We report a systematic study of the optical conductivity of twisted bilayer graphene (tBLG) across a large energy range (1.2 eV to 5.6 eV) for various twist angles, combined with first-principles calculations. At previously unexplored high energies, our data show signatures of multiple van Hove singularities (vHSs) in the tBLG bands, as well as the nonlinearity of the single layer graphene bands and their electron-hole asymmetry. Our data also suggest that excitonic effects play a vital role in the optical spectra of tBLG. Including electron-hole interactions in first-principles calculations is essential to reproduce the shape of the conductivity spectra, and we find evidence of coherent interactions between the states associated with the multiple vHSs in tBLG.
We consider the electronic structure of a slightly twisted graphene bilayer and show the coexistence of van Hove singularities (VHSs) and superlattice Dirac points in a continuum approximation. The graphene-on-graphene moiré pattern gives rise to a periodic electronic potential, which leads to the emergence of the superlattice Dirac points due to the chiral nature of the charge carriers. Owning to the distinguishing real and reciprocal structures, the sublattice exchange even and odd structures of the twisted graphene bilayer (the two types of commensurate structures) result in two different s…
We consider the excitonic effects on the thermal properties in the AB-stacked bilayer graphene. The calculations are based on the bilayer generalization of the usual Hubbard model at the half-filling. The full interaction bandwidth is used without any low-energy assumption. We obtain the unusually high values for the electronic figure of merit even at the room-temperatures which is very promising for the thermoelectric applications of the AB-bilayer structure. We discuss the effects of the interlayer Coulomb interaction and temperature on different thermal parameters in the bilayer graphene an…
Recent experiments on kagome metals AV$_3$Sb$_5$ (A=K,Rb,Cs) [M. Kang et al., Nat. Phys. 18, 301-308 (2022)] identify twofold van Hove singularities (TvHS) with opposite concavity near the Fermi energy, generating two approximately hexagonal Fermi surfaces -- one electron-like and the other hole-like. Here we propose that a TvHS generates a novel time-reversal symmetry breaking excitonic order -- arising due to bound pairs of electrons and holes located at opposite concavity van Hove singularities. We introduce a minimal model for the TvHS and investigate interaction induced many-body instabil…
Magnetic impurity adsorbed on one of the carbon planes of a bilayer graphene is studied. The formation of the many-body SU(2) and SU(4) resonances close to the bandgap is analyzed within the mean field Kotliar-Ruckenstein slave boson approach. Impact of enhanced hybridization and magnetic instability of bilayer doped near the Van Hove singularity on the screening of magnetic moment is discussed.
Recent studies show that two low-energy Van Hove singularities (VHSs) seen as two pronounced peaks in the density of states (DOS) could be induced in twisted graphene bilayer. Here, we report angle dependent VHSs of slightly twisted graphene bilayer studied by scanning tunneling microscopy and spectroscopy. We show that energy difference of the two VHSs follows \DeltaEvhs ~ \hbarνF\DeltaK between 1.0^{\circ} and 3.0^{\circ} (here νF ~ 1.1\times106 m/s is the Fermi velocity of monolayer graphene, \DeltaK = 2Ksin(θ/2) is the shift between the corresponding Dirac points of the twisted graphene bi…
The creation of van der Waals heterostructures based on a graphene monolayer and other two-dimensional crystals has attracted great interest because atomic registry of the two-dimensional crystals can modify the electronic spectra and properties of graphene. Twisted graphene bilayer can be viewed as a special van der Waals structure composed of two mutual misoriented graphene layers, where the sublayer graphene not only plays the role of a substrate, but also acts as an equivalent role as the top graphene layer in the structure. Here we report the electronic spectra of slightly twisted graphen…
Twisted graphene bilayers (TGBs) have low-energy van Hove singularities (VHSs) that are strongly localized around AA-stacked regions of the moire pattern. Therefore, they exhibit novel many-body electronic states, such as Mott-like insulator and unconventional superconductivity. Unfortunately, these strongly correlated states were only observed in magic angle TGBs with the twist angle theta~1.1°, requiring a precisely tuned structure. Is it possible to realize exotic quantum phases in the TGBs not limited at the magic angle? Here we studied electronic properties of a TGB with theta~1.64° and d…
The possibility of triggering correlated phenomena by placing a singularity of the density of states near the Fermi energy remains an intriguing avenue towards engineering the properties of quantum materials. Twisted bilayer graphene is a key material in this regard because the superlattice produced by the rotated graphene layers introduces a van Hove singularity and flat bands near the Fermi energy that cause the emergence of numerous correlated phases, including superconductivity. While the twist angle-dependence of these properties has been explored, direct demonstration of electrostatic co…
