Search

Twisted hexagonal boron nitride (thBN) exhibits emergent ferroelectricity due to the formation of moir\'e superlattices with alternating AB and BA domains. These domains possess electric dipoles, leading to a periodic electrostatic potential that can be imprinted onto other 2D materials placed in its proximity. Here we demonstrate the remote imprinting of moir\'e patterns from twisted hexagonal boron nitride (thBN) onto monolayer MoSe2 and investigate the resulting changes in the exciton properties. We confirm the imprinting of moir\'e patterns on monolayer MoSe2 via proximity using Kelvin probe force microscopy (KPFM) and hyperspectral photoluminescence (PL) mapping. By developing a technique to create large ferroelectric domain sizes ranging from 1 {\mu}m to 8.7 {\mu}m, we achieve unprecedented potential modulation of 387 +- 52 meV. We observe the formation of exciton polarons due to charge redistribution caused by the antiferroelectric moir\'e domains and investigate the optical property changes induced by the moir\'e pattern in monolayer MoSe2 by varying the moir\'e pattern size down to 110 nm. Our findings highlight the potential of twisted hBN as a platform for controlling the optical and electronic properties of 2D materials for optoelectronic and valleytronic applications.

Local interlayer charge polarization of twisted bilayer hexagonal boron nitride (t2BN) is calculated and parametrized as a function of twist angle and perpendicular electric fields through tight-binding calculations on lattice relaxed geometries Lattice relaxations tend to increase the bandwidth of the nearly flat bands, where widths smaller than 1 meV are expected for angle less than 1.08 degree for parallel BN/BN alignment, and for angle less than 1.5 degree for the antiparallel BN/NB alignment. Local interlayer charge polarization maxima of 2.6 pC/m corresponding are expected at the AB and BA stacking sites of BN/BN aligned t2BN in the long moire period limit for angle less than 1 degree, and evolves non-monotonically with a maximum of 3.5 pC/m at angle equal to 1.6 degree before reaching 2 pC/m for angle equal to 6 degree. The electrostatic potential maxima due to the t2BN are overall enhanced by 20 percentage with respect to the rigid system assuming potential modulation depths of up to 300 mV near its surface. In BN/BN aligned bilayers the relative areas of the AB or BA local stacking regions can be expanded or reduced through a vertical electric field depending on its sign.

We study the electronic structure of alternating-twist tetralayer graphene, especially near its magic angle $\theta = 1.75^\circ$, for different AA, AB, and SP sliding geometries at their middle interface that divides two twisted bilayer graphenes. This sliding dependence is shown for the bandwidths, band gaps, and $K$-valley Chern numbers of the lowest-energy valence and conduction bands as a function of twist angle and interlayer potential difference. Our analysis reveals that the AA sliding is most favorable for narrow bands and gaps, and the AB sliding is most prone to developing finite valley Chern numbers. We further analyze the linear longitudinal optical absorptions as a function of photon energy and the absorption map in the moir\'{e} Brillouin zone for specific transition energies. A self-consistent Hartree calculation reveals that the AA system's electronic structure is the most sensitive to variations in carrier density., Comment: 15 pages, 11 figures

Superlattices from twisted graphene mono- and bi-layer systems give rise to on-demand many-body states such as Mott insulators and unconventional superconductors. These phenomena are ascribed to a combination of flat bands and strong Coulomb interactions. However, a comprehensive understanding is lacking because the low-energy band structure strongly changes when the electron filling is varied. Here, we gain direct access to the filling-dependent low energy bands of twisted bilayer graphene (TBG) and twisted double bilayer graphene (TDBG) by applying micro-focused angle-resolved photoemission spectroscopy to in situ gated devices. Our findings for the two systems are in stark contrast: The doping dependent dispersion for TBG can be described in a simple model, combining a filling-dependent rigid band shift with a many-body related bandwidth change. In TDBG, on the other hand, we find a complex behaviour of the low-energy bands, combining non-monotonous bandwidth changes and tuneable gap openings. Our work establishes the extent of electric field tunability of the low energy electronic states in twisted graphene superlattices and can serve to underpin the theoretical understanding of the resulting phenomena., Comment: 26 pages, 4 main figures and 7 supplementary figures

