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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

The dominance of Coulomb interactions over kinetic energy of electrons in narrow, non-trivial moir\'{e} bands of magic-angle twisted bilayer graphene (TBG) gives rise to a variety of correlated phases such as correlated insulators, superconductivity, orbital ferromagnetism, Chern insulators and nematicity. Most of these phases occur at or near an integer number of carriers per moir\'{e} unit cell. Experimental demonstration of ordered states at fractional moir\'{e} band-fillings at zero applied magnetic field $B$, is a challenging pursuit. In this letter, we report the observation of states near half-integer band-fillings of $\nu\approx 0.5$ and $\pm3.5$ at $B\approx 0$ in TBG proximitized by tungsten diselenide (WSe$_2$) through magnetotransport and thermoelectricity measurements. A series of Lifshitz transitions due to the changes in the topology of the Fermi surface implies the evolution of van Hove singularities (VHSs) of the diverging density of states (DOS) at a discrete set of partial fillings of flat bands. Furthermore, at a band filling of $\nu\approx-0.5$, a symmetry-broken Chern insulator emerges at high $B$, compatible with the band structure calculations within a translational symmetry-broken supercell with twice the area of the original TBG moir\'{e} cell. Our results are consistent with a spin/charge density wave ground state in TBG in the zero $B$-field limit., Comment: 16 pages, 16 figures

Nanoscale layered ferromagnets have demonstrated fascinating two-dimensional magnetism down to atomic layers, providing a peculiar playground of spin orders for investigating fundamental physics and spintronic applications. However, strategy for growing films with designed magnetic properties is not well established yet. Herein, we present a versatile method to control the Curie temperature (T_{C}) and magnetic anisotropy during growth of ultrathin Cr_{2}Te_{3} films. We demonstrate increase of the TC from 165 K to 310 K in sync with magnetic anisotropy switching from an out-of-plane orientation to an in-plane one, respectively, via controlling the Te source flux during film growth, leading to different c-lattice parameters while preserving the stoichiometries and thicknesses of the films. We attributed this modulation of magnetic anisotropy to the switching of the orbital magnetic moment, using X-ray magnetic circular dichroism analysis. We also inferred that different c-lattice constants might be responsible for the magnetic anisotropy change, supported by theoretical calculations. These findings emphasize the potential of ultrathin Cr_{2}Te_{3} films as candidates for developing room-temperature spintronics applications and similar growth strategies could be applicable to fabricate other nanoscale layered magnetic compounds., Comment: 30 pages, 6 figures, accepted in ACS Applied Nano Materials

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 $\theta$, interlayer potential difference $\Delta$, and top-bottom layer stacking $\tau$ reveals that flat bands with large Coulomb energy vs bandwidth $U/W > 1$ are expected within a range of $\pm 0.2^{\circ}$ near $\theta \simeq1.5^{\circ}$ and $\theta \simeq1.2^{\circ}$ for $\tau_{\rm AA}$ top-bottom layer stacking, between a wider $1^{\circ} \sim 1.7^{\circ}$ range for $\tau_{\rm AB}$ stacking, whose bands often have finite valley Chern numbers thanks to the opening of primary and secondary band gaps in the presence of a finite $\Delta$, and below $\theta \lesssim 0.6^{\circ}$ for all $\tau$ considered. The largest $U/W$ ratios are expected at the magic angle $\sim 1.5^{\circ}$ when $|\Delta| \sim 0$~meV for AA, and slightly below near $\sim 1.4^{\circ}$ for finite $|\Delta| \sim 25$~meV for AB stackings, and near $\theta \sim 0.4^{\circ}$ for both stackings. When ${\tau}$ is the saddle point stacking vector between AB and BA we observe pronounced anisotropic local density of states (LDOS) strip patterns with broken triangular rotational symmetry. We present optical conductivity calculations that reflect the changes in the electronic structure introduced by the stacking and gate tunable system parameters., Comment: 13 pages 8 figures