The electronic band structure of twisted bilayer graphene develops van Hove singularities whose energy depends on the twist angle between the two layers. Using Raman spectroscopy, we monitor the evolution of the electronic band structure upon doping using the G peak area which is enhanced when the laser photon energy is resonant with the energy separation of the van Hove singularities. Upon charge doping, the Raman G peak area initially increases for twist angles larger than a critical angle and decreases for smaller angles. To explain this behavior with twist angle, the energy of separation o…
Moire-Engineered Excitonic Landscape and Phonon-Mediated Recombination in Twisted WSe2 Bilayers
Indian Institute of Technology Mandi（印度技术学院曼迪分校）；CSIR-National Physical Laboratory（印度科学工业研究理事会国家物理实验室）；Academy of Scientific and Innovative Research (AcSIR)（科学与创新研究学院）；Indian Institute of Science（印度科学学院）；National Institute of Material Science（国家物质科学研究所）
Extensive scanning tunnelling microscopy and spectroscopy experiments complemented by first principles and parameterized tight binding calculations provide a clear answer to the existence, origin and robustness of van Hove singularities (vHs) in twisted graphene layers. Our results are conclusive: vHs due to interlayer coupling are ubiquitously present in a broad range (from 1° to 10°) of rotation angles in our graphene on 6H-SiC(000-1) samples. From the variation of the energy separation of the vHs with rotation angle we are able to recover the Fermi velocity of a graphene monolayer as well a…
We have studied the excitonic gap formation in the Bernal Stacked, bilayer graphene (BLG) structures at half-filling. Considering the local Coulomb interaction between the layers, we calculate the excitonic gap parameter and we discuss the role of the interlayer and intralayer Coulomb interactions and the interlayer hopping on the excitonic pair formation in the BLG. Particularly, we predict the origin of excitonic gap formation and condensation, in relation to the farthermost interband optical transition spectrum. The general diagram of excitonic phase transition is given, explaining differen…
A fully selfconsistent treatment for gap generation and Coulomb screening in excitonic insulators is presented. The method is based on the equations of motion for the relevant dynamical variables combined with a variational approach. Applying the theory for a model system of bilayer graphene, an excitonic groundstate with a gap exceeding 10 meV is predicted.
Electron interactions in undoped bilayer graphene lead to instability of the gapless state, `which-layer' symmetry breaking, and energy gap opening at the Dirac point. In contrast to single layer graphene, the bilayer system exhibits instability even for arbitrarily weak interaction. A controlled theory of this instability for realistic dynamically screened Coulomb interactions is developed, with full acount of dynamically generated ultraviolet cutoff. This leads to an energy gap that scales as a power law of the interaction strength, making the excitonic instability readily observable.
Magic-angle twisted bilayer graphene exhibits quasi-flat low-energy bands with Van Hove singularities close to the Fermi level. These singularities play an important role in the exotic phenomena observed in this material, such as superconductivity and magnetism, by amplifying electronic correlation effects. In this work, we study the correspondence of four-terminal conductance and the Fermi surface topology as a function of the twist angle, pressure, and energy in mesoscopic, ballistic samples of small-angle twisted bilayer graphene. We establish a correspondence between features in the wide-j…
Van Hove singularities (VHS's) in the density of states play an outstanding and diverse role for the electronic and thermodynamic properties of crystalline solids. At the critical point the Fermi surface connectivity changes and topological properties undergo a transition. Opportunities to systematically pass a VHS at the turn of a voltage knob and study its diverse impact are however rare. With the advent of van der Waals heterostructures, control over the atomic registry of neigbouring graphene layers offers an unprecedented tool to generate a low energy VHS easily accessible with convention…
In this paper we discuss the optical response due to the excitonic effect of two types of hBN bilayers: AB and AA'. Understanding the properties of these bilayers is of great utility to the study of twisted bilayers at arbitrary angles, since these two configurations correspond to the limit cases of 0 and 60 degree rotation. To obtain the excitonic response we present a method to solve a four-band Bethe-Salpeter equation, by casting it into a 1D problem, thus greatly reducing the numerical burden of the calculation when compared with strictly 2D methods. We find results in good agreement with …
