Integer Fillings Research Articles

Correlated insulators and charge density wave states in chirally twisted triple bilayer graphene

Motivated by recent experimental observations of displacement-field-tuned correlated insulators at integer and half-integer fillings in chirally twisted triple bilayer graphene (CTTBG) [Phys.Rev.Lett.132.246501], we study the single-particle and interacting physics of CTTBG. We find that there are two inequivalent stacking orders, i.e., AB-AB-BC and AB-AB-AB, and both exhibit flat bands with nontrivial topology. We then use the Hartree–Fock approximation to calculate the rich phase diagram of CTTBG at all integer and half-integer fillings in both stacking orders and under the vertical displacement field. Under a small displacement field, the groundstates are flavor polarized states for AB-AB-BC stacking order and intervalley coherent states for AB-AB-AB stacking order at all integer and half-integer fillings. A larger displacement field will turn them into layer-polarized states. At half-integer fillings, the groundstates also exhibit charge density wave (CDW) order. For AB-AB-AB stacking, the groundstates at half-integer fillings are always 2 × 1 stripe state among a range of displacement fields. For AB-AB-BC stacking, the groundstates at half-integer fillings are also 2 × 1 stripe states under a small displacement field and a larger displacement will possibly favor further translation-symmetry-breaking, depending on filling and the direction of the displacement field. We demonstrate that the CDW states observed in the experiment can originate from the strong Coulomb interaction of the flat band electrons.

Intrinsic dipole Hall effect in twisted MoTe2: magnetoelectricity and contact-free signatures of topological transitions

We discover an intrinsic dipole Hall effect in a variety of magnetic insulating states at integer fillings of twisted MoTe2 moiré superlattice, including topologically trivial and nontrivial ferro-, antiferro-, and ferri-magnetic configurations. The dipole Hall current, in linear response to in-plane electric field, generates an in-plane orbital magnetization M∥ along the field, through which an AC field can drive magnetization oscillation up to THz range. Upon the continuous topological phase transitions from trivial to quantum anomalous Hall states in both ferromagnetic and antiferromagnetic configurations, the dipole Hall current and M∥ have an abrupt sign change, enabling contact-free detection of the transitions through the magnetic stray field. In configurations where the linear response is forbidden by symmetry, the dipole Hall current and M∥ appear as a crossed nonlinear response to both in-plane and out-of-plane electric fields. These magnetoelectric phenomena showcase fascinating functionalities of insulators from the interplay between magnetism, topology, and electrical polarization.

Dynamical Correlations and Order in Magic-Angle Twisted Bilayer Graphene

The interplay of dynamical correlations and electronic ordering is pivotal in shaping phase diagrams of correlated quantum materials. In magic-angle twisted bilayer graphene, transport, thermodynamic, and spectroscopic experiments pinpoint a competition between distinct low-energy states with and without electronic order, as well as between localized and delocalized charge carriers. In this study, we utilize dynamical mean-field theory on the topological heavy fermion model of twisted bilayer graphene to investigate the emergence of electronic correlations and long-range order in the absence of strain. We contrast moment formation, Kondo screening, and ordering on a temperature basis and explain the nature of emergent correlated states based on three central phenomena: (i) the formation of local spin and valley isospin moments around 100 K, (ii) the ordering of the local isospin moments around 10 K preempting Kondo screening, and (iii) a cascadic redistribution of charge between localized and delocalized electronic states upon doping. At integer fillings, we find that low-energy spectral weight is depleted in the symmetric phase, while we find insulating states with gaps enhanced by exchange coupling in the zero-strain ordered phases. Doping away from integer filling results in distinct metallic states: a “bad metal” above the ordering temperature, where scattering off the disordered local moments suppresses electronic coherence, and a “good metal” in the ordered states with coherence of quasiparticles facilitated by isospin order. This finding reveals coherence from order as the microscopic mechanism behind the Pomeranchuk effect observed experimentally by Rozen [] and by Saito []. Upon doping, there is a periodic charge reshuffling between localized and delocalized electronic orbitals leading to cascades of doping-induced Lifshitz transitions, local spectral weight redistributions, and periodic variations of the electronic compressibility ranging from nearly incompressible to negative. Our findings highlight the essential role of charge transfer, hybridization, and ordering in shaping the electronic excitations and thermodynamic properties in twisted bilayer graphene and provide a unified understanding of the most puzzling aspects of scanning tunneling spectroscopy, transport, and compressibility experiments. Published by the American Physical Society 2024

Long-lived isospin excitations in magic-angle twisted bilayer graphene.

