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Understanding the thermal conductivity of chromium doped V2O3 is crucial for optimizing the design of selectors for memory and neuromorphic devices. We utilized the time-domain thermoreflectance technique to measure the thermal conductivity of chromium doped V2O3 across varying concentrations, spanning the doping induced metal-insulator transition. In addition, different oxygen stoichiometries and film thicknesses were investigated in their crystalline and amorphous phases. Chromium doping concentration (0%-30%) and the degree of crystallinity emerged as the predominant factors influencing the thermal properties, while the effect of oxygen flow (600-1400 ppm) during deposition proved to be negligible. Our observations indicate that even in the metallic phase of V2O3, the lattice contribution is the dominant factor in thermal transport with no observable impact from the electrons on heat transport. Finally, the thermal conductivity of both amorphous and crystalline V2O3 was measured at cryogenic temperatures (80-450 K). Our thermal conductivity measurements as a function of temperature reveal that both phases exhibit behavior similar to amorphous materials, indicating pronounced phonon scattering effects in the crystalline phase of V2O3., Comment: Submitted to APL

The roadmap is organized into several thematic sections, outlining current computing challenges, discussing the neuromorphic computing approach, analyzing mature and currently utilized technologies, providing an overview of emerging technologies, addressing material challenges, exploring novel computing concepts, and finally examining the maturity level of emerging technologies while determining the next essential steps for their advancement., Comment: 90 pages, 22 figures, roadmap, neuromorphic

The pressure driven Mott-transition in Chromium doped V2O3 films is investigated by direct electrical measurements on polycrystalline films with thicknesses down to 10 nm, and doping concentrations of 2%, 5% and 15%. A change in resistivity of nearly two orders of magnitude is found for 2% doping. A simulation model based on a scaling law description of the phase transition and percolative behavior in a resistor lattice is developed. This is used to show that despite significant deviations in the film structure from single crystals, the transition behavior is very similar. Finally, the influence of the variability between grains on the characteristics of scaled devices is investigated and found to allow for scaling down to at least 50 nm device width.

We present a fast generative modeling approach for resistive memories that reproduces the complex statistical properties of real-world devices. To enable efficient modeling of analog circuits, the model is implemented in Verilog-A. By training on extensive measurement data of integrated 1T1R arrays (6,000 cycles of 512 devices), an autoregressive stochastic process accurately accounts for the cross-correlations between the switching parameters, while non-linear transformations ensure agreement with both cycle-to-cycle (C2C) and device-to-device (D2D) variability. Benchmarks show that this statistically comprehensive model achieves read/write throughputs exceeding those of even highly simplified and deterministic compact models., Comment: This work has been submitted to the IEEE for possible publication. Copyright may be transferred without notice, after which this version may no longer be accessible. Code is available at https://zenodo.org/doi/10.5281/zenodo.10942560

Memristor-aided logic (MAGIC) design style holds a high promise for realizing digital logic-in-memory functionality. The ability to implement a specific gate in a MAGIC design style hinges on the SET-to-RESET threshold ratio. The TaOx memristive devices exhibit distinct SET-to-RESET ratios, enabling the implementation of OR and NOT operations. As the adoption of the MAGIC design style gains momentum, it becomes crucial to understand the breakdown of energy consumption in the various phases of its operation. This paper presents experimental demonstrations of the OR and NOT gates on a 1T1R crossbar array. Additionally, it provides insights into the energy distribution for performing these operations at different stages. Through our experiments across different gates, we found that the energy consumption is dominated by initialization in the MAGIC design style. The energy split-up is 14.8%, 85%, and 0.2% for execution, initialization, and read operations respectively., Comment: Accepted in VLSID 2024

Brain-inspired computing proposes a set of algorithmic principles that hold promise for advancing artificial intelligence. They endow systems with self learning capabilities, efficient energy usage, and high storage capacity. A core concept that lies at the heart of brain computation is sequence learning and prediction. This form of computation is essential for almost all our daily tasks such as movement generation, perception, and language. Understanding how the brain performs such a computation is not only important to advance neuroscience but also to pave the way to new technological brain-inspired applications. A previously developed spiking neural network implementation of sequence prediction and recall learns complex, high-order sequences in an unsupervised manner by local, biologically inspired plasticity rules. An emerging type of hardware that holds promise for efficiently running this type of algorithm is neuromorphic hardware. It emulates the way the brain processes information and maps neurons and synapses directly into a physical substrate. Memristive devices have been identified as potential synaptic elements in neuromorphic hardware. In particular, redox-induced resistive random access memories (ReRAM) devices stand out at many aspects. They permit scalability, are energy efficient and fast, and can implement biological plasticity rules. In this work, we study the feasibility of using ReRAM devices as a replacement of the biological synapses in the sequence learning model. We implement and simulate the model including the ReRAM plasticity using the neural simulator NEST. We investigate the effect of different device properties on the performance characteristics of the sequence learning model, and demonstrate resilience with respect to different on-off ratios, conductance resolutions, device variability, and synaptic failure., Comment: 23 pages, 13 Figures

Thin films of the prototypical charge transfer insulator NiO appear to be a promising material for novel nanoelectronic devices. The fabrication of the material is challenging however, and mostly a p-type semiconducting phase is reported. Here, the results of a factorial experiment are presented that allow optimization of the film properties of thin films deposited using sputtering. A cluster analysis is performed, and four main types of films are found. Among them, the desired insulating phase is identified. From this material, nanoscale devices are fabricated, which demonstrate that the results carry over to relevant length scales. Initial switching results are reported.

