We study the effect of atomic relaxation on the structure of moiré patterns in twisted graphene on graphite and double layer graphene by large scale atomistic simulations. The reconstructed structure can be described as a superlattice of `hot spots' with vortex-like behaviour of in-plane atomic displacements and increasing out-of-plane displacements with decreasing angle. These lattice distortions affect both scalar and vector potential and the resulting electronic properties. At low misorientation angles (<$\sim$1$^\circ$) the optimized structures deviate drastically from the sinusoidal modulation which is often assumed in calculations of the electronic properties. The proposed structure might be verified by scanning probe microscopy measurements.
We report that the twisted few layer graphite (tFL-graphite) is a new family of moiré heterostructures (MHSs), which has richer and highly tunable moiré flat band structures entirely distinct from all the known MHSs. A tFL-graphite is composed of two few-layer graphite (Bernal stacked multilayer graphene), which are stacked on each other with a small twisted angle. The moiré band structure of the tFL-graphite strongly depends on the layer number of its composed two van der Waals layers. Near the magic angle, a tFL-graphite always has two nearly flat bands coexisting with a few pairs of narrowe…
We address the origin of bead-like edge states observed by scanning tunneling microscopy (STM) in moiré patterns of graphite. Low-bias scanning tunneling spectroscopy measurements indicate these edge states are centered around AB stacking sites, contrarily to the common assumption of them being at AA sites. This shift of the intensity of the beads with respect to the bulk moiré pattern has been corroborated by a tight-binding calculation of the edge states in bilayer nanoribbons. Our results are valid not only for graphite but also for few-layer graphene, where these states have also been rece…
We have observed with STM moiré patterns corresponding to the rotation of one graphene layer on HOPG surface. The moiré patterns were characterized by rotation angle and extension in the plane. Additionally, by identifying border domains and defects we can discriminate between moiré patterns due to rotation on the surface or subsurface layer. For a better understanding of moiré patterns formation we have studied by first principles an array of three graphene layers where the top or the middle layer appears rotated around the stacking axis. We compare the experimental and theoretical results an…
Moiré patterns on Highly Oriented Pyrolytic Graphite surfaces due to dislocated graphene layers were studied. We observed that the apparent corrugations of the moiré patterns in scanning tunnelling microscopy images change as a function of tunnel junction bias. A simple geometric investigation of the atomic structure of the graphene layers generating moiré patterns revealed that different atomic arrangements due to different twist angles can result in similar geometric moiré periods such that, only a small fraction of the observed moiré periodicities may coincide with the real atomic periodici…
The direct experimental probing of locally varying lattice parameters and anisotropic lattice deformations in atomic multilayers is extremely challenging. Here, we develop a new combined numerical/graphical method for the analysis of irregular moiré superstructures measured by scanning tunneling microscopy (STM) on a small-twist-angle ($\sim$0.6$^{\circ}$) graphene on highly oriented pyrolytic graphite (gr/HOPG). We observe distorted moiré patterns with a spatially varying period in annealed gr/HOPG. The nanoscale modulation of the moiré period observed by STM reflects a locally strained (and …
We study the electronic structure of a double-twisted few layer graphite (DTFLG), which consists of three few layer graphite (FLG), i.e. ABA-stacked graphene multilayer, stacked with two twist angles. We consider two categories of DTFLG, alternately twisted case and chirally twisted one, according to the rotation direction of the two twist angles. We show that, once the middle FLG of DTFLG is not thinner than trilayer, both kinds of DTFLG can remarkably host two pairs of degenerate moiré flat bands (MFBs) at $E_f$, twice that of the magic angle twisted bilayer graphene (TBG). The doubled MFBs …
Resonant interlayer coupling in NbSe$_2$-graphite epitaxial moir{é} superlattices
SUPA, School of Physics and Astronomy, University of St Andrews（圣安德鲁斯大学物理与天文学学院）；Department of Physics and Astronomy, University of Manchester（曼彻斯特大学物理与天文学系）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Physics Study Program, Faculty of Science and Technology, Syarif Hidayatullah State Islamic University Jakarta（雅加达希达亚图拉伊斯兰国立大学科技理学院物理学专业）；Institute for Materials Research, Tohoku University（东北大学材料科学研究所）
We consider the role of deformations in graphene heterostructures with hexagonal crystals (including strain, wrinkles and dislocations) on the geometrical properties of moire patterns characteristic for a pair of two incommensurate misaligned isostructural crystals. By, employing a phenomenological theory to describe generic moire perturbation in van der Waals heterostructures of graphene and hexagonal crystals we investigate the electronic properties of such heterostructure.
