Graphene-based materials exhibit remarkable electronic, optical, and mechanical properties, which has resulted in both high scientific interest and huge potential for a variety of applications. Furthermore, the family of graphene-based materials is growing because of developments in preparation methods. Raman spectroscopy is a versatile tool to identify and characterize the chemical and physical properties of these materials, both at the laboratory and mass-production scale. This technique is so important that most of the papers published concerning these materials contain at least one Raman spectrum. Thus, here, we systematically review the developments in Raman spectroscopy of graphene-based materials from both fundamental research and practical (i.e., device applications) perspectives. We describe the essential Raman scattering processes of the entire first- and second-order modes in intrinsic graphene. Furthermore, the shear, layer-breathing, G and 2D modes of multilayer graphene with different stacking orders are discussed. Techniques to determine the number of graphene layers, to probe resonance Raman spectra of monolayer and multilayer graphenes and to obtain Raman images of graphene-based materials are also presented. The extensive capabilities of Raman spectroscopy for the investigation of the fundamental properties of graphene under external perturbations are described, which have also been extended to other graphene-based materials, such as graphene quantum dots, carbon dots, graphene oxide, nanoribbons, chemical vapor deposition-grown and SiC epitaxially grown graphene flakes, composites, and graphene-based van der Waals heterostructures. These fundamental properties have been used to probe the states, effects, and mechanisms of graphene materials present in the related heterostructures and devices. We hope that this review will be beneficial in all the aspects of graphene investigations, from basic research to material synthesis and device applications.

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Raman spectroscopy of graphene-based materials and its applications in related devices.

Heat management has become more and more critical, especially in miniaturized modern devices, so the exploration of highly thermally conductive materials with electrical insulation is of great importance. Here, we report that high-quality one-atom-thin hexagonal boron nitride (BN) has a thermal conductivity (κ) of 751 W/mK at room temperature, the second largest κ per unit weight among all semiconductors and insulators. The κ of atomically thin BN decreases with increased thickness. Our molecular dynamic simulations accurately reproduce this trend, and the density functional theory (DFT) calculations reveal the main scattering mechanism. The thermal expansion coefficients of monolayer to trilayer BN at 300 to 400 K are also experimentally measured for the first time. Owing to its wide bandgap, high thermal conductivity, outstanding strength, good flexibility, and excellent thermal and chemical stability, atomically thin BN is a strong candidate for heat dissipation applications, especially in the next generation of flexible electronic devices.

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High thermal conductivity of high-quality monolayer boron nitride and its thermal expansion.

Graphene, in its ideal form, is a two-dimensional (2D) material consisting of a single layer of carbon atoms arranged in a hexagonal lattice. The richness in morphological, physical, mechanical, and optical properties of ideal graphene has stimulated enormous scientific and industrial interest, since its first exfoliation in 2004. In turn, the production of graphene in a reliable, controllable, and scalable manner has become significantly important to bring us closer to practical applications of graphene. To this end, chemical vapor deposition (CVD) offers tantalizing opportunities for the synthesis of large-area, uniform, and high-quality graphene films. However, quite different from the ideal 2D structure of graphene, in reality, the currently available CVD-grown graphene films are still suffering from intrinsic defective grain boundaries, surface contaminations, and wrinkles, together with low growth rate and the requirement of inevitable transfer. Clearly, a gap still exits between the reality of CVD-derived graphene, especially in industrial production, and ideal graphene with outstanding properties. This Review will emphasize the recent advances and strategies in CVD production of graphene for settling these issues to bridge the giant gap. We begin with brief background information about the synthesis of nanoscale carbon allotropes, followed by the discussion of fundamental growth mechanism and kinetics of CVD growth of graphene. We then discuss the strategies for perfecting the quality of CVD-derived graphene with regard to domain size, cleanness, flatness, growth rate, scalability, and direct growth of graphene on functional substrate. Finally, a perspective on future development in the research relevant to scalable growth of high-quality graphene is presented.

Bridging the Gap between Reality and Ideal in Chemical Vapor Deposition Growth of Graphene

The subject of thermal transport at the mesoscopic scale and in low-dimensional systems is interesting for both fundamental research and practical applications. As the first example of truly two-dimensional materials, graphene has exceptionally high thermal conductivity, and thus provides an ideal platform for the research. Here we review recent studies on thermal and thermoelectric properties of graphene, with an emphasis on experimental progresses. A general physical picture based on the Landauer transport formalism is introduced to understand underlying mechanisms. We show that the superior thermal conductivity of graphene is contributed not only by large ballistic thermal conductance but also by very long phonon mean free path (MFP). The long phonon MFP, explained by the low-dimensional nature and high sample purity of graphene, results in important isotope effects and size effects on thermal conduction. In terms of various scattering mechanisms in graphene, several approaches are suggested to control thermal conductivity. Among them, introducing rough boundaries and weakly-coupled interfaces are promising ways to suppress thermal conduction effectively. We also discuss the Seebeck effect of graphene. Graphene itself might not be a good thermoelectric material. However, the concepts developed by graphene research might be applied to improve thermoelectric performance of other materials.

Thermal and Thermoelectric Properties of Graphene

Wrinkling in Graphene Sheets and Graphene Oxide Papers

The thermal conductivity (κ) of suspended graphene membranes made by chemical vapor deposition (CVD) was measured by micro-Raman mapping. Cracks and wrinkles present in these suspended graphene membranes were identified by micro-Raman mapping, and κ values and their statistics were obtained on membranes free of such imperfections in a single mapping. Based on this new technique, an average κ value of 1875 ± 220 W m−1 K−1 at 420 K was measured on 26 suspended graphene membranes that were free of wrinkles, ~27% higher than the average value measured from 12 graphene membranes with wrinkles. These results suggest that the variation in published thermal conductivity values for suspended graphene samples could, at least in part, be due to the presence or absence of wrinkles.

https://iopscience.iop.org/article/10.1088/0957-4484/23/36/365701/pdf

Qimin Zhang

Papers

Thermal conductivity measurements of suspended graphene with and without wrinkles by micro-Raman mapping