Rhombohedral $N = 3$ trilayer graphene on hexagonal boron nitride (TLG/BN) hosts gate-tunable, valley-contrasting, nearly flat topological bands that can trigger spontaneous quantum Hall phases under appropriate conditions of the valley and spin polarization. Recent experiments have shown signatures of C = 2 valley Chern bands at 1/4 hole filling, in contrast to the predicted value of C = 3. We discuss the low-energy model for rhombohedral N-layer graphene (N = 1, 2, 3) aligned with hexagonal boron nitride (hBN) subject to off-diagonal moire vector potential terms that can alter the valley Chern numbers. Our analysis suggests that topological phase transitions of the flat bands can be triggered by pseudomagnetic vector field potentials associated to moire strain patterns, and that a nematic order with broken rotational symmetry can lead to valley Chern numbers that are in agreement with recent Hall conductivity observations., Comment: 9 pages, 6 figures

Spontaneous orbital magnetism observed in twisted bilayer graphene (tBG) on nearly aligned hexagonal boron nitride (BN) substrate builds on top of the electronic structure resulting from combined G/G and G/BN double moire interfaces. Here we show that tBG/BN commensurate double moire patterns can be classified into two types, each favoring the narrowing of either the conduction or valence bands on average, and obtain the evolution of the bands as a function of the interlayer sliding vectors and electric fields. Finite valley Chern numbers $\pm 1$ are found in a wide range of parameter space when the moire bands are isolated through gaps, while the local density of states associated to the flat bands are weakly affected by the BN substrate invariably concentrating around the AA-stacked regions of tBG. We illustrate the impact of the BN substrate for a particularly pronounced electron-hole asymmetric band structure by calculating the optical conductivities of twisted bilayer graphene near the magic angle as a function of carrier density. The band structures corresponding to other $N$-multiple commensurate moire period ratios indicate it is possible to achieve narrow width $W \lesssim 30$ meV isolated folded band bundles for tBG angles $\theta \lesssim 1^{\circ}$., Comment: 17 pages, 9 figures

Two-dimensional heterostructures with layers of slightly different lattice vectors exhibit a new periodic structure known as moire lattices. Moire lattice formation provides a powerful new way to engineer the electronic structure of two-dimensional materials for realizing novel correlated and topological phenomena. In addition, superstructures of moire lattices can emerge from multiple misaligned lattice vectors or inhomogeneous strain distribution, which offers an extra degree of freedom in the electronic band structure design. High-resolution imaging of the moire lattices and superstructures is critical for quantitative understanding of emerging moire physics. Here we report the nanoscale imaging of moire lattices and superstructures in various graphene-based samples under ambient conditions using an ultra-high-resolution implementation of scanning microwave impedance microscopy. We show that, quite remarkably, although the scanning probe tip has a gross radius of ~100 nm, an ultra-high spatial resolution in local conductivity profiles better than 5 nm can be achieved. This resolution enhancement not only enables to directly visualize the moire lattices in magic-angle twisted double bilayer graphene and composite super-moire lattices, but also allows design path toward artificial synthesis of novel moire superstructures such as the Kagome moire from the interplay and the supermodulation between twisted graphene and hexagonal boron nitride layers., Comment: 16 pages, 5 figures

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 $\theta \sim 0.5^{\circ}, \, 0.85^{\circ}, \,1.3^{\circ}$ for appropriate perpendicular electric field magnitudes and directions. The valley Chern numbers of the electron-hole asymmetric bands depend intrinsically on the details of the hopping terms in the bilayer graphene, and extrinsically on factors like electric fields or average staggered potentials in the graphene layer aligned with the contacting hexagonal boron nitride substrate. This tunability of the band isolation, bandwidth, and valley Chern numbers makes of tMBG a more versatile system than twisted bilayer graphene for finding nearly flat bands prone to strong correlations., Comment: 15 pages, 11 figures

2D materials based superlattices have emerged as a promising platform to modulate band structure and its symmetries. In particular, moir\'e periodicity in twisted graphene systems produces flat Chern bands. The recent observation of anomalous Hall effect (AHE) and orbital magnetism in twisted bilayer graphene has been associated with spontaneous symmetry breaking of such Chern bands. However, the valley Hall state as a precursor of AHE state, when time-reversal symmetry is still protected, has not been observed. Our work probes this precursor state using the valley Hall effect. We show that broken inversion symmetry in twisted double bilayer graphene (TDBG) facilitates the generation of bulk valley current by reporting the first experimental evidence of nonlocal transport in a nearly flat band system. Despite the spread of Berry curvature hotspots and reduced quasiparticle velocities of the carriers in these flat bands, we observe large nonlocal voltage several micrometers away from the charge current path -- this persists when the Fermi energy lies inside a gap with large Berry curvature. The high sensitivity of the nonlocal voltage to gate tunable carrier density and gap modulating perpendicular electric field makes TDBG an attractive platform for valley-twistronics based on flat bands., Comment: 14 pages, 3 figures and supplementary information