During the last decade, valence change memory (VCM) has been extensively studied due to its promising features, such as a high endurance and fast switching times. The information is stored in a high resistive state (logcial '0', HRS) and a low resistive state (logcial '1', LRS). It can also be operated in two different writing schemes, namely a unipolar switching mode (LRS and HRS are written at the same voltage polarity) and a bipolar switching mode (LRS and HRS are written at opposite voltage polarities). VCM, however, still suffers from a large variability during writing operations and also faults occur, which are not yet fully understood and, therefore, require a better understanding of the underlying fault mechanisms. In this study, a new intrinsic failure mechanism is identified, which prohibits RESET times (transition from LRS to HRS) faster than 400 ps and possibly also limits the endurance. We demonstrate this RESET speed limitation by measuring the RESET kinetics of two valence change memory devices (namely Pt/TaO$_\mathrm{x}$/Ta and Pt/ZrO$_\mathrm{x}$/Ta) in the time regime from 50 ns to 50 ps, corresponding to the fastest writing time reported for VCM. Faster RESET times were achieved by increasing the applied pulse voltage. Above a voltage threshold it was, however, no longer possible to reset both types of devices. Instead a unipolar SET (transition from HRS to LRS) event occurred, preventing faster RESET times. The occurrence of the unipolar SET is attributed to an oxygen exchange at the interface to the Pt~electrode, which can be suppressed by introducing an oxygen blocking layer at this interface, which also allowed for 50 ps fast RESET times., Comment: 27 pages, 18 figures and 69 references

The increasing demand for high-density data storage leads to an increasing interest in novel memory concepts with high scalability and the opportunity of storing multiple bits in one cell. A promising candidate is the redox-based resistive switch repositing the information in form of different resistance states. For reliable programming, the underlying physical parameters need to be understood. We reveal that the programmable resistance states are linked to internal series resistances and the fundamental nonlinear switching kinetics. The switching kinetics of Ta$_{2}$O$_{5}$-based cells was investigated in a wide range over 15 orders of magnitude from 250 ps to 10$^{5}$ s. We found strong evidence for a switching speed of 10 ps which is consistent with analog electronic circuit simulations. On all time scales, multi-bit data storage capabilities were demonstrated. The elucidated link between fundamental material properties and multi-bit data storage paves the way for designing resistive switches for memory and neuromorphic applications., Comment: Compiled PDF should contain 24 pages, 5 figures and 50 references

Future development of the modern nanoelectronics and its flagships internet of things and artificial intelligence as well as many related applications is largely associated with memristive elements. This technology offers a broad spectrum of functionalities, however, it follows predominantly a phenomenological approach and crucial challenge/limit for further development remains variability and lack of fundamental materials' design strategy. Here we demonstrate the vital importance of materials' purity for determining memristors' functionalities, showing that part per million foreign elements significantly change the performance. By appropriate choice of chemistry and amount of doping material we can selectively enhance desired operation mode. We highlight how dopant dependent structure and charge/potential distribution in the space charge layers and the cell capacitance determine the device kinetics and functions. We evidence for first time experimentally the relation between materials properties and switching/neuromorphic performance, thus providing rules and directions for a rational design of memristive devices.

Renewable energy conversion and storage, and greenhouse gas emission-free technologies are within the primary tasks and challenges for the society. Hydrogen fuel, produced by alkaline water electrolysis is fulfilling all these demands, however the technology is economically feeble, limited by the slow rate of oxygen evolution reaction. Complex metal oxides were suggested to overcome this problem being low-cost efficient catalysts. However, the insufficient long-term stability, degradation of structure and electrocatalytic activity are restricting their utilization. Here we report on a new perovskite-based self-assembling material BaCo0.98Ti0.02O3-$\delta$:Co3O4 with superior performance, showing outstanding properties compared to current state-of-the-art materials without degeneration of its properties even at 353 K. By chemical and structural analysis the degradation mechanism was identified and modified by selective doping. Short-range order and chemical composition rather than long-range order are factors determining the outstanding performance. The derived general design rules can be used for further development of oxide-based electrocatalytic materials., Comment: 24 pages, 3 Figures and 5 Extended Data Figures, 1 Table, including Suplementary Information

Solid-state programmable metallization cells have attracted considerable attention as memristive elements for Redox-based Resistive Random Access Memory (ReRAM) for low-power and low-voltage applications. In principle, liquid-state metallization cells could offer the same advantages for aqueous systems, such as biomedical lab-on-a-chip devices, but robust resistive switching has not yet been achieved in liquid electrolytes, where electrodeposition is notoriously unstable to the formation of fractal dendrites. Here, the recently discovered physics of shock electrodeposition are harnessed to stabilize aqueous copper growth in polycarbonate nanopores, whose surfaces are modified with charged polymers. Stable bipolar resistive switching is demonstrated for 500 cycles with <10s retention times, prior to any optimization of the geometry or materials.

Redox-based nanoionic resistive memory cells (ReRAMs) are one of the most promising emerging nano-devices for future information technology with applications for memory, logic and neuromorphic computing. Recently, the serendipitous discovery of the link between ReRAMs and memristors and memristive devices has further intensified the research in this field. Here we show on both a theoretical and an experimental level that nanoionic-type memristive elements are inherently controlled by non-equilibrium states resulting in a nanobattery. As a result the memristor theory must be extended to fit the observed non zerocrossing I-V characteristics. The initial electromotive force of the nanobattery depends on the chemistry and the transport properties of the materials system but can also be introduced during ReRAM cell operations. The emf has a strong impact on the dynamic behaviour of nanoscale memories, and thus, its control is one of the key factors for future device development and accurate modelling., Comment: Submitted to Nature Communications, Manuscript: 20 pages, 5 figures, Supplementary Information: 19 pages, 12 figures, 2 tables