Negative friction coefficients, where friction is reduced upon increasing normal load, are predicted for superlubric graphite-hexagonal boron nitride heterojunctions. The origin of this counterintuitive behavior lies in the load-induced suppression of the moiré superstructure out-of-plane distortions leading to a less dissipative interfacial dynamics. Thermally induced enhancement of the out-of-plane fluctuations leads to an unusual increase of friction with temperature. The highlighted frictional mechanism is of a general nature and is expected to appear in many layered material heterojunctio…
A periodic spatial modulation, as created by a moiré pattern, has been extensively studied with the view to engineer and tune the properties of graphene. Graphene encapsulated by hexagonal boron nitride (hBN) when slightly misaligned with the top and bottom hBN layers experiences two interfering moiré patterns, resulting in a so-called super-moiré (SM). This leads to a lattice and electronic spectrum reconstruction. A geometrical construction of the non-relaxed SM patterns allows us to indicate qualitatively the induced changes in the electronic properties and to locate the SM features in the …
We use a hybrid k dot p theory - tight binding (HkpTB) model to describe interlayer coupling simultaneously in both Bernal and twisted graphene structures. For Bernal-aligned interfaces, HkpTB is parametrized using the full Slonczewski-Weiss-McClure (SWMcC) Hamiltonian of graphite, which is then used to refine the commonly used minimal model for twisted interfaces, by deriving additional terms that reflect all details of the full SWMcC model of graphite. We find that these terms introduce some electron-hole asymmetry in the band structure of twisted bilayers, but in twistronic multilayer graph…
Atomic modulations of two-dimensional materials using scanning tunneling microscope (STM) tip-induced forces modifies their mechanical and electrical properties. In situ topographic and spectroscopic probing through electrical tunneling has been used for straining sheets of graphite, monolayer graphene and NbSe2. The findings also resolve a thirty-five-year-old controversy involving numerous proposed models to explain the source of anomalously high measured atomic amplitudes (of up to 24 Angstroms, expected 0.2 Angstroms) from atomic corrugation on graphite surfaces. Our findings attributes th…
Two-dimensional heterostructures with layers of slightly different lattice vectors exhibit a new periodic structure known as moire lattices. Moire lattice formation provides a powerful new way to engineer the electronic structure of two-dimensional materials for realizing novel correlated and topological phenomena. In addition, superstructures of moire lattices can emerge from multiple misaligned lattice vectors or inhomogeneous strain distribution, which offers an extra degree of freedom in the electronic band structure design. High-resolution imaging of the moire lattices and superstructures…
This article reviews progress in the theoretical modelling of the electronic structure of rotationally faulted multilayer graphenes. In these systems the crystallographic axes of neighboring layers are misaligned so that the layer stacking does not occur in the Bernal structure observed in three dimensional graphite and frequently found in exfoliated bilayer graphene. Notably, rotationally faulted graphenes are commonly found in other forms of multilayer graphene including epitaxial graphenes thermally grown on ${\rm SiC \, (000 \bar 1)}$, graphenes grown by chemical vapor deposition, folded m…
Moiré-superlattices are ubiquitous in 2D heterostructures, strongly influencing their electronic properties. They give rise to new Dirac cones and are also at the origin of the superconductivity observed in magic-angle bilayer graphene. The modulation amplitude (corrugation) is an important yet largely unexplored parameter in defining the properties of 2D superlattices. The generally accepted view is that the corrugation monotonically decreases with increasing twist angle, while its effects on the electronic structure diminish as the layers become progressively decoupled. Here we found by latt…
Van der Waals (vdW) heterostructures ---formed by stacking or growing two-dimensional (2D) crystals on top of each other--- have emerged as a new promising route to tailor and engineer the properties of 2D materials. Twisted bilayer graphene (tBLG), a simple vdW structure where the interference between two misaligned graphene lattices leads to the formation of a moiré pattern, is a test bed to study the effects of the interaction and misalignment between layers, key players for determining the electronic properties of these stackings. In this chapter, we present in a pedagogical way the genera…
Graphene, a thinnest material in the world, can form moire structures on different substrates, including graphite, h-BN, or metal surfaces. In such systems the structure of graphene, i. e. its corrugation, as well as its electronic and elastic properties are defined by the combination of the system geometry and local interaction strength at the interface. The corrugation in such structures on metals is heavily extracted from diffraction or local probe microscopy experiments and can be obtained only via comparison with theoretical data, which usually simulate the experimental findings. Here we …