We investigate the many-body instabilities of electrons interacting near Van Hove singularities arising in monolayer and twisted bilayer graphene. We show that a pairing instability must be dominant over the tendency to magnetic order as the Fermi level is tuned to the Van Hove singularity in the conduction band of graphene. As a result of the extended character of the saddle points in the dispersion, we find that the pairing of the electrons takes place preferentially in a channel of f-wave symmetry, with an order parameter vanishing at the position of the saddle points along the Fermi line. …
Excitons in monolayer semiconductors have large optical transition dipole for strong coupling with light field. Interlayer excitons in heterobilayers, with layer separation of electron and hole components, feature large electric dipole that enables strong coupling with electric field and exciton-exciton interaction, at the cost that the optical dipole is substantially quenched (by several orders of magnitude). In this letter, we demonstrate the ability to create a new class of excitons in transition metal dichalcogenide (TMD) hetero- and homo-bilayers that combines the advantages of monolayer-…
By means of atomistic tight-binding calculations, we investigate the effects of uniaxial strain on the electronic bandstructure of twisted graphene bilayer. We find that the bandstructure is dramatically deformed and the degeneracy of the bands is broken by strain. As a conseqence, the number of Dirac cones can double and the van Hove singularity points are separated in energy. The dependence of these effects on the strength of strain, its applied direction and the twist angle is carefully clarified. As an important result, we demonstrate that the position of van Hove singularities can be modu…
We have considered the AB-stacked bilayer graphene Josephson junction. The bilayers are supposed to be in the charge equilibrium states and at the half-filling in each of the electronic layers of the construction and at each value of the external gate. By considering the interacting bilayers in both sides of the junction and by taking into account both intralayer and interlayer Coulomb interaction effects, we have calculated the normal and excitonic tunnel currents through the junction. The electronic band renormalizations have been taken into account, due to the excitonic pairing effects and …
Double-layer electron systems in the quantum Hall regime have excitonic condensate ground states when the layers are close together and the total Landau level filling factor is close to an odd integer. In this paper we discuss the microscopic physics of these states and recent progress toward building a theory of the anomalous collective transport effects that occur in separately contacted bilayers when the condensate is present.
Interaction induced topological states remain one of the fascinating phases in condensed matter physics. The exciton condensate has recently sparked renewed interest due to the discovery of new candidate materials and its driving force to realize exotic topological states. In this work, we explore the exciton orders induced high-order topology in the bilayer quantum spin Hall insulators and find that the topological excitonic corner states can be realized by tuning the gate and magnetic field. When an in-plane Zeeman field is applied to the system, two or four excitonic boundary-obstructed cor…
The effect of tunneling on the transport properties of} quantum Hall double layers in the regime of the excitonic condensate at total filling factor one is studied in counterflow experiments. If the tunnel current $I$ is smaller than a critical $I_C$, tunneling is large and is effectively shorting the two layers. For $I > I_C$ tunneling becomes negligible. Surprisingly, the transition between the two tunneling regimes has only a minor impact on the features of the filling-factor one state as observed in magneto-transport, but at currents exceeding $I_C$ the resistance along the layers increase…
Rotated graphene multilayers form a new class of graphene related systems with electronic properties that drastically depend on the rotation angles. It has been shown that bilayers behave like two isolated graphene planes for large rotation angles. For smaller angles, states in the Dirac cones belonging to the two layers interact resulting in the appearance of two van Hove singularities. States become localised as the rotation angle decreases and the two van Hove singularities merge into one peak at the Dirac energy. Here we go further and consider bilayers with very small rotation angles. In …
We propose a generic topological insulator bilayer (TIB) system to study the excitonic condensation with self-consistent mean-field (SCMF) theory. We show that the TIB system presents the crossover behavior from the Bardeen-Cooper-Schrieffer (BCS) limit to Bose-Einstein condensation (BEC) limit. Moreover, by comparison with traditional semiconductor systems, we find that for the present system the superfluid property in the BEC phase is more sensitive to electron-hole density imbalance and the BCS phase is more robust. Applying this TIB model into Bi$_{2}$Se$_{3}$-family material, we find that…
