Resistive switching (RS) is an interesting property shown by some materials systems that, especially during the last decade, has gained a lot of interest for the fabrication of electronic devices, with electronic nonvolatile memories being those that have received the most attention. The presence and quality of the RS phenomenon in a materials system can be studied using different prototype cells, performing different experiments, displaying different figures of merit, and developing different computational analyses. Therefore, the real usefulness and impact of the findings presented in each study for the RS technology will be also different. This manuscript describes the most recommendable methodologies for the fabrication, characterization, and simulation of RS devices, as well as the proper methods to display the data obtained. The idea is to help the scientific community to evaluate the real usefulness and impact of an RS study for the development of RS technology. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

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Recommended Methods to Study Resistive Switching Devices

Rapid digital technology advancement has resulted in a tremendous increase in computing tasks imposing stringent energy efficiency and area efficiency requirements on next-generation computing. To meet the growing data-driven demand, in-memory computing and transistor-based computing have emerged as potent technologies for the implementation of matrix and logic computing. However, to fulfil the future computing requirements new materials are urgently needed to complement the existing Si complementary metal–oxide–semiconductor technology and new technologies must be developed to enable further diversification of electronics and their applications. The abundance and rich variety of electronic properties of two-dimensional materials have endowed them with the potential to enhance computing energy efficiency while enabling continued device downscaling to a feature size below 5 nm. In this Review, from the perspective of matrix and logic computing, we discuss the opportunities, progress and challenges of integrating two-dimensional materials with in-memory computing and transistor-based computing technologies. This Review discusses the recent progress and future prospects of two-dimensional materials for next-generation nanoelectronics.

Two-dimensional materials for next-generation computing technologies.

Memristive and nanoionic devices have recently emerged as leading candidates for neuromorphic computing architectures. While top-down fabrication based on conventional bulk materials has enabled many early neuromorphic devices and circuits, bottom-up approaches based on low-dimensional nanomaterials have shown novel device functionality that often better mimics a biological neuron. In addition, the chemical, structural and compositional tunability of low-dimensional nanomaterials coupled with the permutational flexibility enabled by van der Waals heterostructures offers significant opportunities for artificial neural networks. In this Review, we present a critical survey of emerging neuromorphic devices and architectures enabled by quantum dots, metal nanoparticles, polymers, nanotubes, nanowires, two-dimensional layered materials and van der Waals heterojunctions with a particular emphasis on bio-inspired device responses that are uniquely enabled by low-dimensional topology, quantum confinement and interfaces. We also provide a forward-looking perspective on the opportunities and challenges of neuromorphic nanoelectronic materials in comparison with more mature technologies based on traditional bulk electronic materials. This Review highlights the progress made towards the development of neuromorphic devices and architectures enabled by low-dimensional nanomaterials

Neuromorphic nanoelectronic materials

The rapid development of information technology has led to urgent requirements for high efficiency and ultralow power consumption. In the past few decades, neuromorphic computing has drawn extensive attention due to its promising capability in processing massive data with extremely low power consumption. Here, we offer a comprehensive review on emerging artificial neuromorphic devices and their applications. In light of the inner physical processes, we classify the devices into nine major categories and discuss their respective strengths and weaknesses. We will show that anion/cation migration-based memristive devices, phase change, and spintronic synapses have been quite mature and possess excellent stability as a memory device, yet they still suffer from challenges in weight updating linearity and symmetry. Meanwhile, the recently developed electrolyte-gated synaptic transistors have demonstrated outstanding energy efficiency, linearity, and symmetry, but their stability and scalability still need to be optimized. Other emerging synaptic structures, such as ferroelectric, metal–insulator transition based, photonic, and purely electronic devices also have limitations in some aspects, therefore leading to the need for further developing high-performance synaptic devices. Additional efforts are also demanded to enhance the functionality of artificial neurons while maintaining a relatively low cost in area and power, and it will be of significance to explore the intrinsic neuronal stochasticity in computing and optimize their driving capability, etc. Finally, by looking into the correlations between the operation mechanisms, material systems, device structures, and performance, we provide clues to future material selections, device designs, and integrations for artificial synapses and neurons.

A comprehensive review on emerging artificial neuromorphic devices

As the research on artificial intelligence booms, there is broad interest in brain-inspired computing using novel neuromorphic devices. The potential of various emerging materials and devices for neuromorphic computing has attracted extensive research efforts, leading to a large number of publications. Going forward, in order to better emulate the brain's functions, its relevant fundamentals, working mechanisms, and resultant behaviors need to be re-visited, better understood, and connected to electronics. A systematic overview of biological and artificial neural systems is given, along with their related critical mechanisms. Recent progress in neuromorphic devices is reviewed and, more importantly, the existing challenges are highlighted to hopefully shed light on future research directions.

Bridging Biological and Artificial Neural Networks with Emerging Neuromorphic Devices: Fundamentals, Progress, and Challenges.

Neuromorphic computing systems, which use electronic synapses and neurons, could overcome the energy and throughput limitations of today’s computing architectures. However, electronic devices that can accurately emulate the short- and long-term plasticity learning rules of biological synapses remain limited. Here, we show that multilayer hexagonal boron nitride (h-BN) can be used as a resistive switching medium to fabricate high-performance electronic synapses. The devices can operate in a volatile or non-volatile regime, enabling the emulation of a range of synaptic-like behaviour, including both short- and long-term plasticity. The behaviour results from a resistive switching mechanism in the h-BN stack, based on the generation of boron vacancies that can be filled by metallic ions from the adjacent electrodes. The power consumption in standby and per transition can reach as low as 0.1 fW and 600 pW, respectively, and with switching times reaching less than 10 ns, demonstrating their potential for use in energy-efficient brain-like computing. Vertically structured electronic synapses, which exhibit both short- and long-term plasticity, can be created using layered two-dimensional hexagonal boron nitride.

