Revealing flat bands and hybridization gaps in a twisted bilayer graphene device with microARPES
Zhihao Jiang, Kimberly Hsieh, Alfred J. H. Jones, Paulina Majchrzak, Chakradhar Sahoo, Kenji Watanabe, Takashi Taniguchi, Jill A. Miwa, Yong P. Chen, Søren Ulstrup
Controlling the electronic structure of two-dimensional materials using the combination of twist angle and electrostatic doping is an effective means to induce emergent phenomena. In bilayer graphene with an interlayer twist angle near the magic angle, the electronic dispersion is strongly modified by a manifold of hybridizing moiré Dirac cones leading to flat band segments with strong electronic correlations. Numerous technical challenges arising from spatial inhomogeneity of interlayer interactions, twist angle and device functionality have so far limited momentum-resolved electronic structure measurements of these systems to static conditions. Here, we present a detailed characterization of the electronic structure exhibiting miniband dispersions for twisted bilayer graphene, near the magic angle, integrated in a functional device architecture using micro-focused angle-resolved photoemission spectroscopy. The optimum conditions for visualizing the miniband dispersion are determined by exploiting the spatial resolution and photon energy tunability of the light source and applied to extract a hybridization gap size of $(0.14 \pm 0.03)$~eV and flat band segments extending across a moiré mini Brillouin zone. \textit{In situ} electrostatic gating of the sample enables significant electron-doping, causing the conduction band states to shift below the Fermi energy. Our work emphasizes key challenges in probing the electronic structure of magic angle bilayer graphene devices and outlines conditions for exploring the doping-dependent evolution of the dispersion that underpins the ability to control many-body interactions in the material.
The incommensurate 30$^{\circ}$ twisted bilayer graphene (BG) possesses both relativistic Dirac fermions and quasiperiodicity with 12-fold rotational symmetry arising from the interlayer interaction [\href{https://science.sciencemag.org/content/361/6404/782}{Ahn et al., Science \textbf{361}, 782 (2018)} and \href{https://www.pnas.org/content/115/27/6928}{Yao et al., Proc. Natl. Acad. Sci. \textbf{115}, 6928 (2018)}]. Understanding how the interlayer states interact with each other is of vital importance for identifying and subsequently engineering the quasicrystalline order in the layered stru…
Band structure determines the motion of electrons in a solid, giving rise to exotic phenomena when properly engineered. Drawing an analogy between electrons and photons, artificially designed optical lattices indicate the possibility of a similar band modulation effect in graphene systems. Yet due to the fermionic nature of electrons, modulated electronic systems promise far richer categories of behaviors than those found in optical lattices. Here, we uncovered a strong modulation of electronic states in bilayer graphene subject to periodic potentials. We observed for the first time the hybrid…
Moiré superlattices serve as a playground for emerging phenomena, such as localization of band states, superconductivity, and localization of excitons. These superlattices are large and are often modeled in the zero angle limit, which obscures the effect of finite twist angles. Here, by means of first-principles calculations we quantify the twist-angle dependence of the moiré potential in the MoS$_2$ homobilayer and identify the contributions from the constituent elements of the moiré potential. Furthermore, by considering the zero-angle limit configurations, we show that the moiré potential i…
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 study the electronic spin relaxation effect in the hole-doped monolayer and bilayer transition-metal dichalcogenides in the presence of the crystal defects. We consider realistic models of the lattice vacancy and actually estimate the spin relaxation rate using the multi-orbital tight-binding model. In the monolayer, the spin-relaxation time is found to be extremely long compared to the momentum relaxation time, and this is attributed to the fact that the spin hybridization in the band structure is suppressed by the mirror reflection symmetry. The bilayer TMD has a much shorter spin relaxat…
We employ magnetocapacitance and far-infrared spectroscopy techniques to study the spectrum of the double-layer electron system in a parabolic quantum well with a narrow tunnel barrier in the centre. For gate-bias-controlled asymmetric electron density distributions in this soft two-subband system we observe both individual subband gaps and double layer gaps at integer filling factor $ν$. The bilayer gaps are shown to be either trivial common for two subbands or caused by hybridization of electron subbands in magnetic field. We describe the observed hybrid gaps at $ν=1$ and $ν=2$ within a simp…
Electron optics in the solid state promises new functionality in electronics through the possibility of realizing micrometer-sized interferometers, lenses, collimators and beam splitters that manipulate electrons instead of light. Until now, however, such functionality has been demonstrated exclusively in one-dimensional devices, such as in nanotubes, and in graphene-based devices operating with p-n junctions. In this work, we describe a novel mechanism for realizing electron optics in two dimensions. By studying a two-dimensional Fabry-Pérot interferometer based on a resonant cavity formed in…