We study the electronic transport properties at the intersection of three topological zero-lines as the elementary current partition node that arises in minimally twisted bilayer graphene. Unlike the partition laws of two intersecting zero-lines, we find that (i) the incoming current can be partitioned into both left-right adjacent topological channels and that (ii) the forward-propagating current is nonzero. By tuning the Fermi energy from the charge-neutrality point to a band edge, the currents partitioned into the three outgoing channels become nearly equal. Moreover, we find that current partition node can be designed as a perfect valley filter and energy splitter controlled by electric gating. By changing the relative electric field magnitude, the intersection of three topological zero-lines can transform smoothly into a single zero line, and the current partition can be controlled precisely. We explore the available methods for modulating this device systematically by changing the Fermi energy, the energy gap size, and the size of central gapless region. The current partition is also influenced by magnetic fields and the system size. Our results provide a microscopic depiction of the electronic transport properties around a unit cell of minimally twisted bilayer graphene and have far-reaching implications in the design of electron-beam splitters and interferometer devices., Comment: arXiv admin note: substantial text overlap with arXiv:1904.12826

Interference of double moire patterns of graphene (G) encapsulated by hexagonal boron nitride (BN) can alter the electronic structure features near the primary/secondary Dirac points and the electron-hole symmetry introduced by a single G/BN moire pattern depending on the relative stacking arrangements of the top/bottom BN layers. We show that strong interference effects are found in nearly aligned BN/G/BN and BN/G/NB and obtain the evolution of the associated density of states as a function of moire superlattice twist angles. For equal moire periods and commensurate patterns with $\Delta \phi = 0^{\circ}$ modulo $60^{\circ}$ angle differences the patterns can add up constructively leading to large pseudogaps of about $\sim 0.5$ eV on the hole side or cancel out destructively depending on their relative sliding, e.g. partially recovering electron-hole symmetry. The electronic structure of moire quasicrystals for $\Delta \phi =30^{\circ}$ differences reveal double moire features in the density of states with almost isolated van Hove singularities where we can expect strong correlations., Comment: 9 pages, 7 figures

Bilayer graphene was theorized to host a moire miniband with flat dispersion if the layers are stacked at specific twist angles known as the magic angles. Recently, such twisted bilayer graphene (tBLG) with the first magic angle twist was reported to exhibit correlated insulating state and superconductivity, where the presence of the flat miniband in the system is thought to be essential for the emergence of these ordered phases in the transport measurements. Tunneling spectroscopy and electronic compressibility measurements in tBLG have revealed a van Hove singularity that is consistent with the presence of the flat miniband. However, a direct observation of the flat dispersion in the momentum-space of such moire miniband in tBLG is still elusive. Here, we report the visualization of the flat moire miniband by using angle-resolved photoemission spectroscopy with nanoscale resolution (nanoARPES). The high spatial resolution in nanoARPES enabled the measurement of the local electronic structure of the tBLG. We clearly demonstrate the existence of the flat moire band near the charge neutrality for tBLG close to the magic angle at room temperature., Comment: 7 pages, 3 figures

We present a multi-scale density functional theory (DFT) informed molecular dynamics and tight-binding (TB) approach to capture the interdependent atomic and electronic structures of twisted bilayer graphene. We calibrate the flat band magic angle to be at $\theta_{\rm M} = 1.08^{\circ}$ by rescaling the interlayer tunneling for different atomic structure relaxation models as a way to resolve the indeterminacy of existing atomic and electronic structure models whose predicted magic angles vary widely between $0.9^\circ \sim 1.3^\circ$. The interatomic force fields are built using input from various stacking and interlayer distance dependent DFT total energies including the exact exchange and random phase approximation (EXX+RPA). We use a Fermi velocity of $\upsilon_{\rm F} \simeq 10^{6}$~m/s for graphene that is enhanced by about $\sim 15\%$ over the local density approximation (LDA) values. Based on this atomic and electronic structure model we obtain high-resolution spectral functions comparable with experimental angle-resolved photoemission spectra (ARPES). Our analysis of the interdependence between the atomic and electronic structures indicates that the intralayer elastic parameters compatible with the DFT-LDA, which are stiffer by $\sim$30\% than widely used reactive empirical bond order force fields, can combine with EXX+RPA interlayer potentials to yield the magic angle at $\sim 1.08^{\circ}$ without further rescaling of the interlayer tunneling.

