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@PHDTHESIS{Chekol:971953,
      author       = {Chekol, Solomon Amsalu},
      othercontributors = {Waser, Rainer and Wuttig, Matthias},
      title        = {{U}nveiling the relaxation dynamics of ${A}g/{H}f{O}_{2}$
                      based diffusive memristors for use in neuromorphic
                      computing},
      school       = {RWTH Aachen University},
      type         = {Dissertation},
      address      = {Aachen},
      publisher    = {RWTH Aachen University},
      reportid     = {RWTH-2023-09925},
      pages        = {1 Online-Ressource : Illustrationen, Diagramme},
      year         = {2023},
      note         = {Veröffentlicht auf dem Publikationsserver der RWTH Aachen
                      University 2024; Dissertation, RWTH Aachen University, 2023},
      abstract     = {The rapid growth in volume and complexity of data and
                      transfer, driven by advancements in information technologies
                      such as artificial intelligence (AI), cloud computing, big
                      data, and machine learning, is placing significant demands
                      on computation power and speed. Traditional computing
                      architectures are facing challenges in meeting these demands
                      due to the Von Neumann bottleneck, which limits the data
                      transfer rate between the memory and the central processing
                      unit and causes high energy consumption. Today, neuromorphic
                      computing (NC) concepts that mimic the structure and
                      function of the biological brain are gaining popularity as
                      they promise energy-efficient and scalable computing
                      solutions. Currently, neuronal functionality is often
                      performed using a transistor-based neuron, which is area-
                      and energy-inefficient. Therefore, research in the "beyond
                      von Neumann" area is aimed at novel volatile switching
                      components with adjustable switching times, low power
                      consumption, and high scalability, which could potentially
                      be used as artificial neurons in NC circuits. These include
                      threshold-switching devices that switch abruptly from the
                      high-resistance state (HRS) to the low-resistance state
                      (LRS) at a defined voltage. As soon as the applied voltage
                      falls below a certain value, the cell relaxes back to the
                      initial HRS state. In particular, diffusive memristors built
                      from volatile electrochemical metallization (ECM) cells are
                      attracting attention in emerging NC areas such as temporal
                      encoding. These diffusive memristors consist of switching
                      layers made from oxides or chalcogenides sandwiched between
                      an electrochemically active electrode (e.g., Ag or Cu) and
                      an inert electrode (e.g., Pt metal). The cells can be
                      miniaturized down to the sub-micrometer range and the
                      switching itself relies on the formation and dissolution of
                      a metallic filament. Since the temporal behavior of
                      diffusive memristors is their main characteristic, it is of
                      crucial importance to understand the relaxation dynamics of
                      these devices from a physical perspective. This is a
                      prerequisite for optimizing and modulating the performance
                      of diffusive memristors, especially for applications
                      requiring precise control of switching times. Previous
                      approaches mainly describe the relaxation time as a function
                      of the given filament diameter while the filament growth
                      process is not considered. In contrast, the present work
                      takes a comprehensive approach based on the physical
                      description of filament formation and relaxation and a
                      possible dependence between the two. The goal is to develop
                      a deeper understanding of the relaxation dynamics of
                      diffusive memristors, with particular emphasis on the
                      influence of SET parameters on the structure and diameter of
                      the filament formed in each case. To this end, devices were
                      fabricated from an amorphous HfO2 layer of a few nanometers
                      thickness sandwiched between electrode layers of Ag and Pt.
                      For material influence studies, SiO2 as an electrolyte layer
                      and two other metals (TiN and W) as alternative counter
                      electrodes (CEs) were also investigated. By evaluating the
                      transient current response to applied voltage pulses, the
                      SET kinetics and relaxation dynamics of the cells were
                      comprehensively analyzed. This allowed the identification of
                      different mechanisms as rate-limiting steps for filament
                      formation. In particular, three processes, namely
                      nucleation, electron-transfer, and mixed processes
                      (electron-transfer and ion-migration), were identified as
                      rate-limiting steps during the SET process. It was shown
                      that the relaxation time strongly depends on the selected
                      SET parameters. This is explained by the different
                      mechanisms of filament formation during the SET event. A
                      slow SET process at low voltage results in a relatively
                      thick filament that takes long to self-rupture. In contrast,
                      fast SET processes at high voltage lead to dendritic
                      filaments with short relaxation times. This assertion is
                      consistent with previous Monte Carlo simulations for similar
                      ECM cells and is further supported by physics-based
                      simulations using the "JART ECM" model developed in
                      collaboration with IWE 2/RWTH. Furthermore, it has been
                      demonstrated that applying a higher voltage pulse amplitude
                      or longer duration leads to a substantial increase in
                      relaxation time. This could be due to a small residual
                      voltage drop across the diffusive memristor in the LRS,
                      which causes further growth of the filament after closure.
                      The new findings resulting from the combined analysis of SET
                      kinetics and relaxation dynamics underline the importance of
                      filament formation for relaxation behavior and provide
                      important information for optimal operating conditions of
                      these threshold switches in NC circuits. In addition, the
                      work addresses the influence of CE material on the SET
                      kinetics of diffusive memristors. For example, both TiN and
                      W CEs slow down the switching speed compared to the Pt
                      electrode. This is attributed to the different
                      electrocatalytic activity of the different metals in the
                      redox reaction. Oxide formation at the interface of
                      non-noble metals (i.e., TiN and W) is also included in the
                      discussion. An important effect for use in NC circuits is
                      the significant influence of a series resistor on the
                      relaxation behavior. It has been shown that the magnitude of
                      the series resistance can strongly influence the
                      relationship between relaxation time and pulse voltage
                      amplitude. This can be attributed to the highly non-linear
                      nature of the SET kinetics and the role that a residual
                      voltage drop across the device in the ON-state plays in
                      promoting continued growth and strengthening of the
                      conductive filament.In summary, this work shows that
                      diffusive memristors based on volatile ECM cells have a high
                      potential for use as artificial neurons and further
                      applications in the field of NC. The obtained results
                      contribute to a deeper physical understanding of the
                      interplay between filament formation and relaxation and can
                      be directly transferred to the optimization of the
                      operational conditions of diffusive memristors in
                      neuromorphic circuits. This represents an important step
                      towards the realization of energy-efficient NC solutions. In
                      addition, the work classifies volatile devices in terms of
                      different adjustable relaxation times against the background
                      of various NC applications.},
      cin          = {520000 / 611610},
      ddc          = {620},
      cid          = {$I:(DE-82)520000_20140620$ / $I:(DE-82)611610_20140620$},
      pnm          = {BMBF 16ME0398K - Verbundprojekt: Neuro-inspirierte
                      Technologien der künstlichen Intelligenz für die
                      Elektronik der Zukunft - NEUROTEC II - (BMBF-16ME0398K) /
                      BMBF 16ME0399 - Verbundprojekt: Neuro-inspirierte
                      Technologien der künstlichen Intelligenz für die
                      Elektronik der Zukunft - NEUROTEC II - (BMBF-16ME0399) /
                      BMBF 03ZU1106AB - NeuroSys: "Memristor Crossbar
                      Architekturen (Projekt A) - B" (BMBF-03ZU1106AB)},
      pid          = {G:(DE-82)BMBF-16ME0398K / G:(DE-82)BMBF-16ME0399 /
                      G:(DE-Juel1)BMBF-03ZU1106AB},
      typ          = {PUB:(DE-HGF)11},
      doi          = {10.18154/RWTH-2023-09925},
      url          = {https://publications.rwth-aachen.de/record/971953},
}