We theoretically investigate silicon doped bilayer graphene, Si-BLG, with different stoichiometry of Si-BLG structures. The dangling bonds of C-Si atoms are found at low concentration ratio of Si atoms inducing sp$^3$-hybridization of buckled pattern in the structure. The Si-BLG with dangling bonds revel strong mechanical response at low strain of a uniaxial load, and the fracture strain is seen at low strain ratio. The sp$^3$-hybridization forms a small bandgap which induces an intermediate thermal and optical response of the system. In contrast, at higher Si concentration ratio, the Young mo…
Excitons in bilayer transition metal dichalcogenides (2L-TMDs) are Coulomb-bound electron/hole pairs that can be viewed as broadly tunable analogs of atomic or molecular systems. Here, we study the properties of 2L-TMD excitons under strong electric field. To overcome the field limit, reached in previous experiments, we developed a new organic/inorganic molecular gating technique. Our approach allows reaching the field > 0.27 V nm-1, about twice higher than previously available. Under this field inter and intra-layer excitonic are brought into an energetic resonance, allowing us to discover ne…
Layer stacking and crystal lattice symmetry play important roles in the band structure and the Landau levels of multilayer graphene. ABA-stacked trilayer graphene possesses mirror-symmetry-protected monolayer-like and bilayer-like band structures. Broken mirror symmetry by a perpendicular electric field therefore induces hybridization between these bands and various quantum Hall phases emerge. We experimentally explore the evolution of Landau levels in ABA-stacked trilayer graphene under electric field. We observe a variety of valley and orbital dependent Landau level evolutions. These evoluti…
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.
The introduction of 'twist' or relative rotation between two atomically thin van der Waals (vdW) membranes gives rise to periodic Moire potential, leading to a substantial altercation of the band structure of the planar assembly. While most of the recent experiments primarily focus on the electronic-band hybridization by probing in-plane transport properties, here we report out-of-plane thermoelectric measurements across the van der Waals gap in twisted bilayer graphene (tBLG), which exhibits an interplay of twist-dependent inter-layer electronic and phononic hybridization. We show that at a l…
We theoretically study a possible topological superconductivity in the interacting two layers of Rashba systems, which can be fabricated by the hetero-structures of semiconductors and oxides. The hybridization, which induces the gap in the single particle dispersion, and the electron-electron interaction between the two layers leads to the novel phase diagram of the superconductivity. It is found that the topological superconductivity {\it without breaking time-reversal symmetry} is realized when (i) the Fermi energy is within the hybridization gap, and (ii) the inter-layer interaction is repu…
Topological insulators (TIs) and graphene present two unique classes of materials which are characterized by spin polarized (helical) and non-polarized Dirac-cone band structures, respectively. The importance of many-body interactions that renormalize the linear bands near Dirac point in graphene has been well recognized and attracted much recent attention. However, renormalization of the helical Dirac point has not been observed in TIs. Here, we report the experimental observation of the renormalized quasi-particle spectrum with a skewed Dirac cone in a single Bi bilayer grown on Bi2Te3 subst…
Non-covalent functionalization via physisorption of organic molecules provides a scalable approach for modifying the electronic structure of graphene while preserving its excellent carrier mobilities. Here we investigated the physisorption of long-chain acenes, namely, hexacene and its fluorinated derivative perfluorohexacene, on bilayer graphene for tunable graphene devices using first principles methods. We find that the adsorption of these molecules leads to the formation of localized states in the electronic structure of graphene close to its Fermi level, which could be readily tuned by an…
Using a multiscale computational approach, we probe the origin and evolution of ultraflatbands in moiré superlattices of twisted bilayer MoS$_2$, a prototypical transition metal dichalcogenide. Unlike twisted bilayer graphene, we find no unique magic angles in twisted bilayer MoS$_2$ for flatband formation. Ultraflatbands form at the valence band edge for twist angles ($θ$) close to 0$^\circ$ and at both the valence and conduction band edges for $θ$ close to 60$^\circ$, and have distinct origins. For$ θ$ close to 0$^\circ$, inhomogeneous hybridization in the reconstructed moiré superlattice is…
The HOMO-LUMO gaps of the bilayer fullerene onions were investigated. For this purpose, the HOMO and LUMO energies were calculated for the isolated fullerenes using the parametrization of the tight binding method with the Harrison-Goodwin modification. Next, the difference of the Fermi levels of the outer and inner shell was calculated by considering the hybridization of the orbitals on the base of the geometric parameters. The results were obtained by the combination of these calculations.