Hexagonal boron nitride ($\it h$-BN) exhibits dominant $\pi$-bands near the Fermi level, similar to graphene. However, unlike graphene, where tight-binding (TB) models accurately reproduce band edges near the $K$ and $K^{\prime}$ points in the Brillouin zone, a wider bandgap in $\it h$-BN necessitates capturing the band edges at both the $K$ and $M$ points for precise bandgap calculations. We present effective TB models derived from $\it ab initio$ calculations using maximally localized Wannier functions (MLWFs) centered on boron and nitrogen sites. These models consider hopping terms of up to four distant neighbors and achieve excellent agreement with $\it ab initio$ results near the $K$ and $M$ points. Furthermore, we compare the band structures from our simplified models with those obtained from $\it ab initio$ calculations and the full tight-binding model to assess their accuracy. To account for the effects of strains, we introduce fitting parametrizations that relate the hopping parameters of the effective TB model to the lattice constant and interlayer distance. Additionally, we utilize the two-center approximation to calculate the interlayer hopping energies based on the relative distances between sublattices to generalize the interlayer hopping parameters across different stacking configurations. We demonstrate the effectiveness of this method by comparing the electronic structure of zero-twist and twisted $\it h$-BN systems with $\it ab initio$ calculations.

Twisted bilayer graphene (tBLG) provides a fascinating platform for engineering flat bands and inducing correlated phenomena. By designing the stacking architecture of graphene layers, twisted multilayer graphene can exhibit different symmetries with rich tunability. For example, in twisted monolayer-bilayer graphene (tMBG) which breaks the C2z symmetry, transport measurements reveal an asymmetric phase diagram under an out-of-plane electric field, exhibiting correlated insulating state and ferromagnetic state respectively when reversing the field direction. Revealing how the electronic structure evolves with electric field is critical for providing a better understanding of such asymmetric field-tunable properties. Here we report the experimental observation of field-tunable dichotomic electronic structure of tMBG by nanospot angle-resolved photoemission spectroscopy (NanoARPES) with operando gating. Interestingly, selective enhancement of the relative spectral weight contributions from monolayer and bilayer graphene is observed when switching the polarity of the bias voltage. Combining experimental results with theoretical calculations, the origin of such field-tunable electronic structure, resembling either tBLG or twisted double-bilayer graphene (tDBG), is attributed to the selectively enhanced contribution from different stacking graphene layers with a strong electron-hole asymmetry. Our work provides electronic structure insights for understanding the rich field-tunable physics of tMBG., Comment: 4 figures

Rhombohedral multilayer graphene (RnG) featuring partially flat bands has emerged as an important platform to probe strong Coulomb correlation effects. Theoretical consideration of local electron-electron interactions are of particular importance for electronic eigenstates with a tendency to spatially localize. We present a method to incorporate mean-field electron-electron interaction corrections in the tight-binding hopping parameters of the band Hamiltonian within the extended Hubbard model that incorporates ab initio estimates of on-site ($U$) and inter-site ($V$) Hubbard interactions for the $\pi$ bands of RnG. Our Coulomb-interaction renormalized band structures feature electron-hole asymmetry, band flatness, band gap, and anti-ferromagnetic ground states in excellent agreement with available experiments for $n \geq 4$. We reinterpret the putative gaps proposed in $n=3$ systems in terms of shifting electron and hole density of states peaks depending on the range of the Coulomb interaction models., Comment: 8 pages, 5 figures