When two-dimensional van der Waals materials are stacked to build heterostructures, moiré patterns emerge from twisted interfaces or from mismatch in lattice constant of individual layers. Relaxation of the atomic positions is a direct, generic consequence of the moiré pattern, with many implications for the physical properties. Moiré driven atomic relaxation may be naively thought to be restricted to the interfacial layers and thus irrelevant for multi-layered heterostructures. However, we provide experimental evidence for the importance of the three dimensional nature of the relaxation in tw…
Despite the structures and properties of tilt grain boundaries of graphite surface and graphene have been extensively studied, their effect on the structures and electronic spectra of graphene layers has not been fully addressed. Here we study effects of one-dimensional tilt grain boundaries on structures and electronic spectra of graphene multilayers by scanning tunneling microscopy and spectroscopy. A tilt grain boundary of a top graphene sheet in graphene multilayers leads to a twist between consecutive layers and generates superstructures (Moiré patterns) on one side of the boundary. Our r…
We study the electron-phonon coupling in twisted bilayer graphene (TBG), which was recently experimentally observed to exhibit superconductivity around the magic twist angle $θ\approx 1.05^\circ$. We show that phonon-mediated electron electron attraction at the magic angle is strong enough to induce a conventional intervalley pairing between graphene valleys $K$ and $K'$ with a superconducting critical temperature $T_c\sim1K$, in agreement with the experiment. We predict that superconductivity can also be observed in TBG at many other angles $θ$ and higher electron densities in higher Moiré ba…
We introduce a theoretical framework for the new concept of three-dimensional (3D) twistronics by developing a generalized Bloch band theory for 3D layered systems with a constant twist angle $θ$ between successive layers. Our theory employs a nonsymmorphic symmetry that enables a precise definition of an effective out-of-plane crystal momentum, and also captures the in-plane moiré pattern formed between neighboring twisted layers. To demonstrate the novel topological physics that can be achieved through 3D twistronics, we present two examples. In the first example of chiral twisted graphite, …
When layers of graphene are rotationally misaligned by the magic angle, the moiré superlattice features extremely flat bands. Due to the enhanced density of states, the Coulomb interaction induces a variety of instabilities. The most prominent occur at integer filling and are therefore commonly attributed to spontaneous polarization of the moiré unit cell's `flavor' degrees of freedom -- spin, valley, and the flat-band degeneracy. As the dominant member of the hierarchy, these correlated states are thought to crucially determine further instabilities at lower energy scales, such as superconduc…
Ferromagnetism is most common in transition metal compounds but may also arise in low-density two-dimensional electron systems, with signatures observed in silicon, III-V semiconductor systems, and graphene moiré heterostructures. Here we show that gate-tuned van Hove singularities in rhombohedral trilayer graphene drive the spontaneous ferromagnetic polarization of the electron system into one or more spin- and valley flavors. Using capacitance measurements on graphite-gated van der Waals heterostructures, we find a cascade of density- and electronic displacement field tuned phase transitions…
We present atomistic calculations on structural and electronic properties of twisted double bilayer graphene (TDBG) consisting of two sets of rotationally misaligned Bernal-stacked bilayer graphene. Obtained equilibrium atomic structures exhibit in-plane strains and the modulation of the interlayer distances at the rotationally mismatched interface layers. We find that the electronic structure of TDBG can have an intrinsic band gap at the charge neutral point for a large range of the twist angle theta. Near theta = 1.25 degree, the intrinsic band gap disappears and TDBG hosts flat bands at the…
We have used scanning tunneling microscopy and spectroscopy to resolve the spatial variation of the density of states of twisted graphene layers on top of a highly oriented pyrolytic graphite substrate. Owing to the twist a moire pattern develops with a periodicity that is substantially larger than the periodicity of a single layer graphene. The twisted graphene layer has electronic properties that are distinctly different from that of a single layer graphene due to the nonzero interlayer coupling. For small twist angles (about 1-3.5 degree) the integrated differential conductivity spectrum ex…
Graphene nanoribbons (GNRs) with widths of a few nanometres are promising candidates for future nano-electronic applications due to their structurally tunable bandgaps, ultrahigh carrier mobilities, and exceptional stability. However, the direct growth of micrometre-long GNRs on insulating substrates, which is essential for the fabrication of nano-electronic devices, remains an immense challenge. Here, we report the epitaxial growth of GNRs on an insulating hexagonal boron nitride (h-BN) substrate through nanoparticle-catalysed chemical vapor deposition (CVD). Ultra-narrow GNRs with lengths of…
We study the stability and electronic structure of magic-angle twisted bilayer graphene on the hexagonal boron nitride (TBG/BN). Full relaxation has been performed for commensurate supercells of the heterostructures with different twist angles ($θ'$) and stackings between TBG and BN. We find that the slightly misaligned configuration with $θ' = 0.54^\circ$ and the AA/AA stacking has the globally lowest total energy due to the constructive interference of the moiré interlayer potentials and thus the greatly enhanced relaxation in its $1 \times 1$ commensurate supercell. Gaps are opened at the F…
