Elsevier

Carbon

Volume 85, April 2015, Pages 383-396
Carbon

Review
Memristive devices based on graphene oxide

https://doi.org/10.1016/j.carbon.2015.01.011Get rights and content

Abstract

Memristors are nanoscale devices able to generate intense fields by the application of relatively low voltages, which warrants peculiar properties such as fast, non-volatile and low-energy electrical switching, as well as the possibility of retaining their internal resistance state according to the history of applied voltage and current. Memristors are predicted to revolutionize the current approaches in computer electronics architecture with their application, for instance, as resistive random access memory. Moreover they are indicated as the first brick to create neuromorphic systems and artificial intelligence. The use of graphene oxide as active material for memristive switching systems offers an exciting alternative to other classes of materials, such as transition metal oxide and organic thin films. Graphene oxide is electrically insulating due to the presence of oxygen functionalities, with the advantage of being truly atomically-thin, which makes it the perfect candidate for the fabrication of memristive devices. Different mechanisms were recently proposed for graphene oxide memristive systems, but a definitive evidence in their support is still missing. This challenge has stimulated an extensive activity towards a robust and predictive understanding of the physical phenomena that lie behind this peculiar behavior. A comparative review of several graphene oxide memristive devices is here provided, with a distinction between two different mechanisms for resistance switching: oxygen ions drift and metal filament formation.

Introduction

The fast and constant development that has characterized the semiconductors industry in the last decades was primarily focused on the miniaturization of devices, in order to achieve a continual improvement of their performances. In this regard, the development of nanoscale structures will be the key point to perpetrate the Moore’s law [1] beyond the actual physical limits, enabling a new era for computing. The development of memristors perfectly fits in this framework, due to their high scalability down to the nanometer scale, as well as the possibility of being exploited in applications such as non-volatile memory and low-power resistive switching devices. For these reasons, since their first demonstration, memristive systems became an issue of investigation for many applications, although their further growth appears to be slowed down due to the complexity in predicting and controlling the chemical/physical mechanisms that lie behind the memristive phenomena, which seem to be extremely stochastic [2].

Despite this drawback, many different working devices were reported in the recent literature. Beside the various perovskite oxide materials [3], [4], binary transition metal oxides (like TiO2 [5], Ta2O5 [6], NiO [7]), chalcogenides [8], [9] and organic materials [10], [11], in the latest years a growing attention was directed to carbon-based devices, in particular to those based on graphene and graphene oxide [12], due to the unique properties of this class of materials.

The aim of this work is to review the recent literature in order to give an overview of the state of the art of graphene-based memristive devices, with a particular attention to their switching mechanism.

This review is organized as follows. In Chapter 2 a brief introduction to the properties and methods for the synthesis of graphene and graphene oxide is given. Chapter 3 introduces the concept of memristor devices, presenting their most relevant proprieties and indicating the characteristics that should define a working device. Chapter 4 is dedicated to the explanation of the Metal/Insulator/Metal mechanism that lies behind graphene oxide based memristive systems. Particular attention is devoted to the discussion of two different mechanisms for resistance switching that were proposed in the literature, i.e. the oxygen ions drift and the metal filament formation. For both mechanisms, a complete description of the phenomena is given and the most significant evidences are summarized. The second part of Chapter 4 is focused on the criteria normally adopted for the choice of materials for the fabrication of top and bottom electrodes, and on the presentation of the characteristics of memristive operation of the different device types. In the last part of Chapter 4 the resistive switching mechanisms in memristive devices based on multilayer structures, conjugated polymer-functionalized GO thin films and their properties are explained. Moreover, a quick overview of other typologies of graphene-based memristive device is given. In Chapter 5 the applications of GO in flexible electronics are summarized. Finally, Chapter 6 gives the conclusive remarks of the review, with a short discussion on future perspectives and developments.

Section snippets

Graphene and graphene oxide

Graphene has attracted worldwide attention because of the strikingly unconventional phenomena that were predicted and measured, which are mainly originated by the fact that electrons behave as massless relativistic particles [13]. From this, a variety of interdisciplinary properties arise, including excellent electron mobility at room temperature (2.5 · 105 cm2 V−1 s−1), high thermal conductivity (5000 Wm−1 K−1), and superior mechanical properties [14], [15], which make this material particularly

Memristors

The existence of a fourth two-terminal circuit component was postulated by Leon O. Chua in 1971 [46], on the basis of a simple logic deduction. Considering the four fundamental circuit variables, i.e. current (I), voltage (V), magnetic flux (φ) and charge (q), six different mathematical relations can be defined in order to invariably couple them. The first two of these relations are given by integrating over time voltage and current, obtaining respectively magnetic flux and charge. Other three

Memristor based on graphene oxide

One of the most common memristor structure reported in literature is the sandwiched Metal/Insulator/Metal (MIM) structure, which can be fabricated using an extremely wide range of metal electrodes and insulators. Graphene oxide synthesized by oxidation and exfoliation of bulk graphite can be easily dispersed in water and then deposited on the bottom electrode material through different techniques, like spin-coating, drop casting, vacuum filtration, ink-jet printing or Langmuir Blodgett

Application of GO in flexible electronics

As previously reported in paragraph 2, GO can be produced from bulk graphite by simple and scalable techniques. GO thin films can be transferred or deposited by a variety of methods, for example by drop casting [89], [36], rapid freezing by spraying [90], dip coating [91], inkjet printing [22], [23], [43] or simply by spin-coating, on any kind of substrate including flexible substrates, and subsequently integrated into practical devices in conjunction with standard CMOS processes [56], allowing

Conclusions

The development of reliable memristive systems is a fundamental technological innovation that will find application in artificial intelligence as resistive random access memory and neuromorphic computing. Several examples of working memristive device based on GO have been proposed in the recent literature, exhibiting good switching proprieties (high switching ratio and low SET and RESET voltage), as well as good retention and endurance times.

However, despite the unique features displayed by GO,

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