Tailoring the band structure of twisted double bilayer graphene with pressure
Bálint Szentpéteri, Peter Rickhaus, Folkert K. de Vries, Albin Márffy, Bálint Fülöp, Endre Tóvári, Kenji Watanabe, Takashi Taniguchi, Andor Kormányos, Szabolcs Csonka, Péter Makk
Twisted two-dimensional structures open new possibilities in band structure engineering. At magic twist angles, flat bands emerge, which give a new drive to the field of strongly correlated physics. In twisted double bilayer graphene dual gating allows changing the Fermi level and hence the electron density and also allows tuning the interlayer potential, giving further control over band gaps. Here, we demonstrate that by applying hydrostatic pressure, an additional control of the band structure becomes possible due to the change of tunnel couplings between the layers. We find that the flat bands and the gaps separating them can be drastically changed by pressures up to 2 GPa, in good agreement with our theoretical simulations. Furthermore, our measurements suggest that in finite magnetic field due to pressure a topologically non-trivial band gap opens at the charge neutrality point at zero displacement field.
Twisted bilayer graphenes with magical angle exhibit strongly correlated electronic properties because of the isolated flat band at the Fermi level. We studied the twisted bilayer graphene with substrates on both layers. The substrate induce Kekul$\acute{e}$ distortion for each graphene layer. The systems are investigated by both continuous Dirac Fermion model and tight binding model. The two investigations give similar conclusion that isolated flat band with ultra-narrow bandwidth could appear.
We report an unusual, non-monotonous dependence of the exchange bias on the thickness of the ferromagnetic layer in a ferromagnet/antiferromagnet bilayer system. We show that in epitaxial CoO/Fe(110) bilayers, the evolution of the Fe magnetic anisotropy, which drives the thickness-induced in-plane spin-reorientation process, controls the interfacial CoO spin directions in the 0-90 degrees range and, consequently, drastically modifies the magnitude of the hysteresis loop shift and its dependence on the thickness of the Fe layer. Our results present a new recipe for tailoring the exchange bias a…
We show that the twisted graphene bilayer can reveal unusual topological properties at low energies, as a consequence of a Dirac-point splitting. These features rely on a symmetry analysis of the electron hopping between the two layers of graphene and we derive a simplified effective low-energy Hamiltonian which captures the essential topological properties of twisted bilayer graphene. The corresponding Landau levels peculiarly reveal a degenerate zero-energy mode which cannot be lifted by strong magnetic fields.
We study the edge states of twisted bilayer graphene and their topological origin. We show that the twisted bilayer graphene has special edge states associated with the moiré pattern, and the emergence of these moiré edge states is linked with the sliding Chern number, which describes topological charge pumping caused by relative interlayer sliding. When one layer of the twisted bilayer is relatively slid with respect to the other layer, the edge states are transferred from a single band to another across the band gap, and the number of the edge states pumped in a sliding cycle is shown to be …
We introduce a minimum tight-binding model with only three parameters extracted from graphene and untwisted bilayer graphene. This model reproduces quantitatively the electronic structure of not only these two systems and bulk graphite near the Fermi level, but also that of twisted bilayer graphene including the value of the magic angle, at which bands at $E_F$ flatten without overlap and two gaps open, one above and one below $E_F$. The Hamiltonian is sufficiently transparent and flexible to be adopted to other twisted layered systems.