We report intriguing and hitherto overlooked low-field room temperature extremely large magnetoresistance (XMR) patterns in graphene/hexagonal boron nitride (h-BN) superlattices that emerge due to the existence of open orbits within each miniband. This finding is set against the backdrop of the experimental discovery of the Hofstadter butterfly in moir superlattices, which has sparked considerable interest in the fractal quantum Hall regime. To cope with the challenge of deciphering the low magnetic field dynamics of moir minibands, we utilize a novel semi-classical calculation method, grounded in zero-field Fermi contours, to predict the nontrivial behavior of the Landau-level spectrum. This is compared with fully quantum simulations, enabling an in-depth and contrasted analysis of transport measurements in high-quality graphene-hBN superlattices. Our results not only highlight the primary observation of the open-orbit induced XMR in this system but also shed new light on other intricate phenomena. These include the nuances of single miniband dynamics, evident through Lifshitz transitions, and the complex interplay of semiclassical and quantum effects between these minibands. Specifically, we document transport anomalies linked to trigonal warping, a semiclassical deviation from the expected linear characteristics of Landau levels, and magnetic breakdown phenomena indicative of quantum tunneling, all effects jointly contributing to the intricacies of a rich electronic landscape uncovered at low magnetic fields., Comment: 5 figures

In Bernal-stacked bilayer graphene (BBG), the Landau levels give rise to an intimate connection between valley and layer degrees of freedom. Adding a moir\'e superlattice potential enriches the BBG physics with the formation of topological minibands - potentially leading to tunable exotic quantum transport. Here, we present magnetotransport measurements of a high-quality bilayer graphene-hexagonal boron nitride (hBN) heterostructure. The zero-degree alignment generates a strong moir\'e superlattice potential for the electrons in BBG and the resulting Landau fan diagram of longitudinal and Hall resistance displays a Hofstadter butterfly pattern with a high level of detail. We demonstrate that the intricate relationship between valley and layer degrees of freedom controls the topology of moir\'e-induced bands, significantly influencing the energetics of interacting quantum phases in the BBG superlattice. We further observe signatures of field-induced correlated insulators, helical edge states and clear quantizations of interaction-driven topological quantum phases, such as symmetry broken Chern insulators.

Interactions among charge carriers in graphene can lead to the spontaneous breaking of multiple degeneracies. When increasing the number of graphene layers following rhombohedral stacking, the dominant role of Coulomb interactions becomes pronounced due to the significant reduction in kinetic energy. In this study, we employ phonon-polariton assisted near-field infrared imaging to determine the stacking orders of tetralayer graphene devices. Through quantum transport measurements, we observe a range of spontaneous broken-symmetry states and their transitions, which can be finely tuned by carrier density n and electric displacement field D. Specifically, we observe a layer antiferromagnetic insulator at n = D = 0 with a gap of approximately 15 meV. Increasing D allows for a continuous phase transition from a layer antiferromagnetic insulator to a layer polarized insulator. By simultaneously tuning n and D, we observe isospin polarized metals, including spin-valley-polarized and spin-polarized metals. These transitions are associated with changes in Fermi surface topology and are consistent with the Stoner criteria. Our findings highlight the efficient fabrication of specially stacked multilayer graphene devices and demonstrate that crystalline multilayer graphene is an ideal platform for investigating a wide range of broken symmetries driven by Coulomb interactions.

We explore the direct to indirect band gap transitions in MX$_2$ (M= Mo/W, X= S/Se) transition metal dichalcogenides heterobilayers for different system compositions, strains, and twist angles based on first principles density functional theory calculations within the G$_0$W$_0$ approximation. The obtained band gaps that typically range between 1.4$-$2.0 eV are direct/indirect for different/same chalcogen atom systems and can often be induced through expansive/compressive biaxial strains of a few percent. A direct to indirect gap transition is verified for heterobilayers upon application of a finite 16$^{\circ}$ twist that weakens interlayer coupling. The large inter-layer exciton binding energies of the order of $\sim$~250~meV estimated by solving the Bethe-Salpeter equation suggest these systems are amenable to be studied through infrared and Raman spectroscopy., Comment: 10 pages, 6 figures

