Raman spectroscopy of graphene and graphite: Disorder, electron phonon coupling, doping and nonadiabatic effects

Raman spectroscopy is an integral part of graphene research. It is used to determine the number and orientation of layers, the quality and types of edge, and the effects of perturbations, such as electric and magnetic fields, strain, doping, disorder and functional groups. This, in turn, provides insight into all sp(2)-bonded carbon allotropes, because graphene is their fundamental building block. Here we review the state of the art, future directions and open questions in Raman spectroscopy of graphene. We describe essential physical processes whose importance has only recently been recognized, such as the various types of resonance at play, and the role of quantum interference. We update all basic concepts and notations, and propose a terminology that is able to describe any result in literature. We finally highlight the potential of Raman spectroscopy for layered materials other than graphene.

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Raman spectroscopy as a versatile tool for studying the properties of graphene

Diamond-like carbon (DLC) is a metastable form of amorphous carbon with significant sp3 bonding. DLC is a semiconductor with a high mechanical hardness, chemical inertness, and optical transparency. This review will describe the deposition methods, deposition mechanisms, characterisation methods, electronic structure, gap states, defects, doping, luminescence, field emission, mechanical properties and some applications of DLCs. The films have widespread applications as protective coatings in areas, such as magnetic storage disks, optical windows and micro-electromechanical devices (MEMs).

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Diamond-like amorphous carbon

Raman spectroscopy has historically played an important role in the structural characterization of graphitic materials, in particular providing valuable information about defects, stacking of the graphene layers and the finite sizes of the crystallites parallel and perpendicular to the hexagonal axis Here we review the defect-induced Raman spectra of graphitic materials from both experimental and theoretical standpoints and we present recent Raman results on nanographites and graphenes The disorder-induced D and D′ Raman features, as well as the G′-band (the overtone of the D-band which is always observed in defect-free samples), are discussed in terms of the double-resonance (DR) Raman process, involving phonons within the interior of the 1st Brillouin zone of graphite and defects In this review, experimental results for the D, D′ and G′ bands obtained with different laser lines, and in samples with different crystallite sizes and different types of defects are presented and discussed We also present recent advances that made possible the development of Raman scattering as a tool for very accurate structural analysis of nano-graphite, with the establishment of an empirical formula for the in- and out-of-plane crystalline size and even fancier Raman-based information, such as for the atomic structure at graphite edges, and the identification of single versus multi-graphene layers Once established, this knowledge provides a powerful machinery to understand newer forms of sp2 carbon materials, such as the recently developed pitch-based graphitic foams Results for the calculated Raman intensity of the disorder-induced D-band in graphitic materials as a function of both the excitation laser energy (Elaser) and the in-plane size (La) of nano-graphites are presented and compared with experimental results The status of this research area is assessed, and opportunities for future work are identified

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Studying Disorder in Graphite-Based Systems by Raman Spectroscopy

Chemically derived graphene oxide (GO) is an atomically thin sheet of graphite that has traditionally served as a precursor for graphene, but is increasingly attracting chemists for its own characteristics. It is covalently decorated with oxygen-containing functional groups - either on the basal plane or at the edges - so that it contains a mixture of sp(2)- and sp(3)-hybridized carbon atoms. In particular, manipulation of the size, shape and relative fraction of the sp(2)-hybridized domains of GO by reduction chemistry provides opportunities for tailoring its optoelectronic properties. For example, as-synthesized GO is insulating but controlled deoxidation leads to an electrically and optically active material that is transparent and conducting. Furthermore, in contrast to pure graphene, GO is fluorescent over a broad range of wavelengths, owing to its heterogeneous electronic structure. In this Review, we highlight the recent advances in optical properties of chemically derived GO, as well as new physical and biological applications.

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Graphene oxide as a chemically tunable platform for optical applications

We have studied the D peak in the Raman spectrum of polycrystalline graphite as a function of excitation energy in the range from 1.16 to 4.3 eV. The D peak disperses with excitation energy (≈50 cm−1/eV) and its intensity decreases with increasing laser energy. The dispersion of the D peak is explained in terms of a novel k → -selective resonant Raman scattering process. The scattering cross-section is resonantly enhanced for phonons on one branch in the phonon dispersion curves which have the same k → -vector as the electronic transition responsible for the resonance.

István Pócsik

Papers

Origin of the D peak in the Raman spectrum of microcrystalline graphite

Surface enhanced Raman scattering (SERS) investigation of amorphous carbon

Characterisation of a-C:H and oxygen-containing Si:C:H films by Raman spectroscopy and XPS

IR study of the formation process of polymeric hydrogenated amorphous carbon film

The state of water in normal and senile cataractous lenses studied by nuclear magnetic resonance.