Twisted bilayer graphene with tiny rotation angles have drawn significant attention due to the observation of the unconventional superconducting and correlated insulating behaviors. In this paper, we employ a full tight-binding model to investigate collective excitations in twisted bilayer graphene near magic angle. The polarization function is obtained from the tight-binding propagation method without diagonalization of the Hamiltonian matrix. With the atomic relaxation considered in the simulation, damped and undamped interband plasmon modes are discovered near magic angle under both room te…
Angle disorder is an intrinsic feature of twisted bilayer graphene and other moiré materials. Here, we discuss electron transport in twisted bilayer graphene in the presence of angle disorder. We compute the local density of states and the Landauer-Büttiker transmission through an angle disorder barrier of width comparable to the moiré period, using a decimation technique based on a real space description. We find that barriers which separate regions where the width of the bands differ by 50% or more lead to a minor suppression of the transmission, and that the transmission is close to one for…
Twisted bilayer graphene provides a new two-dimensional platform for studying electron interaction phenomena and flat band properties such as correlated insulator transition, superconductivity and ferromagnetism at certain magic angles. Here, we present strong evidence of correlated insulator states and superconductivity signatures in p-type twisted double-bilayer WSe$_2$. Enhanced interlayer interactions are observed when the twist angle decreases to a few degrees as reflected by the high-order satellites in the electron diffraction patterns taken from the 2H/3R-stacked domains reconstructed …
Theory predicts that the application of an electric field breaks the inversion symmetry of AB and BA stacked domains in twisted bilayer graphene, resulting in the formation of a triangular network of one-dimensional valley-protected helical states. This two-dimensional network of one-dimensional states has been observed in several studies, but direct experimental evidence that the electronic transport in these one-dimensional states is valley-protected is still lacking. In this study, we report the existence of the network in small-angle twisted bilayer graphene at room temperature. Moreover, …
We numerically calculate the optical conductivity of twisted graphene bilayers within the continuum model. To obtain the imaginary part, we employ the regularized Kramers-Kronig relation allowing us to discuss arbitrary twist angles, chemical potential and temperature. We find that the Drude weight $D$ as function of the chemical potential $μ$ closely follows the shell structure of twisted bilayer displayed by the density of states. For certain angles, this results in a transport gap D=0 at finite $μ$. We also discuss the loss function which, for low doping, is characterized by acoustic interb…
We apply a multiscale modeling approach to study lattice reconstruction in marginally twisted bilayers of transition metal dichalcogenides (TMD). For this, we develop DFT-parametrized interpolation formulae for interlayer adhesion energies of MoSe$_2$, WSe$_2$, MoS$_2$, and WS$_2$, combine those with elasticity theory, and analyze the bilayer lattice relaxation into mesoscale domain structures. Paying particular attention to the inversion asymmetry of TMD monolayers, we show that 3R and 2H stacking domains, separated by a network of dislocations develop for twist angles $θ^{\circ}<θ^{\circ}_P\…
Incommensurately twisted graphene bilayers are described by long-wavelength theories, but to date such theories exist only at small angles of interlayer rotation. We construct a long wavelength theory without such a restriction, instead requiring nearness to commensuration. The theory inherits its energy scale from the exactly commensurate bilayer that it is close to. It is a spatial interpolation between the low-energy theories of commensurate structures with the two possible sublattice exchange (SE) symmetries: SE even and SE odd. In addition to generalizing existing theories, our theory bri…
We report that two rotated layers of blue phosphorene behave as a direct band gap semiconductor. The optical spectrum shows absorption peaks in the visible region of the spectrum and in addition the energy of these peaks can be tuned with the rotational angle. These findings makes twisted bilayer blue phosphorene a strong candidate as a solar cell or photodetection device. Our results are based on ab initio calculations of several rotated blue phosphorene layers.
Recently, the twist angle between adjacent sheets of stacked van der Waals materials emerged as a new knob to engineer correlated states of matter in two-dimensional heterostructures in a controlled manner, giving rise to emergent phenomena such as superconductivity or correlated insulating states. Here,we use an ab initio based approach to characterize the electronic properties of twisted bilayer MoS2. We report that, in marked contrast to twisted bilayer graphene, slightly hole-doped MoS2 realizes a strongly asymmetric px-py Hubbard model on the honeycomb lattice, with two almost entirely di…
We show that a sliding motion between the two layers of a \moire superlattice induces an electric current and realizes a two-dimensional version of the topological Thouless pump when the Fermi energy lies in one of the minigaps. Interestingly, a chiral charge pump, namely, a transverse current induced by the sliding motion, is possible in twisted homobilayers. This result is confirmed by a concrete calculation of the adiabatic current in twisted bilayer graphene. Our work reveals an interesting link between mechanical motion and electricity unique to \moire superlattices, and may find applicat…
We study the transport properties of a twisted bilayer graphene flake contacted by two monolayer nanoribbons which act as leads. We analyze the conductance in terms of the spectra of the bilayer nanoribbon and the monolayer contacts. The low-energy transport properties are governed by the edge states with AB stacking. Remarkably, the electronic conductance in this energy region does not depend much on the relative position of the leads, in contrast with that of bilayer flakes with more symmetric stackings. We attribute this feature to the localization of these low-energy states in the AB edge …
Selection rules and interference effects in angle resolved photoemission spectra from twisted graphene bilayers are studied within a long wavelength theory for the electronic structure. Using a generic model for the interlayer coupling, we identify features in the calculated ARPES momentum distributions that are controlled by the singularities and topological character of its long wavelength spectrum. We distinguish spectral features that are controlled by single-layer singularities in the spectrum, their modification by gauge potentials in each layer generated by the interlayer coupling, and …
We identify a mapping between two-dimensional (2D) electron transport in a minimally twisted graphene bilayer and a 1D quantum walk, where one spatial dimension plays the role of time. In this mapping a magnetic field B perpendicular to the bilayer maps onto an electric field. Bloch oscillations due to the periodic motion in a 1D Bloch band can then be observed in purely DC transport as magnetoconductance oscillations with periodicity set by the Bloch frequency.