Numerous correlated many-body phases, both conventional and exotic, have been reported in magic-angle twisted bilayer graphene (MATBG)1-24. However, the dynamics associated with these correlated states, crucial for understanding the underlying physics, remain unexplored. Here we combine exciton sensing and optical pump-probe spectroscopy to investigate the dynamics of isospin orders in MATBG with WSe2 substrate across the entire flat band, achieving sub-picosecond resolution. We observe remarkably slow isospin dynamics in a broad filling range around ν = 2 and between ν = -3 and -2, with lifetimes of up to 300 ps that decouple from the much faster cooling of electronic temperature (about 10 ps). This non-thermal behaviour demonstrates the presence of abnormally long-lived modes in the isospin degrees of freedom. This observation, not anticipated by theory, implies the existence of long-range propagating collective modes, strong isospin fluctuations and memory effects and is probably associated with an intervalley coherent or incommensurate Kekulé spiral ground state. We further demonstrate non-equilibrium control of the isospin orders previously found around integer fillings. Specifically, through ultrafast manipulation, it can be transiently shifted away from integer fillings. Our study demonstrates a unique probe of collective excitations in MATBG and paves the way for actively controlling non-equilibrium phenomena in moiré systems.

Multiferroicity and Topology in Twisted Transition Metal Dichalcogenides.

Van der Waals heterostructures have recently emerged as an exciting platform for investigating the effects of strong electronic correlations, including various forms of magnetic or electrical orders. Here, we perform an unbiased exact diagonalization study of the effects of interactions on topological flat bands of twisted transition metal dichalcogenides (TMDs) at odd integer fillings. For hole-filling ν_{h}=1, we find that the Chern insulator phase, expected from interaction-induced spin-valley polarization of the bare bands, is quite fragile, and gives way to spontaneous multiferroic order-coexisting ferroelectricity and ferromagnetism, in the presence of long-range Coulomb repulsion. We provide a simple real-space picture to understand the phase diagram as a function of interaction range and strength. Our findings establish twisted TMDs as a novel and highly tunable platform for multiferroicity, and we outline a potential route towards electrical control of magnetism in the multiferroic phase.

High-Mobility Compensated Semimetals, Orbital Magnetization, and Umklapp Scattering in Bilayer Graphene Moiré Superlattices.

Twist-controlled moiré superlattices (MSs) have emerged as a versatile platform for realizing artificial systems with complex electronic spectra. The combination of Bernal-stacked bilayer graphene (BLG) and hexagonal boron nitride (hBN) can give rise to an interesting MS, which has recently featured a set of unexpected behaviors, such as unconventional ferroelectricity and the electronic ratchet effect. Yet, the understanding of the electronic properties of BLG/hBN MS has, at present, remained fairly limited. Here, we combine magneto-transport and low-energy sub-THz excitation to gain insights into the properties of this MS. We demonstrate that the alignment between BLG and hBN crystal lattices results in the emergence of compensated semimetals at some integer fillings of the moiré bands, separated by van Hove singularities where the Lifshitz transition occurs. A particularly pronounced semimetal develops when eight holes reside in the moiré unit cell, where coexisting high-mobility electron and hole systems feature strong magnetoresistance reaching 2350% already at B = 0.25 T. Next, by measuring the THz-driven Nernst effect in remote bands, we observe valley splitting, indicating an orbital magnetization characterized by a strongly enhanced effective gv-factor of 340. Finally, using THz photoresistance measurements, we show that the high-temperature conductivity of the BLG/hBN MS is limited by electron-electron umklapp processes. Our multifaceted analysis introduces THz-driven magnetotransport as a convenient tool to probe the band structure and interaction effects in van der Waals materials and provides a comprehensive understanding of the BLG/hBN MS.

Untwisting Moiré Physics: Almost Ideal Bands and Fractional Chern Insulators in Periodically Strained Monolayer Graphene.