We show that rhombohedral four-layer graphene (4LG) nearly aligned with a hexagonal boron nitride (hBN) substrate often develops nearly flat isolated low energy bands with non-zero valley Chern numbers. The bandwidths of the isolated flatbands are controllable through an electric field and twist angle, becoming as narrow as $\sim10~$meV for interlayer potential differences between top and bottom layers of $|\Delta|\approx 10\sim15~$meV and $\theta \sim 0.5^{\circ}$ at the graphene and boron nitride interface. The local density of states (LDOS) analysis shows that the nearly flat band states are associated to the non-dimer low energy sublattice sites at the top or bottom graphene layers and their degree of localization in the moire superlattice is strongly gate tunable, exhibiting at times large delocalization despite of the narrow bandwidth. We verified that the first valence bands' valley Chern numbers are $C^{\nu=\pm1}_{V1} = \pm n$, proportional to layer number for $n$LG/BN systems up to $n = 8$ rhombohedral multilayers.

We investigate the total energies of spontaneous spin-valley polarized states in bi-, tri-, and tetralayer rhombohedral graphene where the long-range Coulomb correlations are accounted for within the random phase approximation. Our analysis of the phase diagrams for varying carrier doping and perpendicular electric fields shows that the exchange interaction between chiral electrons is the main driver of spin-valley polarization, while the presence of Coulomb correlations brings the flavor polarization phase boundaries to carrier densities close to the complete filling of the Mexican hat shape top at the Dirac points. We find that the tendency towards spontaneous spin-valley polarization is enhanced with the chirality of the bands and therefore with increasing number of layers., Comment: 10 pages, 5 figures

We study the commensuration torques and layer sliding energetics of alternating twist trilayer graphene (t3G) and twisted bilayer graphene on hexagonal boron nitride (t2G/BN) that have two superposed moire interfaces. Lattice relaxations for typical graphene twist angles of $\sim 1^{\circ}$ in t3G or t2G/BN are found to break the out-of-plane layer mirror symmetry, give rise to layer rotation energy local minima dips of the order of $\sim 10^{-1}$ meV/atom at double moire alignment angles, and have sliding energy landscape minima between top-bottom layers of comparable magnitude. Moire superlubricity is restored for twist angles as small as $\sim 0.03^\circ$ away from alignment resulting in suppression of sliding energies by several orders of magnitude of typically $\sim 10^{-4}$ meV/atom, hence indicating the precedence of rotation over sliding in the double moire commensuration process., Comment: 9 pages, 4 figures

We theoretically study the energy and optical absorption spectra of alternating twist multilayer graphene (ATMG) under a perpendicular electric field. We obtain analytically the low-energy effective Hamiltonian of ATMG up to pentalayer in the presence of the interlayer bias by means of first-order degenerate-state perturbation theory, and present general rules for constructing the effective Hamiltonian for an arbitrary number of layers. Our analytical results agree to an excellent degree of accuracy with the numerical calculations for twist angles $\theta \gtrsim 2.2^{\circ}$ that are larger than the typical range of magic angles. We also calculate the optical conductivity of ATMG and determine its characteristic optical spectrum, which is tunable by the interlayer bias. When the interlayer potential difference is applied between consecutive layers of ATMG, the Dirac cones at the two moir\'{e} Brillouin zone corners $\bar{K}$ and $\bar{K}'$ acquire different Fermi velocities, generally smaller than that of monolayer graphene, and the cones split proportionally in energy resulting in a step-like feature in the optical conductivity., Comment: 11 pages, 11 figures, 2 tables

