Graphene is a wonder material with many superlatives to its name. It is the thinnest known material in the universe and the strongest ever measured. Its charge carriers exhibit giant intrinsic mobility, have zero effective mass, and can travel for micrometers without scattering at room temperature. Graphene can sustain current densities six orders of magnitude higher than that of copper, shows record thermal conductivity and stiffness, is impermeable to gases, and reconciles such conflicting qualities as brittleness and ductility. Electron transport in graphene is described by a Dirac-like equation, which allows the investigation of relativistic quantum phenomena in a benchtop experiment. This review analyzes recent trends in graphene research and applications, and attempts to identify future directions in which the field is likely to develop.

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Graphene: Status and Prospects

Graphene has been attracting great interest because of its distinctive band structure and physical properties. Today, graphene is limited to small sizes because it is produced mostly by exfoliating graphite. We grew large-area graphene films of the order of centimeters on copper substrates by chemical vapor deposition using methane. The films are predominantly single-layer graphene, with a small percentage (less than 5%) of the area having few layers, and are continuous across copper surface steps and grain boundaries. The low solubility of carbon in copper appears to help make this growth process self-limiting. We also developed graphene film transfer processes to arbitrary substrates, and dual-gated field-effect transistors fabricated on silicon/silicon dioxide substrates showed electron mobilities as high as 4050 square centimeters per volt per second at room temperature.

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Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper Foils

Problems associated with large-scale pattern growth of graphene constitute one of the main obstacles to using this material in device applications. Recently, macroscopic-scale graphene films were prepared by two-dimensional assembly of graphene sheets chemically derived from graphite crystals and graphene oxides. However, the sheet resistance of these films was found to be much larger than theoretically expected values. Here we report the direct synthesis of large-scale graphene films using chemical vapour deposition on thin nickel layers, and present two different methods of patterning the films and transferring them to arbitrary substrates. The transferred graphene films show very low sheet resistance of approximately 280 Omega per square, with approximately 80 per cent optical transparency. At low temperatures, the monolayers transferred to silicon dioxide substrates show electron mobility greater than 3,700 cm(2) V(-1) s(-1) and exhibit the half-integer quantum Hall effect, implying that the quality of graphene grown by chemical vapour deposition is as high as mechanically cleaved graphene. Employing the outstanding mechanical properties of graphene, we also demonstrate the macroscopic use of these highly conducting and transparent electrodes in flexible, stretchable, foldable electronics.

Large-scale pattern growth of graphene films for stretchable transparent electrodes

There is intense interest in graphene in fields such as physics, chemistry, and materials science, among others. Interest in graphene's exceptional physical properties, chemical tunability, and potential for applications has generated thousands of publications and an accelerating pace of research, making review of such research timely. Here is an overview of the synthesis, properties, and applications of graphene and related materials (primarily, graphite oxide and its colloidal suspensions and materials made from them), from a materials science perspective.

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Graphene and Graphene Oxide: Synthesis, Properties, and Applications

Fabrication techniques developed for graphene research allow the disassembly of many layered crystals (so-called van der Waals materials) into individual atomic planes and their reassembly into designer heterostructures, which reveal new properties and phenomena. Andre Geim and Irina Grigorieva offer a forward-looking review of the potential of layering two-dimensional materials into novel heterostructures held together by weak van der Waals interactions. Dozens of these one-atom- or one-molecule-thick crystals are known. Graphene has already been well studied but others, such as monolayers of hexagonal boron nitride, MoS2, WSe2, graphane, fluorographene, mica and silicene are attracting increasing interest. There are many other monolayers yet to be examined of course, and the possibility of combining graphene with other crystals adds even further options, offering exciting new opportunities for scientific exploration and technological innovation. Research on graphene and other two-dimensional atomic crystals is intense and is likely to remain one of the leading topics in condensed matter physics and materials science for many years. Looking beyond this field, isolated atomic planes can also be reassembled into designer heterostructures made layer by layer in a precisely chosen sequence. The first, already remarkably complex, such heterostructures (often referred to as ‘van der Waals’) have recently been fabricated and investigated, revealing unusual properties and new phenomena. Here we review this emerging research area and identify possible future directions. With steady improvement in fabrication techniques and using graphene’s springboard, van der Waals heterostructures should develop into a large field of their own.

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Van der Waals heterostructures

In this work we present a low cost and scalable technique, via ambient pressure chemical vapor deposition (CVD) on polycrystalline Ni films, to fabricate large area (∼cm2) films of single- to few-layer graphene and to transfer the films to nonspecific substrates. These films consist of regions of 1 to ∼12 graphene layers. Single- or bilayer regions can be up to 20 μm in lateral size. The films are continuous over the entire area and can be patterned lithographically or by prepatterning the underlying Ni film. The transparency, conductivity, and ambipolar transfer characteristics of the films suggest their potential as another materials candidate for electronics and opto-electronic applications.

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Large Area, Few-Layer Graphene Films on Arbitrary Substrates by Chemical Vapor Deposition

Graphene nanoribbons can exhibit either quasi-metallic or semiconducting behavior, depending on the atomic structure of their edges. Thus, it is important to control the morphology and crystallinity of these edges for practical purposes. We demonstrated an efficient edge-reconstruction process, at the atomic scale, for graphitic nanoribbons by Joule heating. During Joule heating and electron beam irradiation, carbon atoms are vaporized, and subsequently sharp edges and step-edge arrays are stabilized, mostly with either zigzag- or armchair-edge configurations. Model calculations show that the dominant annealing mechanisms involve point defect annealing and edge reconstruction.

https://science.sciencemag.org/content/sci/323/5922/1701.full.pdf

Controlled formation of sharp zigzag and armchair edges in graphitic nanoribbons.

The transferring and identification of single- and few- layer graphene sheets from SiO2/Si substrates to other types of substrates is presented. Features across large areas (∼cm2) having single and few-layer graphene flakes, obtained by the microcleaving of highly oriented pyrolytic graphite (HOPG), can be transferred reliably. This method enables the fast localization of graphene sheets on substrates on which optical microscopy does not allow direct and fast visualization of the thin graphene sheets. No major morphological deformations, corrugations, or defects are induced on the graphene films when transferred to the target surface. Moreover, the differentiation between single and bilayer graphene via the G′ (∼2700 cm−1) Raman peak is demonstrated on various substrates. This approach opens up possibilities for the fabrication of graphene devices on a substrate material other than SiO2/Si.

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Hyungbin Son

Papers

Large Area, Few-Layer Graphene Films on Arbitrary Substrates by Chemical Vapor Deposition

Controlled formation of sharp zigzag and armchair edges in graphitic nanoribbons.

Transferring and Identification of Single- and Few-Layer Graphene on Arbitrary Substrates

Synthesis and characterization of long strands of nitrogen-doped single-walled carbon nanotubes

Atomic Step-Templated Formation of Single-Wall Carbon Nanotube Patterns