Twisted bilayer graphene (TBG) hosts nearly flat bands with narrow bandwidths of a few meV at certain {\em magic} twist angles. Here we show that in twisted gapped Dirac material bilayers, or massive twisted bilayer graphenes (MTBG), isolated nearly flat bands below a threshold bandwidth $W_c$ are expected for continuous small twist angles up to a critical $\theta_c$ depending on the flatness of the original bands and the interlayer coupling strength. Narrow bandwidths of $W \lesssim $30 meV are expected for $\theta \lesssim 3^{\circ} $ for twisted Dirac materials with intrinsic gaps of $\sim 2$ eV that finds realization in monolayers of gapped transition metal dichalcogenides (TMDC), silicon carbide (SiC) among others, and even narrower bandwidths in hexagonal boron nitride (BN) whose gaps are $\sim 5$ eV, while twisted graphene systems with smaller gaps of a few tens of meV, e.g. due to alignment with hexagonal boron nitride, show vestiges of the magic angles behavior in the bandwidth evolution. The phase diagram of finite valley Chern numbers of the isolated moire bands expands with increasing difference between the sublattice selective interlayer tunneling parameters. The valley contrasting circular dichroism for interband optical transitions is constructive near $0^{\circ}$ and destructive near $60^{\circ}$ alignments and can be tuned through electric field and gate driven polarization of the mini-valleys. Combining massive Dirac materials with various intrinsic gaps, Fermi velocities, interlayer tunneling strengths suggests optimistic prospects of increasing $\theta_c$ and achieving correlated states with large $U/W$ effective interaction versus bandwidth ratios., Comment: 23 pages, 18 figures

We study the electronic and transport properties of a network of domain walls between insulating domains with opposite valley Chern numbers. We find that the network is semi-metallic with Dirac dispersion near the charge neutrality point and the corresponding electronic states distribute along the domain walls. Near the charge neutrality point, we find quantized conductance in nanoribbon with sawtooth domain wall edges that propagates along the boundaries and is robust against weak disorder. For a trident edged ribbon, we find a small energy gap due to the finite size effect making the nanoribbon an insulator. When the Fermi energy is away from charge neutrality point, all domain walls contribute to the conduction of current. Our results provide a comprehensive analysis of the electronic transport properties in a topological domain wall network that not only agrees qualitatively with experiments on marginally twisted bilayer graphene under a perpendicular electric field, but also can provide useful insights for designing low-power topological quantum devices.

We predict that antiferromagnetic bilayers formed from van der Waals (vdW) materials, like bilayer CrI$_3$, have a strong magnetoelectric response that can be detected by measuring the gate voltage dependence of Faraday or Kerr rotation signals, total magnetization, or anomalous Hall conductivity. Strong effects are possible in single-gate geometries, and in dual-gate geometries that allow internal electric fields and total carrier densities to be varied independently. We comment on the reliability of density-functional-theory estimates of interlayer magnetic interactions in van der Waals bilayers, and on the sensitivity of magnetic interactions to pressure that alters the spatial separation between layers., Comment: This is the version for publish, the SI can be found in previous version

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 parameter space of twist angle $\theta$ and interlayer coupling $\omega$, making it in principle simpler to tailor narrow bandwidth flatbands. Application of vertical pressure can enhance the first magic angle in minimal models at $\theta \sim 1.05^{\circ}$ to larger values of up to $\theta \sim 1.5^{\circ}$ when $ P \sim 2.5$~GPa, where $\theta \propto \omega/ \upsilon_{F}$. Narrow bandwidths are expected in bi-bilayers for a continuous range of small twist angles, i.e. without magic angles, when intrinsic bilayer gaps open by electric fields, or due to remote hopping terms. We find that moderate vertical electric fields can contribute in lifting the degeneracy of the low energy flatbands by enhancing the primary gap near the Dirac point and the secondary gap with the higher energy bands. Distinct valley Chern bands are expected near $0^{\circ}$ or $180^{\circ}$ alignments., Comment: 14 pages, 10 figures in the main tex + supplemental information

