Single-Layer Behavior and Its Breakdown in Twisted Graphene Layers
TL;DR: In this paper, high magnetic field scanning tunneling microscopy and Landau level spectroscopy of twisted graphene layers grown by chemical vapor deposition was performed. But the results were limited to the case of twisted bilayer bilayer graphene.
Abstract: We report high magnetic field scanning tunneling microscopy and Landau level spectroscopy of twisted graphene layers grown by chemical vapor deposition. For twist angles exceeding ~3° the low energy carriers exhibit Landau level spectra characteristic of massless Dirac fermions. Above 20° the layers effectively decouple and the electronic properties are indistinguishable from those in single-layer graphene, while for smaller angles we observe a slowdown of the carrier velocity which is strongly angle dependent. At the smallest angles the spectra are dominated by twist-induced van Hove singularities and the Dirac fermions eventually become localized. An unexpected electron-hole asymmetry is observed which is substantially larger than the asymmetry in either single or untwisted bilayer graphene.
Citations
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University of Cambridge1, Istituto Italiano di Tecnologia2, Lancaster University3, University of Manchester4, Catalan Institution for Research and Advanced Studies5, Technical University of Denmark6, Nokia7, Queen Mary University of London8, University of Trento9, fondazione bruno kessler10, Technische Universität München11, Polytechnic University of Milan12, Centre national de la recherche scientifique13, University of Trieste14, University of Ioannina15, University of Geneva16, Trinity College, Dublin17, Texas Instruments18, University of Paris19, Spanish National Research Council20, Leiden University21, Delft University of Technology22, University of Patras23, École Normale Supérieure24, Radboud University Nijmegen25, Nest Labs26, Airbus UK27, Seoul National University28, Yonsei University29, University of Oxford30, Chalmers University of Technology31, University of Groningen32, STMicroelectronics33, Chemnitz University of Technology34, Max Planck Society35, Aalto University36
TL;DR: An overview of the key aspects of graphene and related materials, ranging from fundamental research challenges to a variety of applications in a large number of sectors, highlighting the steps necessary to take GRMs from a state of raw potential to a point where they might revolutionize multiple industries are provided.
Abstract: We present the science and technology roadmap for graphene, related two-dimensional crystals, and hybrid systems, targeting an evolution in technology, that might lead to impacts and benefits reaching into most areas of society. This roadmap was developed within the framework of the European Graphene Flagship and outlines the main targets and research areas as best understood at the start of this ambitious project. We provide an overview of the key aspects of graphene and related materials (GRMs), ranging from fundamental research challenges to a variety of applications in a large number of sectors, highlighting the steps necessary to take GRMs from a state of raw potential to a point where they might revolutionize multiple industries. We also define an extensive list of acronyms in an effort to standardize the nomenclature in this emerging field.
2,560 citations
Journal Article•
TL;DR: In this article, the effects of the twist angle between different layers in a van der Waals heterostructure have been investigated and it was shown that when this angle is close to the magic angle, the electronic band structure near zero Fermi energy becomes flat, owing to strong interlayer coupling.
Abstract: A van der Waals heterostructure is a type of metamaterial that consists of vertically stacked two-dimensional building blocks held together by the van der Waals forces between the layers. This design means that the properties of van der Waals heterostructures can be engineered precisely, even more so than those of two-dimensional materials. One such property is the 'twist' angle between different layers in the heterostructure. This angle has a crucial role in the electronic properties of van der Waals heterostructures, but does not have a direct analogue in other types of heterostructure, such as semiconductors grown using molecular beam epitaxy. For small twist angles, the moire pattern that is produced by the lattice misorientation between the two-dimensional layers creates long-range modulation of the stacking order. So far, studies of the effects of the twist angle in van der Waals heterostructures have concentrated mostly on heterostructures consisting of monolayer graphene on top of hexagonal boron nitride, which exhibit relatively weak interlayer interaction owing to the large bandgap in hexagonal boron nitride. Here we study a heterostructure consisting of bilayer graphene, in which the two graphene layers are twisted relative to each other by a certain angle. We show experimentally that, as predicted theoretically, when this angle is close to the 'magic' angle the electronic band structure near zero Fermi energy becomes flat, owing to strong interlayer coupling. These flat bands exhibit insulating states at half-filling, which are not expected in the absence of correlations between electrons. We show that these correlated states at half-filling are consistent with Mott-like insulator states, which can arise from electrons being localized in the superlattice that is induced by the moire pattern. These properties of magic-angle-twisted bilayer graphene heterostructures suggest that these materials could be used to study other exotic many-body quantum phases in two dimensions in the absence of a magnetic field. The accessibility of the flat bands through electrical tunability and the bandwidth tunability through the twist angle could pave the way towards more exotic correlated systems, such as unconventional superconductors and quantum spin liquids.
