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      Intralayer and interlayer electron–phonon interactions in twisted graphene heterostructures

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          Abstract

          The understanding of interactions between electrons and phonons in atomically thin heterostructures is crucial for the engineering of novel two-dimensional devices. Electron–phonon (el–ph) interactions in layered materials can occur involving electrons in the same layer or in different layers. Here we report on the possibility of distinguishing intralayer and interlayer el–ph interactions in samples of twisted bilayer graphene and of probing the intralayer process in graphene/h-BN by using Raman spectroscopy. In the intralayer process, the el–ph scattering occurs in a single graphene layer and the other layer (graphene or h-BN) imposes a periodic potential that backscatters the excited electron, whereas for the interlayer process the el–ph scattering occurs between states in the Dirac cones of adjacent graphene layers. Our methodology of using Raman spectroscopy to probe different types of el–ph interactions can be extended to study any kind of graphene-based heterostructure.

          Abstract

          Electron–phonon interactions in van der Waals layered materials can occur either within the same layer (intralayer) or in different layers (interlayer). Here, the authors use multi-wavelength Raman spectroscopy to probe intra- and inter-layer electron–phonon interactions in twisted graphene heterostructures.

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          Studying disorder in graphite-based systems by Raman spectroscopy.

          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 sp(2) 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 (E(laser)) and the in-plane size (L(a)) 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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            Angle-resolved Raman imaging of interlayer rotations and interactions in twisted bilayer graphene.

            Few-layer graphene is a prototypical layered material, whose properties are determined by the relative orientations and interactions between layers. Exciting electrical and optical phenomena have been observed for the special case of Bernal-stacked few-layer graphene, but structure-property correlations in graphene which deviates from this structure are not well understood. Here, we combine two direct imaging techniques, dark-field transmission electron microscopy (DF-TEM) and widefield Raman imaging, to establish a robust, one-to-one correlation between twist angle and Raman intensity in twisted bilayer graphene (tBLG). The Raman G band intensity is strongly enhanced due to a previously unreported singularity in the joint density of states of tBLG, whose energy is exclusively a function of twist angle and whose optical transition strength is governed by interlayer interactions, enabling direct optical imaging of these parameters. Furthermore, our findings suggest future potential for novel optical and optoelectronic tBLG devices with angle-dependent, tunable characteristics.
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              Graphene bilayer with a twist: electronic structure

              Electronic properties of bilayer and multilayer graphene have generally been interpreted in terms of AB or Bernal stacking. However, it is known that many types of stacking defects can occur in natural and synthetic graphite; rotation of the top layer is often seen in scanning tunneling microscopy (STM) studies of graphite. In this paper we consider a graphene bilayer with a relative small angle rotation between the layers and calculate the electronic structure near zero energy in a continuum approximation. Contrary to what happens in a AB stacked bilayer and in accord with observations in epitaxial graphene we find: (a) the low energy dispersion is linear, as in a single layer, but the Fermi velocity can be significantly smaller than the single layer value; (b) an external electric field, perpendicular to the layers, does not open an electronic gap
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                Author and article information

                Contributors
                mpimenta11@gmail.com
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                23 March 2018
                23 March 2018
                2018
                : 9
                : 1221
                Affiliations
                [1 ]ISNI 0000 0001 2181 4888, GRID grid.8430.f, Departamento de Física, Universidade Federal de Minas Gerais, , UFMG, ; Belo Horizonte, 30123-970 Brazil
                [2 ]ISNI 0000 0001 2294 473X, GRID grid.8536.8, Núcleo Multidisciplinar de Pesquisas em Computação - NUMPEX-COMP, Campus Duque de Caxias, , Universidade Federal do Rio de Janeiro, ; Duque de Caxias, 25245-390 RJ Brazil
                [3 ]ISNI 0000 0001 2184 6919, GRID grid.411173.1, Instituto de Física, Universidade Federal Fluminense, , UFF, ; Niterói, 24210-346 RJ Brazil
                [4 ]ISNI 0000 0001 2359 5252, GRID grid.412403.0, MackGraphe - Graphene and Nanomaterials Research Center, , Mackenzie Presbyterian University, ; São Paulo, 01302-907 Brazil
                [5 ]ISNI 0000 0004 0532 0580, GRID grid.38348.34, National Tsing Hua University, ; Hsinchu, 30013 Taiwan
                [6 ]ISNI 0000 0001 0789 6880, GRID grid.21941.3f, National Institute for Materials Science, ; 1-1 Namiki, Tsukuba, 305-0044 Japan
                [7 ]ISNI 0000 0001 2353 1689, GRID grid.11417.32, CEMES/CNRS, , University of Toulouse, ; 31055 Toulouse, France
                [8 ]ISNI 0000 0001 2097 0141, GRID grid.121334.6, Laboratoire Charles Coulomb, CNRS, , University of Montpellier, ; Montpellier, 34095 France
                Author information
                http://orcid.org/0000-0003-4909-0310
                Article
                3479
                10.1038/s41467-018-03479-3
                5865138
                29572537
                63f4103c-8721-47e0-a5f0-e4a8eacc27b8
                © The Author(s) 2018

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 18 October 2017
                : 16 February 2018
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