We formulate the chiral decomposition rules that govern the electronic structure of a broad family of twisted $N+M$ multilayer graphene configurations that combine arbitrary stacking order and a mutual twist. We show that at the magic angle in the chiral limit the low-energy bands of such systems are composed of chiral pseudospin doublets which are energetically entangled with two flat bands per valley induced by the moiré superlattice potential. The analytic analysis is supported by explicit numerical calculations based on realistic parameterization. We further show that applying vertical displacement fields can open up energy gaps between the pseudospin doublets and the two flat bands, such that the flat bands may carry nonzero valley Chern numbers. These results provide guidelines for the rational design of various topological and correlated states in generic twisted graphene multilayers.
We use a tight-binding model and the random-phase approximation to study the Coulomb excitations in simple-hexagonal-stacking multilayer graphene and discuss the field effects. The calculation results include the energy bands, the response functions, and the plasmon dispersions. A perpendicular electric field is predicted to induce significant charge transfer and thus capable of manipulating the energy, intensity, and the number of plasmon modes. This could be further validated by inelastic light scattering or electron-energy-loss spectroscopy.
We present a theoretical study on the electron transmission through the AB-BA stacking boundary in multilayer graphene. Using the tight-binding model and the transfer matrix method, we calculate the electron transmission probability through the boundary as a function of electron Fermi energy in multilayers from bilayer to five-layer. We find that the transmission is strongly suppressed particularly near the band touching point, suggesting that the electronic conductivity in general multilayer graphenes is significantly interfered by stacking fault. The conductivity suppression by stacking faul…
We identify qualitative trends in the stacking sequence dependence of carrier-carrier interaction phenomena in multilayer graphene. Our theory is based on a new approach which explicitly exhibits the important role in interaction phenomena of the momentum-direction dependent intersite phases determined by the stacking sequence. Using this method, we calculate and compare the self-energies, density--density response functions, collective modes, and ground-state energies of several different few layer graphene systems. The influence of electron--electron interactions on important electronic prop…
The crystal structure of solid-state matter greatly affects its electronic properties. For example in multilayer graphene, precise knowledge of the lateral layer arrangement is crucial, since the most stable configurations, Bernal and rhombohedral stacking, exhibit very different electronic properties. Nevertheless, both stacking orders can coexist within one flake, separated by a strain soliton that can host topologically protected states. Clearly, accessing the transport properties of the two stackings and the soliton is of high interest. However, the stacking orders can transform into one a…
Rhombohedral multilayer graphene is a physical realization of the chiral two-dimensional electron gas that can host zero-line modes (ZLMs), also known as kink states, when the local ap opened by inversion symmetry breaking potential changes sign in real space. Here we study how the variations in the local stacking coordination of multilayer graphene affects the formation of the ZLMs. Our analysis indicates that the valley Hall effect develops whenever an interlayer potential difference is able to open up a band gap in stacking faulted multilayer graphene, and that ZLMs can appear at the domain…
Using bilayer CrI$_3$ as an example, we demonstrate that stacking domain walls in van der Waals magnets can host one dimensional (1D) magnon channels, which have lower energies than bulk magnons. Interestingly, some magnon channels are hidden in magnetically homogeneous background and can only be inferred with the knowledge of stacking domain walls. Compared to 1D magnons confined in magnetic domain walls, 1D magnons in stacking domain walls are more stable against external perturbations. We show that the relaxed moiré superlattices of small-angle twisted bilayer CrI$_3$ is a natural realizati…
We study the effect of perpendicular electric fields on the band structures of ABA and ABC graphene multilayers, and find that the electronic screening effect is significantly different between them. In ABA multilayers, the field produces a band overlap and gives a linear screening, while in ABC multilayers, in contrast, it opens an energy gap in the surface-state band at low energy, leading to a strong screening effect essentially non-linear to the field amplitude. The energy gap of a large ABC stack sharply rises when the external field exceeds a certain critical value.