A new implementation of stochastic many-body perturbation theory for periodic 2D systems is presented. The method is used to compute quasiparticle excitations in twisted bilayer phosphorene. Excitation energies are studied using stochastic $G_0W_0$ and partially self-consistent $\bar ΔGW_0$ approaches. The approach is inexpensive; it is used to study twisted systems with unit cells containing $>2,700$ atoms ($>13,500$ valence electrons), which corresponds to a minimum twisting angle of $\approx 3.1^\circ$. Twisted bilayers exhibit band splitting, increased localization and formation of localiz…
The electric structure of twisted bilayer GeSe, which shows a rectangular moiré pattern, is analyzed using a $\bm{k}\cdot\bm{p}$ type effective continuum model. The effective model is constructed on the basis of the the local approximation method, where the local lattice structure of a twisted bilayer system is approximated by its untwisted bilayer with parallel displacement, and the required parameters are fixed with the help of the first-principles method. By inspecting the twist angle dependence of the physical properties, we reveal a relation between the effective potential under moiré pat…
Flatbands with extremely narrow bandwidths on the order of a few mili-electron volts can appear in twisted multilayer graphene systems for appropriate system parameters. Here we investigate the electronic structure of a twisted bi-bilayer graphene, or twisted double bilayer graphene, to find the parameter space where isolated flatbands can emerge as a function of twist angle, vertical pressure, and interlayer potential differences. We find that in twisted bi-bilayer graphene the bandwidth is generally flatter than in twisted bilayer graphene by roughly up to a factor of two in the same paramet…
The mechanisms of optical activity and quantum transport of twisted bilayer graphene are studied. The formation of unique electron states in the bilayer systems is studied using an effective continuum model. Such states are shown to support the correlation of transverse motions of electrons in two graphene layers. Because of the chiral structure of the atomic lattices, the contribution of such drag correlations is incompletely cancelled, thus resulting in a drag term of the optical conductivity tensor. We show that the drag term of the conductivity is the manifestation of the spatial dispersio…
We investigate the band structure of twisted monolayer-bilayer graphene (tMBG), or twisted graphene on bilayer graphene (tGBG), as a function of twist angles and perpendicular electric fields in search of optimum conditions for achieving isolated nearly flat bands. Narrow bandwidths comparable or smaller than the effective Coulomb energies satisfying $U_{\textrm{eff}} /W \gtrsim 1$ are expected for twist angles in the range of $0.3^{\circ} \sim 1.5^{\circ}$, more specifically in islands around $θ\sim 0.5^{\circ}, \, 0.85^{\circ}, \,1.3^{\circ}$ for appropriate perpendicular electric field magn…
Higher-order topological insulators are newly proposed topological phases of matter, whose bulk topology manifests as localized modes at two- or higher-dimensional lower boundaries. In this work, we propose the twisted bilayer graphenes with large angles as higher-order topological insulators, hosting topological corner charges. At large commensurate angles, the intervalley scattering opens up the bulk gap and the corner states occur at half filling. Based on both first-principles calculations and analytic analysis, we show the striking results that the emergence of the corner states do not de…
Control over minivalley polarization and interlayer coupling is demonstrated in double bilayer graphene twisted with an angle of 2.37$^\circ$. This intermediate angle is small enough for the minibands to form and large enough such that the charge carrier gases in the layers can be tuned independently. Using a dual-gated geometry we identify and control all possible combinations of minivalley polarization via the population of the two bilayers. An applied displacement field opens a band gap in either of the two bilayers, allowing us to even obtain full minivalley polarization. In addition, the …