Understanding the mechanism of high temperature (high Tc) superconductivity is a central problem in condensed matter physics. It is often speculated that high Tc superconductivity arises from a doped Mott insulator as described by the Hubbard model. An exact solution of the Hubbard model, however, is extremely challenging due to the strong electron-electron correlation. Therefore, it is highly desirable to experimentally study a model Hubbard system in which the unconventional superconductivity can be continuously tuned by varying the Hubbard parameters. Here we report signatures of tunable superconductivity in ABC-trilayer graphene (TLG) / boron nitride (hBN) moir\'e superlattice. Unlike "magic angle" twisted bilayer graphene, theoretical calculations show that under a vertical displacement field the ABC-TLG/hBN heterostructure features an isolated flat valence miniband associated with a Hubbard model on a triangular superlattice. Upon applying such a displacement field we find experimentally that the ABC-TLG/hBN superlattice displays Mott insulating states below 20 Kelvin at 1/4 and 1/2 fillings, corresponding to 1 and 2 holes per unit cell, respectively. Upon further cooling, signatures of superconducting domes emerge below 1 kelvin for the electron- and hole-doped sides of the 1/4 filling Mott state. The electronic behavior in the TLG/hBN superlattice is expected to depend sensitively on the interplay between the electron-electron interaction and the miniband bandwidth, which can be tuned continuously with the displacement field D. By simply varying the D field, we demonstrate transitions from the candidate superconductor to Mott insulator and metallic phases. Our study shows that TLG/hBN heterostructures offer an attractive model system to explore rich correlated behavior emerging in the tunable triangular Hubbard model., Comment: 14 pages, 4 figures

High mobility single and few-layer graphene sheets are in many ways attractive as nanoelectronic circuit hosts but lack energy gaps, which are essential to the operation of field-effect transistors. One of the methods used to create gaps in the spectrum of graphene systems is to form long period moire patterns by aligning the graphene and hexagonal boron nitride (h-BN) substrate lattices. Here, we use planar tunneling devices with thin h-BN barriers to obtain direct and accurate tunneling spectroscopy measurements of the energy gaps in single- and bi-layer graphene-h-BN superlattice structures at charge neutrality (first Dirac point) and at integer moire band occupancies (second Dirac point, SDP) as a function of external electric and magnetic fields and the interface twist angle. In single-layer graphene we find, in agreement with previous work, that gaps are formed at neutrality and at the hole-doped SDP, but not at the electron-doped SDP. Both primary and secondary gaps can be determined accurately by extrapolating Landau fan patterns to zero magnetic field and are as large as $\simeq$ 17 meV for devices in near perfect alignment. For bilayer graphene, we find that gaps occur only at charge neutrality where they can be modified by an external electric field. Tunneling signatures of in-gap states around neutrality suggest the development of edge modes related to topologically non-trivial valley projected bands due to the combination of an external electric field and moire superlattice patterns., Comment: 6 figures

We investigate the bandwidth compression due to out of plane pressure of the moire flatbands near charge neutrality in twisted bilayer graphene for a continuous range of small rotation angles of up to $\sim2.5^{\circ}$. The flatband bandwidth minima angles are found to grow linearly with interlayer coupling {\omega} and decrease with Fermi velocity. Application of moderate pressure values of up to 2.5 GPa achievable through a hydraulic press should allow accessing a flatband for angles as large as $\sim 1.5$^{\circ}$ instead of $\sim 1 \circ$ at zero pressure. This reduction of the moir\'e pattern length for larger twist angle implies an increase of the effective Coulomb interaction scale per moire cell by about 50% and enhance roughly by a factor of $\sim 2$ the elastic energy that resists the commensuration strains due to the moire pattern. Our results suggest that application of pressure on twisted bilayer graphene nanodevices through a hydraulic press will notably facilitate the device preparation efforts required for exploring the ordered phases near magic angle flatbands., Comment: 6 pages 3 figures

Van der Waals heterostructures employing graphene and hexagonal boron nitride (hBN) crystals have emerged as a promising platform for plasmonics thanks to the tunability of their collective modes with carrier density and record values for plasmonics figures of merit. In this Article we investigate theoretically the role of moir\'e-pattern superlattices in nearly aligned graphene on hBN by using continuum-model Hamiltonians derived from ab initio calculations. We calculate the system's energy loss function for a variety of chemical potential values that are accessible in gated devices. Our calculations reveal that the electron-hole asymmetry of the moir\'e bands leads to a remarkable asymmetry of the plasmon dispersion between positive and negative chemical potentials, showcasing the intricate band structure and rich absorption spectrum across the secondary Dirac point gap for the hole bands., Comment: 7 pages, 6 figures