We derive a general relation between the stacking vector ${\bf u}$ describing the relative shift of two layers of bilayer graphene and the Chern index. We find $C = ν- \text{sign}\left(|V_{AB}|-|V_{BA}|\right)$, where $ν$ is a valley index and $|V_{αβ}|$ the absolute value of stacking potentials that depend on ${\bf u}$ and that uniquely determine the interlayer interaction; AA stacking plays no role in the topological character. With this expression we show that while ideal and relaxed minimally twisted bilayer graphene appear so distinct as to be almost different materials, their Chern index…
The effect of different stacking order of graphene multilayers on the electric field induced band gap is investigated. We considered a positively charged top and a negatively charged back gate in order to independently tune the band gap and the Fermi energy of three and four layer graphene systems. A tight-binding approach within a self-consistent Hartree approximation is used to calculate the induced charges on the different graphene layers. We found that the gap for trilayer graphene with the ABC stacking is much larger than the corresponding gap for the ABA trilayer. Also we predict that fo…
There has been a lot of excitement around the observation of superconductivity in twisted bilayer graphene, associated to flat bands close to the Fermi level. Such correlated electronic states also occur in multilayer rhombohedral stacked graphene (RG), which has been receiving increasing attention in the last years. In both natural and artificial samples however, multilayer stacked Bernal graphene (BG) occurs more frequently, making it desirable to determine what is their relative stability and under which conditions RG might be favored. Here, we study the energetics of BG and RG in bulk and …
We study the electronic structure of multilayer graphenes with a mixture of Bernal and rhombohedral stacking and propose a general scheme to understand the electronic band structure of an arbitrary configuration. The system can be viewed as a series of finite Bernal graphite sections connected by stacking faults. We find that the low-energy eigenstates are mostly localized in each Bernal section, and, thus, the whole spectrum is well approximated by a collection of the spectra of independent sections. The energy spectrum is categorized into linear, quadratic and cubic bands corresponding to sp…
We calculate the conductivity of arbitrarily stacked multilayer graphene sheets within a relaxation time approximation, considering both short-range and long-range impurities. We theoretically investigate the feasibility of identifying the stacking order of these multilayers using transport measurements. For relatively clean samples, the conductivities of the various stacking configurations depend on the carrier density as a power-law for over two decades. This dependence arises from a low density decomposition of the multilayer band structure into a sum of chiral Hamiltonians. For dirty sampl…
Due to the observed superconductivity, the alternating twisted trilayer graphene (ATTLG) has drawn great research interest very recently, in which three monolayer graphene (MLG) are stacked in alternating twist way. If one or several of the MLG in ATTLG are replaced by a multilayer graphene, we get a double twisted multilayer graphene (DTMLG). In this work, we theoretically illustrate that, if the DTMLG has a mirror symmetry along z direction like the ATTLG, there exists a mirror symmetry decomposition (MSD), by which the DTMLG can be exactly decoupled into two subsystems with opposite parity.…
We present an analytical theory to describe three-dimensional magnetic textures in perpendicularly magnetized magnetic multilayers that arise in the presence of magnetostatic interactions and the Dzyaloshinskii-Moriya interaction (DMI). We demonstrate that domain walls in multilayers develop a complex twisted structure, which persists even for films with strong DMI. The origin of this twist is surface-volume stray field interactions that manifest as a depth-dependent effective field whose form mimics the DMI effective field. We find that the wall twist has a minor impact on the equilibrium sky…
Successful synthesis of the nitrogenated holey two-dimensional structures C2N (Nat. Commun. 2015, 6, 1-7) using simply wet-chemical reaction offer a cost-effective way to generate other 2D materials with novel optical and electronic properties. Using the few-layer C2N as models, we have performed an ab initio study of electronic properties of layered C2N. Band gaps of this system exhibit monotone decreasing as the number of layers increase. And a direct-gap to indirect-gap transition at the bulk C2N. Besides, when we apply an out-of-plane electric field on few-layer C2N, the band gap of multil…
