Leakage current and resistive switching mechanisms in SrTiO3

PhD ThesisResistive switching random access memory devices have attracted considerable attention due to exhibiting fast programming, non-destructive readout, low power-consumption, high-density integration, and low fabrication-cost. Resistive switching has been observed in a wide range of materials but the underpinning mechanisms still have not been understood completely. This thesis presents a study of the leakage current and resistive switching mechanisms of SrTiO3 metal-insulator-metal devices fabricated using atomic layer deposition and pulse laser deposition techniques. First, the conduction mechanisms in SrTiO3 are investigated. The leakage current characteristics are highly sensitive to the polarity and magnitude of applied voltage bias, punctuated by sharp increases at high field. The characteristics are also asymmetric with bias and the negative to positive current crossover point always occurs at a negative voltage bias. A model comprising thermionic field emission and tunnelling phenomena is proposed to explain ii the dependence of leakage current upon the device parameters quantitatively. SrTiO3 also demonstrates bipolar switching behaviour where the current-density versus voltage (J-V) characteristics show asymmetry at all temperatures examined, with resistive switching behaviour observed at elevated temperatures. The asymmetry is explained by the relative lack of electron traps at one electrode, which is determined from the symmetric J-V curve obtained at room temperature due to the redistribution of the dominant electrical defects in the film. Evidence is presented for a model of resistive switching that originates from defect diffusion (possibly oxygen vacancies) at high temperatures. Finally, a peculiar resistive switching behaviour was observed in pulse laser deposited SrTiO3. This switching depends on both the amplitude and polarity of the applied voltage, and cannot be described as either bipolar or unipolar resistive switching. This behaviour is termed antipolar due to the opposite polarity of the set voltage relative to the previous reset voltage. The proposed model based on electron injection by tunnelling at interfaces and a Poole-Frenkel mechanism through the bulk is extended to explain the antipolar resistive switching behaviour. This model is quantified by use of a simple mathematical equation to simulate the experimental results

Resistance switching devices based on amorphous insulator-metal thin films

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 materials, spanning a large library of oxide and nitride insulator films, dispersed with transition and main-group metal atoms. Nanometallic RRAMs have superior properties that set them apart from other RRAMs. The critical switching voltage is independent of the film thickness/device area/temperature/switching speed. Trapped electrons are relaxed by electron-phonon interaction, adding stability which enables long-term memory retention. As electron-phonon interaction is mechanically altered, trapped electron can be destabilized, and sub-picosecond switching has been demonstrated using an electromagnetically generated stress pulse. AC impedance spectroscopy confirms the resistance state is spatially uniform, providing a capacitance that linearly scales with area and inversely scales with thickness. The spatial uniformity is also manifested in outstanding uniformity of switching properties. Device degradation, due to moisture, electrode oxidation and dielectrophoresis, is minimal when dense thin films are used or when a hermetic seal is provided. The potential for low power operation, multi-bit storage and complementary stacking have been demonstrated in various RRAM configurations.Comment: 523 pages, 215 figures, 10 chapter

Evaluation des performances des mémoires CBRAM (Conductive bridge memory) afin d’optimiser les empilements technologiques et les solutions d’intégration

The constant evolution of the data storage needs over the last decades have led the technological landscape to completely change and reinvent itself. From the early stage of magnetic storage to the most recent solid state devices, the bit density keeps increasing toward what seems from a consumer point of view infinite storage capacity and performances. However, behind each storage technology transition stand density and performances limitations that required strong research work to overcome. This manuscript revolves around one of the promising emerging technology aiming to revolutionize data storage landscape: the Conductive Bridge Random Access Memory (CBRAM). This technology based on the reversible formation and dissolution of a conductive path in a solid electrolyte matrix offers great advantages in term of power consumption, performances, density and the possibility to be integrated in the back end of line. However, for this technology to be competitive some roadblocks still have to be overcome especially regarding the technology variability, reliability and thermal stability. This manuscript proposes a comprehensive understanding of the CBRAM operations based on experimental results and a specially developed Kinetic Monte Carlo model. This understanding creates bridges between the physical properties of the materials involved in the devices and the devices performances (Forming, SET and RESET time and voltage, retention, endurance, variability). A strong emphasis is placed on the current limitations of the technology previously stated and how to overcome these limitations. Improvement of the thermal stability and device reliability are demonstrated with optimized operating conditions and proper devices engineering.Ces dernières décennies, la constante évolution des besoins de stockage de données a mené à un bouleversement du paysage technologique qui s’est complètement métamorphosé et réinventé. Depuis les débuts du stockage magnétique jusqu’aux plus récents dispositifs fondés sur l’électronique dit d’état solide, la densité de bits stockés continue d’augmenter vers ce qui semble du point de vue du consommateur comme des capacités de stockage et des performances infinies. Cependant, derrière chaque transition et évolution des technologies de stockage se cachent des limitations en termes de densité et performances qui nécessitent de lourds travaux de recherche afin d’être surmontées et repoussées. Ce manuscrit s’articule autour d’une technologie émergeante prometteuse ayant pour vocation de révolutionner le paysage du stockage de données : la mémoire à pont conducteur ou Conductive Bridge Random Access Memory (CBRAM). Cette technologie est fondée sur la formation et dissolution réversible d’un chemin électriquement conducteur dans un électrolyte solide. Elle offre de nombreux avantages face aux technologies actuelles tels qu’une faible consommation électrique, de très bonnes performances d’écriture et de lecture et la capacité d’être intégré aux seins des interconnexions métalliques d’une puce afin d’augmenter la densité de stockage. Malgré tout, pour que cette technologie soit compétitive certaines limitations ont besoin d’être surmontées et particulièrement sa variabilité et sa stabilité thermique qui posent encore problème. Ce manuscrit propose une compréhension physique globale du fonctionnement de la technologie CBRAM fondée sur une étude expérimentale approfondie couplée à un modèle Monte Carlo cinétique spécialement développé. Cette compréhension fait le lien entre les propriétés physiques des matériaux composant la mémoire CBRAM et ses performances (Tension et temps d’écriture et d’effacement, rétention de donnée, endurance et variabilité). Un fort accent est mis la compréhension des limites actuelle de la technologie et comment les repousser. Grâce à une optimisation des conditions d’opérations ainsi qu’à un travail d’ingénierie des dispositifs mémoire, il est démontré dans ce manuscrit une forte amélioration de la stabilité thermique ainsi que de la variabilité des états écrits et effacés