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…
Recent advances in the field of vertically stacked 2D materials have revealed a rich exciton landscape. In particular, it has been demonstrated that out-of-plane electrical fields can be used to tune the spectral position of spatially separated interlayer excitons. Other studies have shown that there is a strong hybridization of exciton states, resulting from the mixing of electronic states in both layers. However, the connection between the twist-angle dependent hybridization and field-induced energy shifts has remained in the dark. Here, we investigate on a microscopic footing the interplay …
The existence of strong trigonal warping around the K point for the low energy electronic states in multilayer (N$\geq$2) graphene films and graphite is well established. It is responsible for phenomena such as Lifshitz transitions and anisotropic ballistic transport. The absolute orientation of the trigonal warping with respect to the center of the Brillouin zone is however not agreed upon. Here, we use quasiparticle scattering experiments on a gated bilayer graphene/hexagonal boron nitride heterostructure to settle this disagreement. We compare Fourier transforms of scattering interference m…
We study local moment formation for adatoms on bilayer graphene (BLG) within a mean-field theory of the Anderson impurity model. The wavefunctions of the BLG electrons induce strong particle-hole asymmetry and band dependence of the hybridization, which is shown to result in unusual features in the impurity model phase diagram. We also study the effect of varying the chemical potential, as well as varying an electric field perpendicular to the bilayer; the latter modifies the density of states of electrons in BLG and, more significantly, shifts the impurity energy. We show that this leads to r…
Monolayer WTe2 stripes are quantum spin Hall (QSH) insulators. Density functional theory was used for investigating the electronic properties of the stripes and steps in bilayer Td-WTe2. For the stripes oriented along the dimer chains of W atoms (x direction), the hybridization between the two layers suppresses the QSH states. However, the QSH nature can be recovered by forming a step, depending on the atomic structure of the step. Conversely, the stripes and steps along the y direction maintain the QSH states. These findings can expand the application range of the QSH states in WTe2.
Two-dimensional layered materials offer the possibility to create artificial vertically stacked structures possessing an additional degree of freedom - $the$ $interlayer$ $twist$. We present a comprehensive optical study of artificially stacked bilayers (BLs) MoS$_2$ encapsulated in hexagonal BN with interlayer twist angle ranging from 0 to 60 degrees using Raman scattering and photoluminescence spectroscopies. It is found that the strength of the interlayer coupling in the studied BLs can be estimated using the energy dependence of indirect emission versus the A$_\textrm{1g}$-E$_\textrm{2g}^1…
The structure optimization, phonon, and ab initio finite temperature molecular dynamics calculations have been performed to predict that bilayer silicene has stable structure with AB stacking geometry and is more favorable energetically to synthesize than monolayer silicene, a two-dimensional honeycomb lattice with buckled geometry. Marvellously, its electronic bands show that the charge carriers behave like relativistic Dirac fermions with linear energy dispersions near the K points. An insightful analysis has been presented to understand the low-energy electronic excitations based on tight-b…
Anderson impurity problem is considered for a graphene bilayer subject to a gap-opening bias. In-gap localized states are produced even when the impurity level overlaps with the continuum of band electrons. The effect depends strongly on the polarity of the applied bias as long as hybridization with the impurity occurs within a single layer. For an impurity level inside the conduction band a positive bias creates the new localized in-gap state. A negative bias does not produce the same result and leads to a simple broadening of the impurity level. The implications for transport are discussed i…
A major theoretical challenge of studying twisted transition metal dichalcogenide (TMD) bilayers is that the unit cell of such structures is very large and therefore difficult to address using first-principles methods. However, twisted TMD bilayers form moiré patterns, which consist of regions of commensurate stacking, either smoothly interpolated into one another or separated by sharp domain walls. In this paper, we study twisted TMD bilayers by studying the properties of the constituent commensurate structures. Using density functional theory (DFT), we compute band structures for commensurat…