Moiré systems have emerged in recent years as a rich platform to study strong correlations. Here, we will propose a simple, experimentally feasible setup based on periodically strained graphene that reproduces several key aspects of twisted moiré heterostructures-but without introducing a twist. We consider a monolayer graphene sheet subject to a C_{2}-breaking periodic strain-induced pseudomagnetic field with period L_{M}≫a, along with a scalar potential of the same period. This system has almost ideal flat bands with valley-resolved Chern number ±1, where the deviation from ideal band geometry is analytically controlled and exponentially small in the dimensionless ratio (L_{M}/l_{B})^{2}, where l_{B} is the magnetic length corresponding to the maximum value of the pseudomagnetic field. Moreover, the scalar potential can tune the bandwidth far below the Coulomb scale, making this a very promising platform for strongly interacting topological phases. Using a combination of strong-coupling theory and self-consistent Hartree-Fock, we find quantum anomalous Hall states at integer fillings. At fractional filling, exact diagonaliztion reveals a fractional Chern insulator at parameters in the experimentally feasible range. Overall, we find that this system has larger interaction-induced gaps, smaller quasiparticle dispersion, and enhanced tunability compared to twisted graphene systems, even in their ideal limit.

Magnetic Field-Stabilized Wigner Crystal States in a Graphene Moiré Superlattice.

ABC-stacked trilayer graphene on boron nitride (ABC-TLG/hBN) moiré superlattices provides a tunable platform for exploring Wigner crystal states in which the electron correlation can be controlled by electric and magnetic fields. Here we report the observation of magnetic field-stabilized Wigner crystal states in a ABC-TLG/hBN. We show that correlated insulating states emerge at multiple fractional and integer fillings corresponding to ν = 1/3, 2/3, 1, 4/3, 5/3, and 2 electrons per moiré lattice site under a magnetic field. These correlated insulating states can be attributed to generalized Mott states for the integer fillings and generalized Wigner crystal states for the fractional fillings. The generalized Wigner crystal states are stabilized by a vertical magnetic field and are strongest at one magnetic flux quantum per three moiré superlattices. The ν = 2 insulating state persists up to 30 T, which can be described by a Mott-Hofstadter transition at a high magnetic field.

Kondo Lattice Model of Magic-Angle Twisted-Bilayer Graphene: Hund's Rule, Local-Moment Fluctuations, and Low-Energy Effective Theory.

We apply a generalized Schrieffer-Wolff transformation to the extended Anderson-like topological heavy fermion (THF) model for the magic-angle (θ=1.05°) twisted bilayer graphene (MATBLG) [Phys. Rev. Lett. 129, 047601 (2022)PRLTAO0031-900710.1103/PhysRevLett.129.047601], to obtain its Kondo lattice limit. In this limit localized f electrons on a triangular lattice interact with topological conduction c electrons. By solving the exact limit of the THF model, we show that the integer fillings ν=0,±1,±2 are controlled by the heavy f electrons, while ν=±3 is at the border of a phase transition between two f-electron fillings. For ν=0,±1,±2, we then calculate the Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions between the f moments in the full model and analytically prove the SU(4) Hund's rule for the ground state which maintains that two f electrons fill the same valley-spin flavor. Our (ferromagnetic interactions in the) spin model dramatically differ from the usual Heisenberg antiferromagnetic interactions expected at strong coupling. We show the ground state in some limits can be found exactly by employing a positive semidefinite "bond-operators" method. We then compute the excitation spectrum of the f moments in the ordered ground state, prove the stability of the ground state favored by RKKY interactions, and discuss the properties of the Goldstone modes, the (reason for the accidental) degeneracy of (some of) the excitation modes, and the physics of their phase stiffness. We develop a low-energy effective theory for the f moments and obtain analytic expressions for the dispersion of the collective modes. We discuss the relevance of our results to the spin-entropy experiments in TBG.