On‐Demand Reconfiguration of Nanomaterials: When Electronics Meets Ionics

Rapid advances in the semiconductor industry, driven largely by device scaling, are now approaching fundamental physical limits and face severe power, performance, and cost constraints. Multifunctional materials and devices may lead to a paradigm shift toward new, intelligent, and efficient computing systems, and are being extensively studied. Herein examines how, by controlling the internal ion distribution in a solid‐state film, a material’s chemical composition and physical properties can be reversibly reconfigured using an applied electric field, at room temperature and after device fabrication. Reconfigurability is observed in a wide range of materials, including commonly used dielectric films, and has led to the development of new device concepts such as resistive random‐access memory. Physical reconfigurability further allows memory and logic operations to be merged in the same device for efficient in‐memory computing and neuromorphic computing systems. By directly changing the chemical composition of the material, coupled electrical, optical, and magnetic effects can also be obtained. A survey of recent fundamental material and device studies that reveal the dynamic ionic processes is included, along with discussions on systematic modeling efforts, device and material challenges, and future research directions.By controlling the internal ion distribution in a solid‐state film, the material’s chemical composition and physical (i.e., electrical, optical, and magnetic) properties can be reversibly reconfigured, in situ, using an applied electric field. The reconfigurability is achieved in a wide range of materials, and can lead to the development of new memory, logic, and multifunctional devices and systems.Peer Reviewedhttps://deepblue.lib.umich.edu/bitstream/2027.42/141225/1/adma201702770.pdfhttps://deepblue.lib.umich.edu/bitstream/2027.42/141225/2/adma201702770_am.pd

Chalcogenide and metal-oxide memristive devices for advanced neuromorphic computing

Energy-intensive artificial intelligence (AI) is prevailing and changing the world, which requires energy-efficient computing technology. However, traditional AI driven by von Neumann computing systems suffers from the penalties of high-energy consumption and time delay due to frequent data shuttling. To tackle the issue, brain-inspired neuromorphic computing that performs data processing in memory is developed, reducing energy consumption and processing time. Particularly, some advanced neuromorphic systems perceive environmental variations and internalize sensory signals for localized in-senor computing. This methodology can further improve data processing efficiency and develop multifunctional AI products. Memristive devices are one of the promising candidates for neuromorphic systems due to their non-volatility, small size, fast speed, low-energy consumption, etc. In this thesis, memristive devices based on chalcogenide and metal-oxide materials are fabricated for neuromorphic computing systems. Firstly, a versatile memristive device (Ag/CuInSe2/Mo) is demonstrated based on filamentary switching. Non-volatile and volatile features are coexistent, which play multiple roles of non-volatile memory, selectors, artificial neurons, and artificial synapses. The conductive filaments’ lifetime was controlled to present both volatile and non-volatile behaviours. Secondly, the sensing functions (temperature and humidity) are explored based on Ag conductive filaments. An intelligent matter (Ag/Cu(In, Ga)Se2/Mo) endowing reconfigurable temperature and humidity sensations is developed for sensory neuromorphic systems. The device reversibly switches between two states with differentiable semiconductive and metallic features, demonstrating different responses to temperature and humidity variations. Integrated devices can be employed for intelligent electronic skin and in-sensor computing. Thirdly, the memristive-based sensing function of light was investigated. An optoelectronic synapse (ITO/ZnO/MoO3/Mo) enabling multi-spectrum sensitivity for machine vision systems is developed. For the first time, this optoelectronic synapse is practical for front-end retinomorphic image sensing, convolution processing, and back-end neuromorphic computing. This thesis will benefit the development of advanced neuromorphic systems pushing forward AI technology