1,961 citations
TL;DR: In this paper, the authors review the recent progress and challenges of 2D van der Waals interactions and offer a perspective on the exploration of 2DLM-based vdWHs for future application in electronics and optoelectronics.
Abstract: Two-dimensional layered materials (2DLMs) have been a central focus of materials research since the discovery of graphene just over a decade ago. Each layer in 2DLMs consists of a covalently bonded, dangling-bond-free lattice and is weakly bound to neighbouring layers by van der Waals interactions. This makes it feasible to isolate, mix and match highly disparate atomic layers to create a wide range of van der Waals heterostructures (vdWHs) without the constraints of lattice matching and processing compatibility. Exploiting the novel properties in these vdWHs with diverse layering of metals, semiconductors or insulators, new designs of electronic devices emerge, including tunnelling transistors, barristors and flexible electronics, as well as optoelectronic devices, including photodetectors, photovoltaics and light-emitting devices with unprecedented characteristics or unique functionalities. We review the recent progress and challenges, and offer our perspective on the exploration of 2DLM-based vdWHs for future application in electronics and optoelectronics. With a dangling-bond-free surface, two dimensional layered materials (2DLMs) can enable the creation of diverse van der Waals heterostructures (vdWHs) without the conventional constraint of lattice matching or process compatibility. This Review discusses the recent advances in exploring 2DLM vdWHs for future electronics and optoelectronics.
1,850 citations
TL;DR: The essential Raman scattering processes of the entire first- and second-order modes in intrinsic graphene are described and the extensive capabilities of Raman spectroscopy for the investigation of the fundamental properties of graphene under external perturbations are described.
Abstract: 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.
1,184 citations
TL;DR: Graphene is at the center of an ever growing research effort due to its unique properties, interesting for both fundamental science and applications as mentioned in this paper, and a key requirement for applications is the development of industrial-scale, reliable, inexpensive production processes.
968 citations
References
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TL;DR: It is shown experimentally that when this angle is close to the ‘magic’ angle the electronic band structure near zero Fermi energy becomes flat, owing to strong interlayer coupling, and these flat bands exhibit insulating states at half-filling, which are not expected in the absence of correlations between electrons.
Abstract: A van der Waals heterostructure is a type of metamaterial that consists of vertically stacked two-dimensional building blocks held together by the van der Waals forces between the layers. This design means that the properties of van der Waals heterostructures can be engineered precisely, even more so than those of two-dimensional materials. One such property is the 'twist' angle between different layers in the heterostructure. This angle has a crucial role in the electronic properties of van der Waals heterostructures, but does not have a direct analogue in other types of heterostructure, such as semiconductors grown using molecular beam epitaxy. For small twist angles, the moire pattern that is produced by the lattice misorientation between the two-dimensional layers creates long-range modulation of the stacking order. So far, studies of the effects of the twist angle in van der Waals heterostructures have concentrated mostly on heterostructures consisting of monolayer graphene on top of hexagonal boron nitride, which exhibit relatively weak interlayer interaction owing to the large bandgap in hexagonal boron nitride. Here we study a heterostructure consisting of bilayer graphene, in which the two graphene layers are twisted relative to each other by a certain angle. We show experimentally that, as predicted theoretically, when this angle is close to the 'magic' angle the electronic band structure near zero Fermi energy becomes flat, owing to strong interlayer coupling. These flat bands exhibit insulating states at half-filling, which are not expected in the absence of correlations between electrons. We show that these correlated states at half-filling are consistent with Mott-like insulator states, which can arise from electrons being localized in the superlattice that is induced by the moire pattern. These properties of magic-angle-twisted bilayer graphene heterostructures suggest that these materials could be used to study other exotic many-body quantum phases in two dimensions in the absence of a magnetic field. The accessibility of the flat bands through electrical tunability and the bandwidth tunability through the twist angle could pave the way towards more exotic correlated systems, such as unconventional superconductors and quantum spin liquids.