Being used in optoelectronic devices as ultra-thin conductor-insulator junctions, detailed investigations are needed about how exactly h-BN and graphene hybridize. Here, we present a comprehensive ab initio study of hot carrier dynamics governed by electron-phonon scattering at the h-BN/graphene interface, using graphite (bulk), monolayer and bilayer graphene as benchmark materials. In contrast to monolayer graphene, all multilayer structures possess low-energy optical phonon modes that facilitate carrier thermalization. We find that the h-BN/graphene interface represents an exception with com…
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…
We theoretically demonstrate that a system formed by two coupled graphene sheets enables a negative damping regime wherein graphene plasmons are pumped by a DC current. This effect is triggered by electrons drifting through one of the graphene sheets and leads to the spontaneous light emission (spasing) and wave instabilities in the mid-infrared range. It is shown that there is a deep link between the drift-induced instabilities and wave instabilities in moving media, as both result from the hybridization of oscillators with oppositely signed frequencies. With a thickness of few nanometers and…
30$^{\circ}$ twisted bilayer graphene demonstrates the quasicrystalline electronic states with 12-fold symmetry. These states are however far away from the Fermi level, which makes conventional Dirac fermion behavior dominating the low energy spectrum in this system. By using tight-binding approximation, we study the effect of external pressure and electric field on the quasicrystalline electronic states. Our results show that by applying the pressure perpendicular to graphene plane one can push the quasicrystalline electronic states towards the Fermi level. Then, the electron or hole doping o…
Twisted bilayer graphene (TwBLG) is one of the simplest van der Waals heterostructures, yet it yields a complex electronic system with intricate interplay between moiré physics and interlayer hybridization effects. We report on electronic transport measurements of high mobility small angle TwBLG devices showing clear evidence for insulating states at the superlattice band edges, with thermal activation gaps several times larger than theoretically predicted. Moreover, Shubnikov-de Haas oscillations and tight binding calculations reveal that the band structure consists of two intersecting Fermi …
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-…
We investigate the electronic band structure and the proximity exchange effect in bilayer graphene on a family of ferromagnetic multilayers Cr$_2$X$_2$Te$_6$, X=Ge, Si, and Sn, with first principles methods. In each case the intrinsic electric field of the heterostructure induces an orbital gap on the order of 10 meV in the graphene bilayer. The proximity exchange is strongly band dependent. For example, in the case of Cr$_2$Ge$_2$Te$_6$, the low-energy valence band of bilayer graphene has exchange splitting of 8 meV, while the low energy conduction band's splitting is 30 times less (0.3 meV).…
Moiré excitons are emergent optical excitations in 2D semiconductors with deep moiré superlattice potentials. While these excitations have been realized in several platforms, a system with dynamically tunable moiré potential to tailor the moiré exciton properties is yet to be realized. Here, we present a continuously tunable moiré potential in a monolayer WSe2 that is enabled by its proximity to twisted bilayer graphene (TBG) near the magic-angle. Due to its flat electronic bands, charge distribution is highly localized and forms a triangular lattice in TBG. Tuning the local charge density via…
We study a magnetic impurity intercalated in bilayer graphene. A representative configuration generates a hybridization function with strong dependence on the conduction-electron energy, including a full gap with one hard and one soft edge. Shifts of the chemical potential via gating or doping drive the system between non-Kondo (free-moment) and Kondo-screened phases, with strong variation of the Kondo scale. Quantum phase transitions near the soft edge are of Kosterlitz-Thouless type, while others are first order. Near the hard edge, a bound-state singlet appears inside the gap; although of s…