The competing ground states of bilayer graphene are studied by applying renormalization group techniques to a bilayer honeycomb lattice with nearest neighbor hopping. In the absence of interactions, the Fermi surface of this model at half-filling consists of two nodal points with momenta $\mathbf{K}$, $\mathbf{K}'$, where the conduction band and valence band touch each other, yielding a semi-metal. Since near these two points the energy dispersion is quadratic with perfect particle-hole symmetry, excitonic instabilities are inevitable if inter-band interactions are present. Using a perturbativ…
Using Diffusion Monte Carlo simulations we have investigated the ground state of a symmetric electron-hole bilayer and determined its phase diagram at T=0. We find clear evidence of an excitonic condensate, whose stability however is affected by in-layer electronic correlation. This stabilizes the electron-hole plasma at large values of the density or inter-layer distance, and the Wigner crystal at low density and large distance. We have also estimated pair correlation functions and low order density matrices, to give a microscopic characterization of correlations, as well as to try and estima…
In a continuous search for the energy-efficient electronic switches, a great attention is focused on tunnel field-effect transistors (TFETs) demonstrating an abrupt dependence of the source-drain current on the gate voltage. Among all TFETs, those based on one-dimensional (1D) semiconductors exhibit the steepest current switching due to the singular density of states near the band edges, though the current in 1D structures is pretty low. In this paper, we propose a TFET based on 2D graphene bilayer which demonstrates a record steep subthreshold slope enabled by van Hove singularities in the de…
The low-energy bands of twisted bilayer graphene form Dirac cones with approximate electron-hole symmetry at small rotation angles. These crossings are protected by the emergent symmetries of moiré patterns, conferring a topological character to the bands. Strain accumulated between layers (heterostrain) shifts the Dirac points both in energy and momentum. The overlap of conduction and valence bands favors an excitonic instability of the Fermi surface close to the neutrality point. The spontaneous condensation of electron-hole pairs breaks time reversal symmetry and the separate conservation o…
Van Hove singularity-driven giant Nernst signal in twisted double bilayer graphene
Indian Institute of Science（印度科学研究所）；Tel-Aviv University（特拉维夫大学）；The Ohio State University（俄亥俄州立大学）；Weizmann Institute of Science（魏茨曼科学研究所）；National Institute of Material Science（国家材料研究所）；Tata Institute of Fundamental Research（塔塔基础研究所）
In the present work, we consider the excitonic effects in the twisted bilayer graphene (tBLG) within the rotated bilayer Hubbard model. Both, intralayer and interlayer Coulomb interactions have been considered and the half-filling condition is imposed for the electronic densities is both layers of the bilayer. We calculate the excitonic pairing gap parameter and the chemical potential for different twist angles and different values of the interlayer Coulomb interaction parameter. Furthermore, we show the appearance of the electronic flat bands in the electronic band structure, mediated by the …
Motivated by recent studies that reported the successful synthesis of monolayer Mg(OH)$_{2}$ [Suslu \textit{et al.}, Sci. Rep. \textbf{6}, 20525 (2016)] and hexagonal (\textit{h}-)AlN [Tsipas \textit{et al}., Appl. Phys. Lett. \textbf{103}, 251605 (2013)], we investigate structural, electronic, and optical properties of vertically stacked $h$-AlN and Mg(OH)$_{2}$, through \textit{ab initio} density-functional theory (DFT), many-body quasi-particle calculations within the GW approximation, and the Bethe-Salpeter equation (BSE). It is obtained that the bilayer heterostructure prefers the $AB^{\p…
Bilayer electron-hole systems undergo excitonic condensation when the distance d between the layers is smaller than the typical distance between particles within a layer. All excitons in this condensate have a fixed dipole moment which points perpendicular to the layers, and therefore this condensate of dipoles couples to external electromagnetic fields. We study the transport properties of this dipolar condensate system based on a phenomenological model which takes into account contributions from the condensate and quasiparticles. We discuss, in particular, the drag and counterflow transport,…
By employing the first-principles GW-Bethe-Salpeter Equation (BSE) simulation, we obtain, for the first time, the accurate quasiparticle (QP) band gap, optical absorption spectra and their dependence on the gate field of gated bilayer graphene (GBLG). Many-electron effects are shown to be extremely important to understand these excited-state properties; enhanced electron-electron interactions dramatically enlarge the QP band gap; infrared optical absorption spectra are dictated by bright bound excitons. Our results well explain recent experiments and satisfyingly solve the puzzle about the inc…
We consider the optical properties of the half-filled AB-stacked bilayer graphene with the excitonic pairing and condensation between the layers. Both intra and interlayer local Coulomb interaction effects have been taken into account and the role of the exact Fermi energy has been discussed in details. We have calculated the absorption coefficient, refractive index, dielectric response functions and the electron energy loss spectrum for different interlayer Coulomb interaction regimes and for different temperatures. Considering the full four-band model for the interacting AB bilayer graphene,…