New phases of matter can be stabilized by a combination of diverging electronic density of states, strong interactions, and spin-orbit coupling. Recent experiments in magic-angle twisted bilayer graphene (TBG) have uncovered a wealth of novel phases as a result of interaction-driven spin-valley flavour polarization. In this work, we explore correlated phases appearing due to the combined effect of spin-orbit coupling-enhanced valley polarization and large density of states below half filling ($\nu \lesssim 2$) of the moir\'e band in a TBG coupled to tungsten diselenide. We observe anomalous Hall effect, accompanied by a series of Lifshitz transitions, that are highly tunable with carrier density and magnetic field. Strikingly, the magnetization shows an abrupt sign change in the vicinity of half-filling, confirming its orbital nature. The coercive fields reported are about an order of magnitude higher than previous studies in graphene-based moir\'e systems, presumably aided by a Stoner instability favoured by the van Hove singularities in the malleable bands. While the Hall resistance is not quantized at zero magnetic fields, indicative of a ground state with partial valley polarization, perfect quantization and complete valley polarization are observed at finite fields. Our findings illustrate that singularities in the flat bands in the presence of spin-orbit coupling can stabilize ordered phases even at non-integer moir\'e band fillings., Comment: 17 pages, 15 figures

We calculate the electronic structure of AA'AA'...-stacked alternating twist N-layer (tNG) graphene for N = 3, 4, 5, 6, 8, 10, 20 layers and bulk alternating twist (AT) graphite systems where the lattice relaxations are modeled by means of molecular dynamics simulations. We show that the symmetric AA'AA'... stacking is energetically preferred among all interlayer sliding geometries for progressively added layers up to N=6. Lattice relaxations enhance electron-hole asymmetry, and reduce the magic angles with respect to calculations with fixed tunneling strengths that we quantify from few layers to bulk AT-graphite. Without a perpendicular electric field, the largest magic angle flat-band states locate around the middle following the largest eigenvalue eigenstate in a 1D-chain model of layers, while the density redistributes to outer layers for smaller magic twist angles corresponding to higher order effective bilayers in the 1D chain. A perpendicular electric field decouples the electronic structure into $N$ Dirac bands with renormalized Fermi velocities with distinct even-odd band splitting behaviors, showing a gap for N=4 while for odd layers a Dirac cone remains between the flat band gaps. The magic angle error tolerance estimated from density of states maxima expand progressively from $0.05^{\circ}$ in t2G to up to $0.2^{\circ}$ in AT-graphite, hence allowing a greater flexibility in multilayers. Decoupling of tNG into t2G with different interlayer tunneling proportional to the eigenvalues of a 1D layers chain allows to map tNG-multilayers bands onto those of periodic bulk AT-graphite's at different $k_z$ values. We also obtain the Landau level density of states in the quantum Hall regime for magnetic fields of up to 50~T and confirm the presence of nearly flat bands around which we can develop suppressed density of states gap regions by applying an electric field in N > 3 systems., Comment: 21 pages, 15 figures

We investigate the electronic structure of alternating-twist triple Bernal-stacked bilayer graphene (t3BG) as a function of interlayer coupling $\omega$, twist angle $\theta$, interlayer potential difference $\Delta$, and top-bottom bilayers sliding vector $\boldsymbol{\tau}$ for three possible configurations AB/AB/AB, AB/BA/AB, and AB/AB/BA. The parabolic low-energy band dispersions in a Bernal-stacked bilayer and gap-opening through a finite interlayer potential difference $\Delta$ allows the flattening of bands in t3BG down to $\sim 20$~meV for twist angles $\theta \lesssim 2^{\circ}$ regardless of the stacking types. The easier isolation of the flat bands and associated reduction of Coulomb screening thanks to the intrinsic gaps of bilayer graphene for finite $\Delta$ facilitate the formation of correlation-driven gaps when it is compared to the metallic phases of twisted trilayer graphene under electric fields. We obtain the stacking dependent Coulomb energy versus bandwidth $U/W \gtrsim 1$ ratios in the $\theta$ and $\Delta$ parameter space. We also present the expected $K$-valley Chern numbers for the lowest-energy nearly flat bands., Comment: 15 pages, 10 figures