We construct an analytic continuum model to describe the electronic structure and the electron-phonon interaction in twisted bilayer graphenes with arbitrary lattice deformation. Starting from the tight-binding model, we derive the interlayer Hamiltonian in the presence of general lattice displacement, and obtain a long-wavelength continuum expression for smooth deformation. We show that the continuum model correctly describes the band structures of the lattice-relaxed twisted bilayer graphenes. We apply the formula to the phonon vibration, and derive an explicit expression of the electron-pho…
In the presence of a finite interlayer displacement field bilayer graphene has an energy gap that is dependent on stacking and largest for the stable AB and BA stacking arrangements. When the relative orientations between layers are twisted through a small angle to form a moir$\mathrm{\acute{e}}$ pattern, the local stacking arrangement changes slowly. We show that for non-zero displacement fields the low-energy physics of twisted bilayers is captured by a phenomenological helical network model that describes electrons localized on domain walls separating regions with approximate AB and BA stac…
The experimental control over the twist angle in twisted bilayer graphene has not been reported and its realistic structure is most likely incommensurate. In this paper, we develop a tight-binding virtual crystal approximation theory to study the electronic properties in incommensurate twisted bilayer graphene. The theory yields the electronic band structure and the local density of states for any incommensurate twist angle θ between the graphene sheets. Angle dependent Van Hove singularities are observed in the numerically calculated local density of states. In accord with observations in sca…
We derive a simple formula for the real-space chirality of twisted bilayer graphene that can be related to the cross-product of its sheet currents. This quantity shows well-defined plateaus for the first remote band as function of the gate voltage which are approximately quantized for commensurate twist angles. The zeroth plateau corresponds to the first magic angle where a sign change occurs due to an emergent $C_6$-symmetry. Our observation offers a new definition of the magic angle based on a macroscopic observable which is accessible in typical transport experiments.
We develop a general theory of the layer circular photogalvanic effect (LCPGE) in quasi two-dimensional chiral bilayers, which refers to the appearance of a polarization-dependent, out-of-plane dipole moment induced by circularly polarized light. We elucidate the geometric origin of the LCPGE as two types of interlayer coordinate shift weighted by the quantum metric tensor and the Berry curvature, respectively. As a concrete example, we calculate the LCPGE in twisted bilayer graphene, and find that it exhibits a resonance peak whose frequency can be tuned from visible to infrared as the twisti…
We investigate the gap in the single-electron spectrum of twisted bilayer graphene. In a perfect infinite lattice of a twisted bilayer, the gap varies exponentially in response to weak changes of the twist angle. Such a large sensitivity makes theoretical predictions of the gap nearly impossible, since experimentally the twist angle is always known with finite accuracy. To address this issue, we numerically study finite clusters of twisted bilayer graphene. For finite systems, changing the twist angle causes a gradual crossover between gapless and gapped regimes. The crossover occurs when the …
The transport properties of a twisted bilayer graphene barrier are investigated for various twist angles. Remarkably, for small twist angles around the magic angle $θ_m \sim 1.05^{\circ}$, the local currents around the AA-stacked regions are strongly enhanced compared to the injected electron rate. Furthermore, the total and counterflow (magnetic) current patterns show high correlations in these regions, given rise to well-defined magnetic moments that form a magnetic Moiré superlattice. The orientation and magnitude of these magnetic moments changes as function of the gate voltage and possibl…
Twisted bilayer graphene (tBLG) represents a family of unique materials with optoelectronic properties tuned by the rotation angle between the two layers. The presented work shows an additional way of tweaking the electronic structure of tBLG: by modifying the interlayer distance, for example by a small uniaxial out-of-plane compression. We have focused on the optical transition energy, which shows a clear dependence on the interlayer distance, both experimentally and theoretically.