We theoretically study the correlated insulator states, quantum anomalous Hall (QAH) states, and field-induced topological transitions between different correlated states in twisted multilayer graphene systems. Taking twisted bilayer-monolayer graphene and twisted double-bilayer graphene as examples, we show that both systems stay in spin polarized, $C_{3z}$-broken insulator states with zero Chern number at 1/2 filling of the flat bands under finite displacement fields. In some cases these spin polarized, nematic insulator states are in the quantum valley Hall phase by virtue of the nontrivial…
Stacking two-dimensional layered materials such as graphene and transitional metal dichalcogenides with nonzero interlayer twist angles has recently become attractive because of the emergence of novel physical properties. Stacking of one-dimensional nanomaterials offers the lateral stacking offset as an additional parameter for modulating the resulting material properties. Here, we report that the edge states of twisted bilayer zigzag graphene nanoribbons (TBZGNRs) can be tuned with both the twist angle and the stacking offset. Strong edge state variations in the stacking region are first reve…
Janus dichalcogenide multilayers provide a paradigmatic platform to engineer electronic phenomena dominated by spin-orbit coupling. Their unique spin-orbit effects stem from local mirror symmetry breaking in each layer, which induces a colossal Rashba spin-orbit effect in comparison with the conventional dichalcogenide counterparts. Here we put forward twisted dichalcogenide bilayers as a simple platform to realize spin-orbit correlated states. We demonstrate the emergence of flat bands featuring strong spin-momentum locking and the emergence of non-collinear symmetry broken states when intera…
Graphene layers are known to stack in two stable configurations, namely ABA or ABC stacking, with drastically distinct electronic properties. Unlike the ABA stacking, little has been done to experimentally investigate the electronic properties of ABC graphene multilayers. Here, we report the first magneto optical study of a large ABC domain in a graphene multilayers flake, with ABC sequences exceeding 17 graphene sheets. The ABC-stacked multilayers can be fingerprinted with a characteristic electronic Raman scattering response, which persists even at room temperatures. Tracing the magnetic fie…
We address the intrinsic polarisation and screening of external electric field in a broad range of ordered and twisted configurations of multilayer graphene, using an ab initio approach combining density functional theory and the Wannier function formalism. We show that multilayer graphene is intrinsically polarized due to the crystal field effect, an effect that is often neglected in tight-binding models of twisted bilayer graphene and similar systems. This intrinsic polarization of the order of up to few tens of meVs has different out-of-plane alignments in ordered and twisted graphene multi…
Three-Dimensional Non-Foliated Fractional Quantum Hall Phases with Irrational Anyons in Twisted van der Waals Multilayers
Pohang University of Science and Technology（浦项科技大学）；Daegu Gyeongbuk Institute of Science and Technology (DGIST)（大邱庆北科学技术院）；Korea Advanced Institute of Science and Technology（韩国科学技术院）；Institute for Basic Science（基础科学研究院）
Using a numerical tight-binding approach based on the Chebyshev-Bogoliubov-de Gennes method we describe Josephson junctions made of multilayer graphene contacted by top superconducting gates. Both Bernal (ABA) and rhombohedral (ABC) stacking are considered and we find that the type of stacking has a strong effect on the proximity effect and the supercurrent flow. For both cases the pair amplitude shows a polarization between dimer and non-dimer atoms, being more pronounced for rhombohedral stacking. Even though the proximity effect in non-dimer sites is enhanced when compared to single layer g…
We study interlayer transport of multilayer graphenes in magnetic field with various stacking structures (AB, ABC, and AA types) by calculating the Hall and longitudinal conductivities as functions of Fermi energy. Their behavior depends strongly on the stacking structures and selection of the layers. The Hall conductivity between different layers is no longer quantized. Moreover, for AB stacking, the interlayer conductivity vanishes around zero energy with increasing layer separation, and shows negative values in particular cases. The fact that longitudinal interlayer conductivity suppressed …
Scanning tunneling microscopy (STM) images are obtained for the first time on few layer and twisted multilayer epitaxial graphene states synthesized on n+ 6H-SiC a-plane non-polar surface. The twisted graphene is determined to have a rotation angle of 5.4° between the top two layers, by comparing moiré patterns from stick and ball models of bilayer graphene to experimentally obtained images. Furthermore, the experimental moiré pattern shows dynamic behavior, continuously shuffling between two stable surface arrangements one bond length apart. The moiré pattern shifts by more than 1 nm, making …