Emergence of correlations in twisted monolayer–trilayer graphene heterostructures

Twisted bilayer graphene heterostructures have recently emerged as a well-established platform for studying strongly correlated phases, such as correlated insulating, superconducting, and topological states. Extending this notion to twisted multilayer graphene heterostructures has exhibited more diverse correlated phases, as some fundamental properties related to symmetry and band structures are correspondingly modified. Here, we report the observations of correlated states in twisted monolayer–trilayer (Bernal stacked) graphene heterostructures. Correlated phases at integer fillings of the moiré unit cell are revealed at a high displacement field and stabilized with a moderate magnetic field on the electron-doping side at a twist angle of 1.45°, where the lift of degeneracy at the integer fillings is observed in the Landau fan diagram. Our results demonstrate the effectiveness of moiré engineering in an extended structure and provide insights into electric-field tunable correlated phases.

Polynomial sign problem and topological Mott insulator in twisted bilayer graphene

We show that for magic-angle twisted bilayer graphene (TBG) away from charge neutrality, although quantum Monte Carlo (QMC) simulations suffer from the sign problem, the computational complexity is at most polynomial at certain integer fillings. For even integer fillings, this polynomial complexity survives even if an extra inter-valley attractive interaction is introduced, on top of Coulomb repulsions. This observation allows us to simulate magic-angle twisted bilayer graphene and to obtain accurate phase diagram and dynamical properties. At the chiral limit and filling $\nu=1$, the simulations reveal a thermodynamic transition separating metallic state and a $C=1$ correlated Chern insulator -- topological Mott insulator (TMI) -- and the pseudogap spectrum slightly above the transition temperature. The ground state excitation spectra of the TMI exhibit a spin-valley U(4) Goldstone mode and a time reversal restoring excitonic gap smaller than the single particle gap. These results are qualitatively consistent with the recent experimental findings at zero-field and $\nu=1$ filling in $h$-BN nonaligned TBG.

Topological Exact Flat Bands in Two-Dimensional Materials under Periodic Strain.

We study flat bands and their topology in 2D materials with quadratic band crossing points under periodic strain. In contrast to Dirac points in graphene, where strain acts as a vector potential, strain for quadratic band crossing points serves as a director potential with angular momentum ℓ=2. We prove that when the strengths of the strain fields hit certain "magic" values, exact flat bands with C=±1 emerge at charge neutrality point in the chiral limit, in strong analogy to magic angle twisted-bilayer graphene. These flat bands have ideal quantum geometry for the realization of fractional Chern insulators, and they are always fragile topological. The number of flat bands can be doubled for certain point group, and the interacting Hamiltonian is exactly solvable at integer fillings. We further demonstrate the stability of these flat bands against deviations from the chiral limit, and discuss possible realization in 2D materials.

Collective excitations of the Chern-insulator states in commensurate double moiré superlattices of twisted bilayer graphene on hexagonal boron nitride

We study the collective excitation modes of the Chern insulator states in magic-angle twisted bilayer graphene aligned with hexagonal boron nitride (TBG/BN) at odd integer fillings ($\nu$) of the flat bands. For the $1 \times 1$ commensurate double moir\'{e} superlattices in TBG/BN at three twist angles ($\theta'$) between BN and graphene, self-consistent Hartree-Fock calculations show that the electron-electron interaction and the broken $C_{2z}$ symmetry lead to the Chern-insulator ground states with valley-spin flavor polarized HF bands at odd $\nu$. In the active-band approximation, the HF bands in the same flavor of TBG/BN are much more separated than those of the pristine TBG with TBG/BN having a larger intra-flavor band gap so that the energies of the lowest intra-flavor exciton modes of TBG/BN computed within the time-dependent HF method are much higher than those of TBG and reach about 20 meV, and the exciton wavefunctions of TBG/BN become less localized than those of TBG. The inter-flavor valley-wave modes in TBG/BN have excitation energies higher than 2.5 meV which is also much larger than that of TBG, while the spin-wave modes all have zero excitation gap. In contrast to TBG with particle-hole symmetric excitation modes for positive and negative $\nu$, the excitation spectrums and gaps of TBG/BN at positive $\nu$ are rather different from those at negative $\nu$. The quantitative behavior of the excitation spectrum of TBG/BN also varies with $\theta'$. Full HF calculations demonstrate that more HF bands besides the two central bands can have rather large contributions from the single-particle flat-band states, then the lowest exciton modes that determine the optical properties of the Chern insulator states in TBG/BN are generally the ones between the remote and flat-like bands, while the valley-wave modes have similar energies as those in the active-band approximation.