Crystal fields occur due to a potential difference between chemically different atomic species. In Van-der-Waals heterostructures such fields are naturally present perpendicular to the planes. It has been realized recently that twisted graphene multilayers provide powerful playgrounds to engineer electronic properties by the number of layers, the twist angle, applied electric biases, electronic interactions and elastic relaxations, but crystal fields have not received the attention they deserve. Here we show that the bandstructure of large-angle twisted double bilayer graphene is strongly modi…
Lattice reconstruction in twisted transition-metal dichalcogenide (TMD) bilayers gives rise to piezo- and ferroelectric moiré potentials for electrons and holes, as well as a modulation of the hybridisation across the bilayer. Here, we develop hybrid $\mathbf{k}\cdot \mathbf{p}$ tight-binding models to describe electrons and holes in the relevant valleys of twisted TMD homobilayers with parallel (P) and anti-parallel (AP) orientations of the monolayer unit cells. We apply these models to describe moiré superlattice effects in twisted WSe${}_2$ bilayers, in conjunction with microscopic \emph{ab…
Using density functional theory, we investigate the interplay between the stacking order and sequence of bilayers composed of an Fe and a Rh layer on the Re(0001) and their magnetic properties. We find that fcc/ffc stacked bilayers are energetically very unfavorable, while all other combinations of hcp and fcc stacking are energetically close. The magnetic interactions are evaluated by mapping the DFT total energies onto a spin model, which contains Heisenberg exchange, Dzyaloshinskii-Moriya interaction, the magnetocrystalline anisotropy energy, and higher-order exchange interactions. We find …
We introduce a new approach that allows one complete control over the modulation of the effective twist angle change in few-layer van der Waals heterostructures by irradiating them with longitudinal waves of light at the end of a waveguide. As a specific application, we consider twisted bilayer graphene and show that one can tune the magic angles to be either larger or smaller, allowing in-situ experimental control of the phase diagram of this and other related materials. A waveguide allows one to circumvent the free-space constraints on the absence of longitudinal electric field components of…
We present an effective (minimal) theory for chiral two-dimensional materials. These materials possess an electro-magnetic coupling without exhibiting a topological gap. As an example, we study the response of doped twisted bilayers, unveiling unusual phenomena in the zero frequency limit. An in-plane magnetic field induces a huge paramagnetic response at the neutrality point and, upon doping, also gives rise to a substantial longitudinal Hall response. The system also accommodates nontrivial longitudinal plasmonic modes which are associated with a longitudinal magnetic moment, thus endowing t…
The charge susceptibility of twisted bilayer graphene is investigated in the Dirac cone, respectively random-phase approximation. For small enough twist angles $θ\lesssim 2^\circ$ we find weakly Landau damped interband plasmons, i.~e., collective excitonic modes which exist in the undoped material, with an almost constant energy dispersion. In this regime, the loss function can be described as a Fano resonance and we argue that these excitations arise from the interaction of quasi-localised states with the incident light field. These predictions can be tested by nano-infrared imaging and possi…
We theoretically study the electronic structure of small-angle twisted bilayer graphene with a large potential asymmetry between the top and bottom layers. We show that the emergent helical states known to appear on the triangular AB-BA domain boundary do not actually form a percolating network, but instead they provide independent, perfect one-dimensional channels propagating in three different directions. Using the continuum-model Hamiltonian, we demonstrate that an applied bias causes two well-defined energy windows which contain sparsely distributed one-dimensional channels. The origin of …
The electronic properties of twisted bilayer graphene on SiC substrate were studied via combination of transport measurements and scanning tunneling microscopy. We report the observation of enhanced intervalley scattering from one Dirac cone to the other, which contributes to weak localization, of the twisted bilayer graphene by increasing the interlayer coupling strength. Our experiment and analysis demonstrate that the enhanced intervalley scattering is closely related to the periodic AB stacked atoms (the A atom of layer 1 and the B atom of layer 2 that have the same horizontal positions) t…