We construct a quantum Ginsburg-Landau theory to study the quantum phase transition from the excitonic superfluid (ESF) to a possible pseudo-spin density wave (PSDW) at some intermediate distances driven by the magneto-roton minimum collapsing at a finite wavevector. We analyze the properties of the PSDW and explicitly show that a square lattice is the favorite lattice. We suggest that correlated hopping of vacancies in the active and passive layers in the PSDW state leads to very large and temperature dependent drag consistent with the experimental data. Comparisons with previous microscopic …
Graphene, a single sheet of graphite with honeycomb lattice structure, has massless carriers with tunable density and polarity. We investigate the ground state phase diagram of two graphene sheets (embedded in a dielectric) separated by distance $d$ where the top layer has electrons and the bottom layer has holes, using mean-field theory. We find that a uniform excitonic condensate occurs over a large range of carrier densities and is weakly dependent on the relative orientation of the two sheets. We obtain the excitonic gap, quasiparticle energy and the density of states. We show that both, t…
Superfluidity in e-h bilayers in graphene and GaAs has been predicted many times but not observed. A key problem is how to treat the screening of the Coulomb interaction for pairing. Different mean-field theories give dramatically different conclusions, and we test them against diffusion Monte-Carlo calculations. We get excellent agreement with the mean-field theory that uses screening in the superfluid state, but large discrepancies with the others. The theory predicts no superfluidity in existing devices and gives pointers for new devices to generate superfluidity.
The physics of vortices, instantons and deconfinement is studied for layered superfluids in connection to bilayer quantum Hall systems at filling fraction nu=1. We develop an effective gauge theory taking into account both vortices and instantons induced by interlayer tunneling. The renormalization group flow of the gauge charge and the instanton fugacity shows that the coupling of the gauge field to vortex matter produces a continuous transition between the confining phase of free instantons and condensed vortices and a deconfined gapless superfluid where magnetic charges are bound into dipol…
Structural engineering of van der Waals heterostructures via stacking and twisting has recently been used to create moiré superlattices, enabling the realization of new optical and electronic properties in solid-state systems. In particular, moiré lattices in twisted bilayers of transition metal dichalcogenides (TMDs) have been shown to lead to exciton trapping, host Mott insulating and superconducting states, and act as unique Hubbard systems whose correlated electronic states can be detected and manipulated optically. Structurally, these twisted heterostructures also feature atomic reconstru…
In this paper, we consider the spectral properties of the bilayer graphene with the local excitonic pairing interaction between the electrons and holes. We consider the generalized Hubbard model, which includes both intralayer and interlayer Coulomb interaction parameters. The solution of the excitonic gap parameter is used to calculate the electronic band structure, single-particle spectral functions, the hybridization gap, and the excitonic coherence length in the bilayer graphene. We show that the local interlayer Coulomb interaction is responsible for the semimetal-semiconductor transition…
The stacking and bending of graphene are trivial but extremely powerful agents of control over graphene's manifold physics. By changing the twist angle, one can drive the system over a plethora of exotic states via strong electron correlation, thanks to the moiré superlattice potentials, while the periodic or triaxial strains induce discretization of the band structure into Landau levels without the need for an external magnetic field. We fabricated a hybrid system comprising both the stacking and bending tuning knobs. We have grown the graphene monolayers by chemical vapor deposition, using $…
Topological phases, van Hove singularities, and spin texture in magic-angle twisted bilayer graphene in the presence of proximity-induced spin-orbit couplings
Motivated by measurements of compressibility and STM spectra in twisted bilayer graphene, we analyze the pattern of symmetry breaking for itinerant fermions near a van Hove singularity. Making use of an approximate SU(4) symmetry of the Landau functional, we show that the structure of the spin/isospin order parameter changes with increasing filling via a cascade of transitions. We compute the feedback from different spin/isospin orders on fermions and argue that each order splits the initially 4-fold degenerate van Hove peak in a particular fashion, consistent with the STM data and compressibi…