Electronic synapses made of layered two-dimensional materials

Potassium Hydroxide Mixed with Lithium Hydroxide: An Advanced Electrolyte for Oxygen Evolution Reaction

Hafnia-based ferroelectric thin films are promising for semiconductor memory and neuromorphic computing applications. Amorphous, as-deposited, thin-film binary alloys of HfO2 and ZrO2 transform to the metastable, orthorhombic ferroelectric phase during post-deposition annealing and cooling. This transformation is generally thought to involve formation of a tetragonal precursor phase that distorts into the orthorhombic phase during cooling. In this work, we systematically study the effects of atomic layer deposition (ALD) temperature on the ferroelectricity of post-deposition-annealed Hf0.5Zr0.5O2 (HZO) thin films. Seed crystallites having interplanar spacings consistent with the polar orthorhombic phase are observed by a plan-view transmission electron microscope in HZO thin films deposited at an elevated ALD temperature. After ALD under conditions that promote formation of these nanocrystallites, high-polarization (Pr > 18 μC/cm2) ferroelectric switching is observed after rapid thermal annealing (RTA) at low temperature (350 °C). These results indicate the presence of minimal non-ferroelectric phases retained in the films after RTA when the ALD process forms nanocrystalline particles that seed subsequent formation of the polar orthorhombic phase.

Nanocrystallite Seeding of Metastable Ferroelectric Phase Formation in Atomic Layer-Deposited Hafnia-Zirconia Alloys.

As an emerging nonvolatile memory technology, HfO2‐based ferroelectrics exhibit excellent compatibility with silicon CMOS process flows; however, the reliability of polarization switching in these materials remains a major challenge. During repeated field programming and erase of the polarization state of initially pristine HfO2‐based ferroelectric capacitors, the magnitude of the measured polarization increases, a phenomenon known as “wake‐up”. In this study, the authors attempt to understand what causes the wake‐up effect in Hf0.5Zr0.5O2 (HZO) capacitors using nondestructive methods that probe statistically significant sample volumes. Synchrotron X‐ray diffraction reveals a concerted shift in HZO Bragg peak position as a function of polarization switching cycle number in films prepared under conditions such that they exhibit extremely large (≈3000%) wake‐up. In contrast, a control sample with insignificant wake‐up shows no such peak shift. Capacitance – voltage measurements show evolution in the capacitance loop with switching cycle number for the wake‐up sample and no change for the control sample. Piezoresponse force microscopy measurements are utilized to visualize the domain switching with wake‐up. The combination of these observations clearly demonstrates that wake‐up is caused by a field‐driven phase transformation of the tetragonal phase to the metastable ferroelectric orthorhombic phase during polarization switching of HZO capacitors.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/aelm.202300016

Field‐Induced Ferroelectric Phase Evolution During Polarization “Wake‐Up” in Hf0.5Zr0.5O2 Thin Film Capacitors

Ferroelectric properties of individual TiN/Hf0.5Zr0.5O2/TiN capacitors have been measured for technologically relevant areas as small as 60 nm <inline-formula> <tex-math notation="LaTeX">$\times70$ </tex-math></inline-formula> nm, using direct detection of ultralow charge. A crossbar architecture has been utilized to fabricate the ferroelectric capacitors. Switching polarization of <inline-formula> <tex-math notation="LaTeX">$40.1 \mu \text{C}$ </tex-math></inline-formula>/cm<inline-formula> <tex-math notation="LaTeX">$^{2} \ge \text{P}_{\text{sw}} \ge 16.7 \mu \text{C}$ </tex-math></inline-formula>/cm2 and coercive field 1.4 MV/cm <inline-formula> <tex-math notation="LaTeX">$\ge \text{E}_{c} \ge1.09$ </tex-math></inline-formula> MV/cm have been observed for sizes between <inline-formula> <tex-math notation="LaTeX">$1.1 \mu \text{m}$ </tex-math></inline-formula>2 and 4200 nm2 without discernable trend as function of capacitor size in the present data set. Measured bipolar stress endurance exceeds the maximum measured cycles of 1010 although some capacitors start to show signs of degradation after 109 cycles. A clear correlation between Psw degradation and increased leakage current is observed. The direct measurement of such small area capacitors has been enabled by equipment and circuit design innovations. The present setup allows direct measurement of ferroelectric properties for capacitors as small as 1900 nm2 while further improvements could extend the size limit to 950 nm2 where the design window appears to close.

Zhouchangwan Yu

Papers

Electronic synapses made of layered two-dimensional materials

Potassium Hydroxide Mixed with Lithium Hydroxide: An Advanced Electrolyte for Oxygen Evolution Reaction

Nanocrystallite Seeding of Metastable Ferroelectric Phase Formation in Atomic Layer-Deposited Hafnia-Zirconia Alloys.

Field‐Induced Ferroelectric Phase Evolution During Polarization “Wake‐Up” in Hf0.5Zr0.5O2 Thin Film Capacitors

Measurement of Ferroelectric Properties of Nanometer Scaled Individual Metal/Hf0.5Zr0.5O2/Metal Capacitors