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Register a new userRaman-scattering study of the phonon dispersion in twisted bi-layer graphene
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Added by
Luiz Gustavo Cancado
Publication date
2013
fields
Physics
and research's language is
English
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Bi-layer graphene with a twist angle theta between the layers generates a superlattice structure known as Moir{e} pattern. This superlattice provides a theta-dependent q wavevector that activates phonons in the interior of the Brillouin zone. Here we show that this superlattice-induced Raman scattering can be used to probe the phonon dispersion in twisted bi-layer graphene (tBLG). The effect reported here is different from the broadly studied double-resonance in graphene-related materials in many aspects, and despite the absence of stacking order in tBLG, layer breathing vibrations (namely ZO phonons) are observed.
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Twisted bi-layer graphene (tBLG) has recently attracted interest due to the peculiar electrical properties that arise from its random rotational configurations. Our experiments on CVD-grown graphene from Cu foil and transferred onto Si substrates, with an oxide layer of 100 nm, reveal naturally-produced bi-layer graphene patches which present different colorations when shined with white light. In particular yellow-, pink- and blue- colored areas are evidenced. Combining optical microscopy, Raman spectroscopy and transmission electron microscopy we have been able to assign these colorations to ranges of rotational angles between the two graphene layers. Optical contrast simulations have been carried out, proving that the observation of the different colorations is due to the angle-dependent electronic properties of tBLG combined with the reflection that results from the layered structure tBLG / 100 nm-thick SiO2 / Si. Our results could lead the way to an easy selective identification of bi-layer graphene merely through the observation on an optical microscope.
The results of micro-Raman scattering measurements performed on three different ``graphitic materials: micro-structured disks of highly oriented pyrolytic graphite, graphene multi-layers thermally decomposed from carbon terminated surface of 4H-SiC and an exfoliated graphene monolayer are presented. Despite its multi-layer character, most parts of the surface of the graphitized SiC substrates shows a single-component, Lorentzian shape, double resonance Raman feature in striking similarity to the case of a single graphene monolayer. Our observation suggests a very weak electronic coupling between graphitic layers on the SiC surface, which therefore can be considered to be graphene multi-layers with a simple (Dirac-like) band structure.
We study electronic contribution to the Raman scattering signals of two-, three- and four-layer graphene with layers at one of the interfaces twisted by a small angle with respect to each other. We find that the Raman spectra of these systems feature two peaks produced by van Hove singularities in moir{e} minibands of twistronic graphene, one related to direct hybridization of Dirac states, and the other resulting from band folding caused by moir{e} superlattice. The positions of both peaks strongly depend on the twist angle, so that their detection can be used for non-invasive characterization of the twist, even in hBN-encapsulated structures.
The band structure of bilayer graphene is tunable by introducing a relative twist angle between the two layers, unlocking exotic phases, such as superconductor and Mott insulator, and providing a fertile ground for new physics. At intermediate twist angles around 10{deg}, highly degenerate electronic transitions hybridize to form excitonic states, a quite unusual phenomenon in a metallic system. We probe the bright exciton mode using resonant Raman scattering measurements to track the evolution of the intensity of the graphene Raman G peak, corresponding to the E2g phonon. By cryogenically cooling the sample, we are able to resolve both the incoming and outgoing resonance in the G peak intensity evolution as a function of excitation energy, a prominent manifestation of the bright exciton serving as the intermediate state in the Raman process. For a sample with twist angle 8.6{deg}, we report a weakly temperature dependent resonance broadening ${gamma}$ ${approx}$ 0.07 eV. In the limit of small inhomogeneous broadening, the observed ${gamma}$ places a lower bound for the bright exciton scattering lifetime at 10 fs in the presence of charges and excitons excited by the light pulse for Raman measurement, limited by the rapid exciton-exciton and exciton-charge scattering in graphene.
Magneto-Raman scattering experiments from the surface of graphite reveal novel features associated to purely electronic excitations which are observed in addition to phonon-mediated resonances. Graphene-like and graphite domains are identified through experiments with $sim 1mu m$ spatial resolution performed in magnetic fields up to 32T. Polarization resolved measurements emphasize the characteristic selection rules for electronic transitions in graphene. Graphene on graphite displays the unexpected hybridization between optical phonon and symmetric across the Dirac point inter Landau level transitions. The results open new experimental possibilities - to use light scattering methods in studies of graphene under quantum Hall effect conditions.
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