The large lattice constant of Moire superlattice formed in twisted bilayer graphene for small twist enables observing the Landau levels splitting into Hofstadter butterflies in energy spectra for moderate magnetic field. This is expected for generic system under homogeneous bias conditions but its robustness against spatial potential fluctuations is left open question. We study the energy structure of twisted bilayer system in dependence of both, the homogeneous magnetic field and the bias voltage applied exclusively in its central part. Although the translational symmetry is broken, the energ…
Twisted graphene bilayers develop highly localised states around AA-stacked regions for small twist angles. We show that interaction effects may induce either an antiferromagnetic (AF) and a ferromagnetic (F) polarization of said regions, depending on the electrical bias between layers. Remarkably, F-polarised AA regions under bias develop spiral magnetic ordering, with a relative $120^\circ$ misalignment between neighbouring regions due to a frustrated antiferromagnetic exchange. This remarkable spiral magnetism emerges naturally without the need of spin-orbit coupling, and competes with the …
The bands of graphite are extremely sensitive to topological defects which modify the electronic structure. In this paper we found non-dispersive flat bands no farther than 10 meV of the Fermi energy in slightly twisted bilayer graphene as a signature of a transition from a parabolic dispersion of bilayer graphene to the characteristic linear dispersion of graphene. This transition occurs for relative rotation angles of layers around $1.5^o$ and is related to a process of layer decoupling. We have performed ab-initio calculations to develop a tight binding model with an interaction Hamiltonian…
The large surface-to-volume ratio in atomically thin 2D materials allows to efficiently tune their properties through modifications of their environment. Artificial stacking of two monolayers into a bilayer leads to an overlap of layer-localized wave functions giving rise to a twist angle-dependent hybridization of excitonic states. In this joint theory-experiment study, we demonstrate the impact of interlayer hybridization on bright and momentum-dark excitons in twisted WSe$_2$ bilayers. In particular, we show that the strong hybridization of electrons at the $Λ$ point leads to a drastic reds…
We investigate the electronic density redistribution of rotated bilayer graphene under a perpendicular electric field, showing that the layers are actually coupled even for large angles. This layer-layer coupling is evidenced by the charge transfer on these structures as a function of the external voltage. We find an inhomogeneous excess charge distribution that is related to the moiré patterns for small angles, but that persists for larger angles where the carriers' velocity is equal to that of single layer graphene. Our results show that rotated bilayer systems are coupled for all rotation a…
The Josephson effect is one of the most studied macroscopic quantum phenomena in condensed matter physics and has been an essential part of the quantum technologies development over the last decades. It is already used in many applications such as magnetometry, metrology, quantum computing, detectors or electronic refrigeration. However, developing devices in which the induced superconductivity can be monitored, both spatially and in its magnitude, remains a serious challenge. In this work, we have used local gates to control confinement, amplitude and density profile of the supercurrent induc…
Currently there is a lively discussion concerning Fermi velocity renormalization in twisted bilayers and several contradicted experimental results are reported. Here we study electronic structures of the twisted bilayers by scanning tunneling microscopy (STM) and spectroscopy (STS). The interlayer coupling strengths between the adjacent bilayers are measured according to energy separations of two pronounced low-energy van Hove singularities (VHSs) in the STS spectra. We demonstrate that there is a large range of values for the interlayer interaction in different twisted bilayers. Below the VHS…
We present a simple derivation of a continuum Hamiltonian for bilayer graphene with an arbitrary smooth lattice deformation -- technically in a fashion parametrized by displacement fields with small gradients. We show that this subsumes the continuum model of Bistritzer and Macdonald for twisted bilayer grapheneas well as many generalizations and extensions of it. The derivation is carried out entirely in real space.
Electronic structures and their Landau quantizations in twisted graphene bilayer and trilayer are investigated using scanning tunnelling microscopy and spectroscopy. In the twisted trilayer, the top graphene layer and second layer are AB (Bernal) stacking and there is a stacking misorientation between the second layer and third layer. Both the twisted bilayer and trilayer exhibit two pronounced low-energy van Hove singularities (VHSs) in their spectra. Below the VHSs, the observed Landau level quantization in the twisted bilayer is identical to that of massless Dirac fermion in graphene monola…