We investigate the layer localization control of two-dimensional states in multilayer metal-organic frameworks (MOFs). For finite stackings of (NiC4S4)3 MOFs, the weak van der Waals coupling between adjacent layers leads to a Fermi level dependent distribution of the electronic states in the monolayers. Such distribution is reflected in the topological edge states of multilayer nanoribbons. Moreover, by applying an external electric field, parallel to the stacking direction, the spacial localization of the electronic states can be controlled for a chosen Fermi energy. This localization behavio…
Peeling, shearing, and sliding are important mechanical phenomena in van der Waals solids. However, theoretically they have been studied mostly using minimal periodic cells and in the context of accurate quantum simulations. Here, we investigate the peeling of large-scale multilayer graphene stacks with varying thicknesses, stackings, and peeling directions by using classical molecular dynamics simulations with a registry-dependent interlayer potential. Simulations show that, while at large scale the peeling proceeds smoothly, at small scale the registry shifts and sliding patterns of the laye…
Abstract: We report on emergence of an abnormal electronic polarization in twisted double bilayer WSe2 in antiparallel interface stacking geometry, where local centrosymmetry of atomic registries at the twist interface does not favor the spontaneous electronic polarizations as recently observed in the parallel interface stacking geometry. The unconventional ferroelectric behaviors probed by electronic transport measurement occur at half filling insulating states at 1.5 K and gradually disappear at about 40 K. Single band Hubbard model based on the triangular moiré lattice and the interlayer ch…
Twisted bilayers of nodal superconductors were recently proposed as a promising platform to host superconducting phases that spontaneously break time-reversal symmetry. Here we extend this analysis to twisted multilayers, focusing on two high-symmetry stackings with alternating ($\pm θ$) and constant ($θ$) twist angles. In analogy to alternating-twist multilayer graphene, the former can be mapped to twisted bilayers with renormalized interlayer couplings, along with a remnant gapless monolayer when the number of layers $L$ is odd. In contrast, the latter exhibits physics beyond twisted bilayer…
We construct a continuum model of twisted trilayer graphene using {\it ab initio} density-functional-theory calculations, and apply it to address twisted trilayer electronic structure. Our model accounts for moiré variation in site energies, hopping between outside layers and within layers. We focus on the role of a mirror symmetry present in ABA graphene trilayers with a middle layer twist. The mirror symmetry is lost intentionally when a displacement field is applied between layers, and unintentionally when the top layer is shifted laterally relative to the bottom layer. We use two band stru…
The advent of topological phases of matter revealed a variety of observed boundary phenomena, such as chiral and helical modes found at the edges of two-dimensional (2D) topological insulators. Antichiral states in 2D semimetals, i.e., copropagating edge modes on opposite edges compensated by a counterpropagating bulk current, are also predicted, but, to date, no realization of such states in a solid-state system has been found. Here, we put forward a procedure to realize antichiral states in twisted van der Waals multilayers, by combining the electronic Dirac-cone spectra of each layer throug…
We propose a generalized Peierls substitution method in conjunction with the tight-binding model to explore the magnetic quantization and quantum Hall effect in twisted multilayer graphene under a magnetic field. The Bloch-basis tight-binding Hamiltonian is constructed for large twist angle while a simplified tight-binding model is employed for the magic angle. We investigate extensively the band structures, Landau levels (LLs), and quantum Hall conductivity (QHC) of twisted bilayer graphene and twisted double bilayer graphene, as well as their dependence on the twist angle. Comparison between…
Interlayer interactions perturb the electronic structure of two-dimensional materials and lead to new physical phenomena, such as van Hove singularities and Hofstadter's butterfly pattern. Silicene, the recently discovered two-dimensional form of silicon, is quite unique, in that silicon atoms adopt competing <i>sp</i><sup>2</sup> and <i>sp</i><sup>3</sup> hybridization states leading to a low-buckled structure promising relatively strong interlayer interaction. In multilayer silicene, the stacking order provides an important yet rarely explored degree of freedom for tuning its electronic stru…
