The discovery of the enhancement of Raman scattering by molecules adsorbed on nanostructured metal surfaces is a landmark in the history of spectroscopic and analytical techniques. Significant experimental and theoretical effort has been directed toward understanding the surface-enhanced Raman scattering (SERS) effect and demonstrating its potential in various types of ultrasensitive sensing applications in a wide variety of fields. In the 45 years since its discovery, SERS has blossomed into a rich area of research and technology, but additional efforts are still needed before it can be routinely used analytically and in commercial products. In this Review, prominent authors from around the world joined together to summarize the state of the art in understanding and using SERS and to predict what can be expected in the near future in terms of research, applications, and technological development. This Review is dedicated to SERS pioneer and our coauthor, the late Prof. Richard Van Duyne, whom we lost during the preparation of this article.

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Present and Future of Surface-Enhanced Raman Scattering

The accumulation and extrusion of Ca2+ in the pre- and postsynaptic compartments play a critical role in initiating plastic changes in biological synapses. To emulate this fundamental process in electronic devices, we developed diffusive Ag-in-oxide memristors with a temporal response during and after stimulation similar to that of the synaptic Ca2+ dynamics. In situ high-resolution transmission electron microscopy and nanoparticle dynamics simulations both demonstrate that Ag atoms disperse under electrical bias and regroup spontaneously under zero bias because of interfacial energy minimization, closely resembling synaptic influx and extrusion of Ca2+, respectively. The diffusive memristor and its dynamics enable a direct emulation of both short- and long-term plasticity of biological synapses, representing an advance in hardware implementation of neuromorphic functionalities.

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Memristors with diffusive dynamics as synaptic emulators for neuromorphic computing

Modern computers are based on the von Neumann architecture in which computation and storage are physically separated: data are fetched from the memory unit, shuttled to the processing unit (where computation takes place) and then shuttled back to the memory unit to be stored. The rate at which data can be transferred between the processing unit and the memory unit represents a fundamental limitation of modern computers, known as the memory wall. In-memory computing is an approach that attempts to address this issue by designing systems that compute within the memory, thus eliminating the energy-intensive and time-consuming data movement that plagues current designs. Here we review the development of in-memory computing using resistive switching devices, where the two-terminal structure of the devices, their resistive switching properties, and direct data processing in the memory can enable area- and energy-efficient computation. We examine the different digital, analogue, and stochastic computing schemes that have been proposed, and explore the microscopic physical mechanisms involved. Finally, we discuss the challenges in-memory computing faces, including the required scaling characteristics, in delivering next-generation computing. This Review Article examines the development of in-memory computing using resistive switching devices.

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In-memory computing with resistive switching devices

This review article attempts to provide a comprehensive review of the recent progress in the so-called resistive random access memories (RRAMs) First, a brief introduction is presented to describe the construction and development of RRAMs, their potential for broad applications in the fields of nonvolatile memory, unconventional computing and logic devices, and the focus of research concerning RRAMs over the past decade Second, both inorganic and organic materials used in RRAMs are summarized, and their respective advantages and shortcomings are discussed Third, the important switching mechanisms are discussed in depth and are classified into ion migration, charge trapping/de-trapping, thermochemical reaction, exclusive mechanisms in inorganics, and exclusive mechanisms in organics Fourth, attention is given to the application of RRAMs for data storage, including their current performance, methods for performance enhancement, sneak-path issue and possible solutions, and demonstrations of 2-D and 3-D crossbar arrays Fifth, prospective applications of RRAMs in unconventional computing, as well as logic devices and multi-functionalization of RRAMs, are comprehensively summarized and thoroughly discussed The present review article ends with a short discussion concerning the challenges and future prospects of the RRAMs

Recent progress in resistive random access memories: Materials, switching mechanisms, and performance

Creating functional electrical circuits using individual or ensemble molecules, often termed as “molecular-scale electronics”, not only meets the increasing technical demands of the miniaturization of traditional Si-based electronic devices, but also provides an ideal window of exploring the intrinsic properties of materials at the molecular level. This Review covers the major advances with the most general applicability and emphasizes new insights into the development of efficient platform methodologies for building reliable molecular electronic devices with desired functionalities through the combination of programmed bottom-up self-assembly and sophisticated top-down device fabrication. First, we summarize a number of different approaches of forming molecular-scale junctions and discuss various experimental techniques for examining these nanoscale circuits in details. We then give a full introduction of characterization techniques and theoretical simulations for molecular electronics. Third, we highlig...

