Resistive switching (RS) devices are emerging electronic components that could have applications in multiple types of integrated circuits, including electronic memories, true random number generators, radiofrequency switches, neuromorphic vision sensors, and artificial neural networks. The main factor hindering the massive employment of RS devices in commercial circuits is related to variability and reliability issues, which are usually evaluated through switching endurance tests. However, we note that most studies that claimed high endurances >106 cycles were based on resistance versus cycle plots that contain very few data points (in many cases even <20), and which are collected in only one device. We recommend not to use such a characterization method because it is highly inaccurate and unreliable (i.e., it cannot reliably demonstrate that the device effectively switches in every cycle and it ignores cycle-to-cycle and device-to-device variability). This has created a blurry vision of the real performance of RS devices and in many cases has exaggerated their potential. This article proposes and describes a method for the correct characterization of switching endurance in RS devices; this method aims to construct endurance plots showing one data point per cycle and resistive state and combine data from multiple devices. Adopting this recommended method should result in more reliable literature in the field of RS technologies, which should accelerate their integration in commercial products