We investigate the electronic structure of the flat bands induced by moir\'e superlattices and electric fields in nearly aligned ABC trilayer graphene-boron nitride interfaces where Coulomb effects can lead to correlated gapped phases. Our calculations indicate that valley-spin resolved isolated superlattice flat bands that carry a finite Chern number $C = 3$ proportional to layer number can appear near charge neutrality for appropriate perpendicular electric fields and twist angles. When the degeneracy of the bands is lifted by Coulomb interactions these topological bands can lead to anomalous quantum Hall phases that embody orbital and spin magnetism. Narrow bandwidths of $\sim10$ meV achievable for a continuous range of twist angles $\theta \lesssim 0.6^{\circ}$ with moderate interlayer potential differences of $\sim$50 meV make the TLG/BN systems a promising platform for the study of electric-field tunable Coulomb interaction driven spontaneous Hall phases., Comment: 8 pages, 6 figures, 1 table

Unconventional superconductivity often arises from Cooper pairing between neighboring atomic sites, stipulating a characteristic pairing symmetry in the reciprocal space. The twisted bilayer graphene (TBG) presents a new setting where superconductivity emerges on the flat bands whose Wannier wavefunctions spread over many graphene unit cells, forming the so-called Moir\'e pattern. To unravel how Wannier states form Cooper pairs, we study the interplay between electronic, structural, and pairing instabilities in TBG. For comparisons, we also study graphene on boron-nitride (GBN) possessing a different Moir\'e pattern, and single-layer graphene (SLG) without a Moir\'e pattern. For all cases, we compute the pairing eigenvalues and eigenfunctions by solving a linearized superconducting gap equation, where the spin-fluctuation mediated pairing potential is evaluated from materials specific tight-binding band structures. We find an extended $s$-wave as the leading pairing symmetry in TBG, in which the nearest-neighbor Wannier sites form Cooper pairs with same phase. In contrast, GBN assumes a $p+ip$-wave pairing between nearest-neighbor Wannier states with odd-parity phase, while SLG has the $d+id$-wave symmetry for inter-sublattice pairing with even-parity phase. Moreover, while $p+ip$, and $d+id$ pairings are chiral, and nodeless, but the extended $s$-wave channel possesses accidental {\it nodes}. The nodal pairing symmetry makes it easily distinguishable via power-law dependencies in thermodynamical entities, in addition to their direct visualization via spectroscopies.

Mott insulator plays a central role in strongly correlated physics, where the repulsive Coulomb interaction dominates over the electron kinetic energy and leads to insulating states with one electron occupying each unit cell. Doped Mott insulator is often described by the Hubbard model3, which can give rise to other correlated phenomena such as unusual magnetism and even high-temperature superconductivity. A tunable Mott insulator, where the competition between the Coulomb interaction and the kinetic energy can be varied in situ, can provide an invaluable model system for the study of Mott physics. Here we report the realization of such a tunable Mott insulator in the ABC trilayer graphene (TLG) and hexagonal boron nitride (hBN) heterostructure with a moir\'e superlattice. Unlike massless Dirac electrons in monolayer graphene, electrons in pristine ABC TLG are characterized by quartic energy dispersion and large effective mass that are conducive for strongly correlated phenomena. The moir\'e superlattice in TLG/hBN heterostructures leads to narrow electronic minibands that are gate tunable. Each filled miniband contains 4 electrons in one moir\'e lattice site due to the spin and valley degeneracy of graphene. The Mott insulator states emerge at 1/4 and 1/2 fillings, corresponding to one electron and two electrons per site, respectively. Moreover, the Mott states in the ABC TLG/hBN heterostructure exhibit unprecedented tunability: the Mott gap can be modulated in situ by a vertical electrical field, and at the meantime, the electron doping can be gate-tuned to fill the band from one Mott insulating state to another. Our observation of a tunable Mott insulator opens up exciting opportunities to explore novel strongly correlated phenomena in two-dimensional moir\'e superlattice heterostructures., Comment: 11 pages, 4 figures