3,005 citations
University of Cambridge1, Istituto Italiano di Tecnologia2, Lancaster University3, University of Manchester4, Catalan Institution for Research and Advanced Studies5, Technical University of Denmark6, Nokia7, Queen Mary University of London8, University of Trento9, fondazione bruno kessler10, Technische Universität München11, Polytechnic University of Milan12, Centre national de la recherche scientifique13, University of Trieste14, University of Ioannina15, University of Geneva16, Trinity College, Dublin17, Texas Instruments18, University of Paris19, Spanish National Research Council20, Leiden University21, Delft University of Technology22, University of Patras23, École Normale Supérieure24, Radboud University Nijmegen25, Nest Labs26, Airbus UK27, Seoul National University28, Yonsei University29, University of Oxford30, Chalmers University of Technology31, University of Groningen32, STMicroelectronics33, Chemnitz University of Technology34, Max Planck Society35, Aalto University36
TL;DR: An overview of the key aspects of graphene and related materials, ranging from fundamental research challenges to a variety of applications in a large number of sectors, highlighting the steps necessary to take GRMs from a state of raw potential to a point where they might revolutionize multiple industries are provided.
Abstract: We present the science and technology roadmap for graphene, related two-dimensional crystals, and hybrid systems, targeting an evolution in technology, that might lead to impacts and benefits reaching into most areas of society. This roadmap was developed within the framework of the European Graphene Flagship and outlines the main targets and research areas as best understood at the start of this ambitious project. We provide an overview of the key aspects of graphene and related materials (GRMs), ranging from fundamental research challenges to a variety of applications in a large number of sectors, highlighting the steps necessary to take GRMs from a state of raw potential to a point where they might revolutionize multiple industries. We also define an extensive list of acronyms in an effort to standardize the nomenclature in this emerging field.
2,560 citations
TL;DR: In this paper, the authors review the recent progress and challenges of 2D van der Waals interactions and offer a perspective on the exploration of 2DLM-based vdWHs for future application in electronics and optoelectronics.
Abstract: Two-dimensional layered materials (2DLMs) have been a central focus of materials research since the discovery of graphene just over a decade ago. Each layer in 2DLMs consists of a covalently bonded, dangling-bond-free lattice and is weakly bound to neighbouring layers by van der Waals interactions. This makes it feasible to isolate, mix and match highly disparate atomic layers to create a wide range of van der Waals heterostructures (vdWHs) without the constraints of lattice matching and processing compatibility. Exploiting the novel properties in these vdWHs with diverse layering of metals, semiconductors or insulators, new designs of electronic devices emerge, including tunnelling transistors, barristors and flexible electronics, as well as optoelectronic devices, including photodetectors, photovoltaics and light-emitting devices with unprecedented characteristics or unique functionalities. We review the recent progress and challenges, and offer our perspective on the exploration of 2DLM-based vdWHs for future application in electronics and optoelectronics. With a dangling-bond-free surface, two dimensional layered materials (2DLMs) can enable the creation of diverse van der Waals heterostructures (vdWHs) without the conventional constraint of lattice matching or process compatibility. This Review discusses the recent advances in exploring 2DLM vdWHs for future electronics and optoelectronics.
1,850 citations
TL;DR: The essential Raman scattering processes of the entire first- and second-order modes in intrinsic graphene are described and the extensive capabilities of Raman spectroscopy for the investigation of the fundamental properties of graphene under external perturbations are described.
Abstract: 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.
1,184 citations
TL;DR: Graphene is at the center of an ever growing research effort due to its unique properties, interesting for both fundamental science and applications as mentioned in this paper, and a key requirement for applications is the development of industrial-scale, reliable, inexpensive production processes.
968 citations