Molecular-Scale Electronics: From Concept to Function

Nanoscale metal inclusions play an important role in solid-state dielectric devices. Here, the authors demonstrate that these inclusions can change their shape, size and position in response to an applied electric field, and that electrochemical processes can lead to metal cluster nucleation and growth.

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Electrochemical dynamics of nanoscale metallic inclusions in dielectrics

Redox-based nanoionic resistive memory cells are one of the most promising emerging nanodevices for future information technology with applications for memory, logic and neuromorphic computing. Recently, the serendipitous discovery of the link between redox-based nanoionic-resistive memory cells 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-zero-crossing 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 redox-based nanoionic-resistive memory 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.

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Nanobatteries in redox-based resistive switches require extension of memristor theory

The realization of logic operations within passive crossbar memory arrays is a promising approach to expand the fields of application of such architectures. Material implication was recently suggested as the basic function of memristive crossbar junctions, and single bipolar resistive switches (BRS) as well as complementary resistive switches (CRS) were shown to be capable of realizing this logical functionality. Based on a systematic analysis of the Boolean functions, we demonstrate here that 14 of 16 Boolean functions can be realized with a single BRS or CRS cell in at most three sequential cycles. Since the read-out step is independent of the logic operation steps, the result of the logic operation is directly stored to memory, making logic-in-memory applications feasible.

https://iopscience.iop.org/article/10.1088/0957-4484/23/30/305205/pdf

Beyond von Neumann—logic operations in passive crossbar arrays alongside memory operations

Resistive switching memories (ReRAMs) are the major candidates for replacing the state-of-the-art memory technology in future nanoelectronics. These nonvolatile memory cells are based on nanoionic redox processes and offer prospects for high scalability, ultrafast write and read access, and low power consumption. The interfacial electrochemical reactions of oxidation and reduction of ions necessarily needed for resistive switching result inevitably in nonequilibrium states, which play a fundamental role in the processes involved during device operation. We report on nonequilibrium states in SiO2-based ReRAMs being induced during the resistance transition. It is demonstrated that the formation of metallic cations proceeds in parallel to reduction of moisture, supplied by the ambient. The latter results in the formation of an electromotive force in the range of up to 600 mV. The outcome of the study highlights the hitherto overlooked necessity of a counter charge/reaction to keep the charge electroneutrality in cation-transporting thin films, making it hard to analyze and compare experimental results under different ambient conditions such as water partial pressure. Together with the dependence of the electromotive force on the ambient, these results contribute to the microscopic understanding of the resistive switching phenomena in cation-based ReRAMs.

Generic Relevance of Counter Charges for Cation-Based Nanoscale Resistive Switching Memories

The strongly nonlinear switching kinetics of electrochemical metallization memory (ECM) cells are investigated using an advanced 1D simulation model. It is based on the electrochemical growth and dissolution of a Ag or Cu filament within a solid thin film and accounts for nucleation effects, charge transfer, and cation drift. The model predictions are consistent with experimental switching results of a time range of 12 orders of magnitude obtained from silver iodide (AgI) based ECM cells. By analyzing the simulation results the electrochemical processes limiting the switching kinetics are revealed. This study provides new insights into the understanding of the limiting electrochemical processes determining the switching kinetics of ECM cells.

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Stefan Tappertzhofen

Papers

Electrochemical dynamics of nanoscale metallic inclusions in dielectrics

Nanobatteries in redox-based resistive switches require extension of memristor theory

Beyond von Neumann—logic operations in passive crossbar arrays alongside memory operations

Generic Relevance of Counter Charges for Cation-Based Nanoscale Resistive Switching Memories

Switching kinetics of electrochemical metallization memory cells