We theoretically show that the three-dimensional (3D) topological insulator (TI)/thin-film ferromagnetic metal (FMM) bilayer structure is possible to be a quantum anomalous Hall (QAH) insulator with a wide global band gap. Studying the band structure and the weight distributions of eigenstates, we demonstrate that the attachment of a metallic thin-film on the 3DTI can shift the topologically non-trivial state into the metal layers due to the hybridization of bands around the original Dirac point. By introducing the magnetic exchange interaction in the thin-film layers, we compute the anomalous…
The First Magic Angle Beyond the Chiral Limit in Twisted Bilayer Graphene
Universidad Nacional Autónoma de México (UNAM)（墨西哥国立自治大学）；NYU Shanghai（纽约大学上海分校）；NYU-ECNU Institute of Physics at NYU Shanghai（纽约大学上海纽约大学物理研究所）；Hainan University（海南大学）；IMDEA Nanoscience（IMDEA纳米科学研究所）；Donostia International Physics Center（圣塞巴斯蒂安国际物理中心）
We construct a heavy fermion representation for twisted bilayer graphene (TBG) systems. Two local orbitals (per spin/valley) are analytically found, which are exactly the maximally localized zero modes of the continuum Hamiltonian near the AA-stacking center. They have similar properties to the Wannier functions in [arXiv:2111.05865v2], but also have a clear interpretation as the zeroth pseudo Landau levels (ZLL) of Dirac fermions under the uniform strain field created by twisting [arXiv:1810.03103v3]. The electronic states of TBG can be viewed as the hybridization between these ZLL orbitals a…
Electronic Reconstruction at the Quasicrystal-Moiré Crossover in Twisted Bilayer Graphene
National Cheng Kung University（国立成功大学）；Center for Quantum Frontiers of Research & Technology (QFort), National Cheng Kung University（国立成功大学量子前沿研究与技术中心）；National Taiwan University（国立台湾大学）；Center for Condensed Matter Sciences, National Taiwan University（国立台湾大学凝聚态科学中心）；Center of Atomic Initiative for New Materials, National Taiwan University（国立台湾大学原子级新材料创新中心）
Filling factor $ν=1$ bilayer electron systems in the quantum Hall regime have an excitonic-condensate superfluid ground state when the layer separation $d$ is less than a critical value $d_c$. On a quantum Hall plateau current injected and removed through one of the two layers drives a dissipationless edge current that carries parallel currents, and a dissipationless bulk supercurrent that carries opposing currents in the two layers. In this paper we discuss the theory of finite supercurrent bilayer states, both in the presence and in the absence of symmetry breaking inter-layer hybridization.…
Magic-angle twisted bilayer graphene (MATBG) is notable as a highly tunable platform for investigating strongly correlated phenomena such as high-$T_c$ superconductivity and quantum spin liquids, due to easy control of doping level through gating and sensitive dependence of the magic angle on hydrostatic pressure. Experimental observations of correlated insulating states, unconventional superconductivity and ferromagnetism in MATBG indicate that this system exhibits rich exotic phases. In this work, using density functional theory calculations in conjunction with the effective screening medium…
The electronic states of a single Bi(111) bilayer and its edges, suggested as a two dimensional topological insulator, are investigated by scanning tunneling spectroscopy (STS) and first-principles calculations. Well-ordered bilayer films and islands with zigzag edges are grown epitaxially on a cleaved Bi$_{2}$Te$_{2}$Se crystal. The calculation shows that the band gap of the Bi bilayer closes with a formation of a new but small hybridization gap due to the strong interaction between Bi and Bi$_{2}$Te$_{2}$Se. Nevertheless, the topological nature of the Bi bilayer and the topological edge stat…
Moire superlattices in twisted transition metal dichalcogenide bilayers have emerged as a rich platform for exploring strong correlations using optical spectroscopy. Despite observation of rich Mott-Wigner physics stemming from an interplay between the periodic potential and Coulomb interactions, the absence of tunnel coupling induced hybridization of electronic states ensured a classical layer degree of freedom in these experiments. Here, we investigate a MoSe$_2$ homobilayer structure where inter-layer coherent tunnelling and layer-selective optical transitions allow for electric field contr…
One-Dimensional Electronic States in a Moiré Superlattice of Twisted Bilayer WTe2
Osaka University（大阪大学）；Kyushu University（九州大学）；The University of Tokyo（东京大学）；Stony Brook University（石溪大学）；Japan Advanced Institute of Science and Technology（日本科学技术高级学院）