Stacking domain boundaries occur in Van der Waals heterostacks whenever there is a twist angle or lattice mismatch between subsequent layers. Not only can these domain boundaries host topological edge states, imaging them has been instrumental to determine local variations in twisted bilayer graphene. Here, we analyse the mechanisms causing stacking domain boundary contrast in Bright Field Low-Energy Electron Microscopy (BF-LEEM) for both graphene on SiC, where domain boundaries are caused by strain and for twisted few layer graphene. We show that when domain boundaries are between the top two…
We study the effect of vertical electric field (E-field) on the electronic properties of multilayer graphene. We show that the effective mass, electron velocity and density-of-state of a bilayer graphene are modified under the E-field. We also study the transformation of the band structure of multilayer graphenes. E-field induces finite (zero) bandgap in the even (odd)-layer ABA-stacking graphene. On the other hand, finite bandgap is induced in all ABC-stacking graphene. We also identify the optimum E-field to obtain the maximum bandgap in the multilayer graphenes. Finally we compare our resul…
Twisted graphene multilayers provide tunable platforms to engineer flat bands and exploit the associated strongly correlated physics. The two-dimensional nature of these systems makes them suitable for encapsulation by materials that break specific symmetries. In this context, recently discovered two-dimensional helimagnets, such as the multiferroic monolayer NiI$_2$, are specially appealing for breaking time-reversal and inversion symmetries due to their nontrivial spin textures. Here we show that this spin texture can be imprinted on the electronic structure of twisted bilayer graphene by pr…
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\…
We present an analytical model to study the electronic properties, including full band structure, low energy dispersions around the Dirac point and density of states of the ABC-stacking $N$-layer graphene (ABCNLG). An ABCNLG can be simulated by a linear atomic chain with $2N$ atoms. With only nearest-neighbor inter- and intra-layer hopping integrals taken into account, the Hamiltonian representation is a complex $2N \times 2N$ tridiagonal matrix $H_0$. Through a unitary transformation, we can reduce the $2N \times 2N$ Hamiltonian matrix into two real $N \times N$ tridiagonal matrices $\mathbb{…
Trilayer graphene with a twisted middle layer has recently emerged as a new platform exhibiting correlated phases and superconductivity near its magic angle. A detailed characterization of its electronic structure in the parameter space of twist angle $θ$, interlayer potential difference $Δ$, and top-bottom layer stacking $τ$ reveals that flat bands with large Coulomb energy vs bandwidth $U/W > 1$ are expected within a range of $\pm 0.2^{\circ}$ near $θ\simeq1.5^{\circ}$ and $θ\simeq1.2^{\circ}$ for $τ_{\rm AA}$ top-bottom layer stacking, between a wider $1^{\circ} \sim 1.7^{\circ}$ range for …
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…
We uncover a new type of magic-angle phenomena when an AA-stacked graphene bilayer is twisted relative to another graphene system with band touching. In the simplest case this constitutes a trilayer system formed by an AA-stacked bilayer twisted relative to a single layer of graphene. We find multiple anisotropic Dirac cones coexisting in such twisted multilayer structures at certain angles, which we call "Dirac magic." We trace the origin of Dirac magic angles to the geometric structure of the twisted AA-bilayer Dirac cones relative to the other band-touching spectrum in the moiré reciprocal …
Fractional Chern insulators in alternating twisted multilayer MoTe$_{2}$
Huazhong University of Science and Technology（华中科技大学）；Wuhan National High Magnetic Field Center, Huazhong University of Science and Technology（华中科技大学武汉国家高能磁场中心）；Hubei Fundamental Research Center for Physics（湖北省物理基础研究中心）
Realization of high-quality van der Waals (vdW) heterostructures with tailored properties by stacking two-dimensional (2D) layers requires atomically clean interfaces. Because of strong adhesion between the constituent layers, the vdW forces could drive trapped contaminants together into submicron-size bubbles, which leaves large interfacial areas atomically clean. Such a phenomenon is dubbed self-cleaning mechanism in 2D systems. Here, we demonstrate the breakdown of self-cleaning mechanism for nanoscale interfacial bubbles in tiny-angle twisted bilayer graphene (TBG). In the tiny-angle TBG, …