Chern insulator phases and spontaneous spin and valley order in a moiré lattice model for magic-angle twisted bilayer graphene

At a certain ``magic'' relative twist angle of two graphene sheets it remains a challenge to obtain a detailed description of the proliferation of correlated topological electronic phases and their filling dependence. We perform a self-consistent real-space Hartree-Fock study of an effective moir\'e lattice model to map out the preferred ordered phases as a function of Coulomb interaction strength and moir\'e flat-band filling factor. It is found that a quantum valley Hall phase, previously discovered at charge neutrality, is present at all integer fillings for sufficiently large interactions. However, except for charge neutrality, additional spontaneous spin/valley polarization is present in the ground state at nonzero integer fillings, leading to Chern insulator phases and anomalous quantum Hall effects at odd filling factors, thus constituting an example of interaction-driven nontrivial topology. At weaker interactions, all nonzero integer fillings feature metallic inhomogeneous spin/valley ordered phases which may also break additional point group symmetries of the system. We discuss these findings in the light of previous theoretical studies on and recent experimental developments related to magic-angle twisted bilayer graphene.

Coupled Ferroelectricity and Correlated States in a Twisted Quadrilayer MoS2 Moiré Superlattice

Moiré superlattices have emerged as a highly controllable quantum platform for exploration of various fascinating phenomena, such as Mott insulator states, ferroelectric order, unconventional superconductivity and orbital ferromagnetism. Although remarkable progress has been achieved, current research in moiré physics has mainly focused on the single species properties, while the coupling between distinct moiré quantum phenomena remains elusive. Here we demonstrate, for the first time, the strong coupling between ferroelectricity and correlated states in a twisted quadrilayer MoS2 moiré superlattice, where the twist angles are controlled in sequence to be ∼ 57°, ∼ 0°, and ∼ –57°. Correlated insulator states are unambiguously established at moiré band filling factors v = 1, 2, 3 of twisted quadrilayer MoS2. Remarkably, ferroelectric order can occur at correlated insulator states and disappears quickly as the moiré band filling deviates from the integer fillings, providing smoking gun evidences of the coupling between ferroelectricity and correlated states. Our results demonstrate the coupling between different moiré quantum properties and will hold great promise for new moiré physics and applications.

Competing spin-valley entangled and broken symmetry states in the N=1 Landau level of graphene

We study many-body ground states for the partial integer fillings of the $N=1$ Landau level in graphene, by constructing a model that accounts for the lattice scale corrections to the Coulomb interactions. Interestingly, in contrast to the $N=0$ Landau level, this model contains not only pure delta function interactions but also some of its derivatives. Due to this we find several important differences with respect to the $N=0$ Landau level. For example at quarter filling when only a single component is filled, there is a degeneracy lifting of the quantum hall ferromagnets and ground states with entangled spin and valley degrees of freedom can become favourable. Moreover at half-filling of the $N=1$ Landau level, we have found a new phase that is absent in the $N=0$ Landau level, that combines characteristics of the Kekul\'{e} state and an antiferromagnet. We also find that according to the parameters extracted in a recent experiment, at half-filling of the $N=1$ Landau level graphene is expected to be in a delicate competition between an AF and a CDW state, but we also discuss why the models for these recent experiments might be missing some important terms.

Fractional correlated insulating states at one-third filled magic angle twisted bilayer graphene

The observation of superconductivity and correlated insulating states in twisted bilayer graphene has motivated much theoretical progress at integer fillings. However, little attention has been given to fractional fillings. Here we show that the three-peak structure of Wannier orbitals, dictated by the symmetry and topology of flat bands, facilitates the emergence of a state we name a “fractional correlated insulator” at commensurate fractional filling of ν = n ± 1/3. Specifically for the filling of 1/3 electrons per moiré unit cell, we show that short-range interactions lead to an extensive entropy due to the “breathing” degree of freedom of an irregular honeycomb lattice that emerges through defect lines. The leading further-range interaction lifts this degeneracy and selects a ferromagnetic nematic state that breaks AB/BA sublattice symmetry. The proposed fractional correlated insulating state might underlie the suppression of superconductivity at ν = 2 − 1/3 filling observed in ref. 1.

Detecting Symmetry Breaking in Magic Angle Graphene Using Scanning Tunneling Microscopy.

A growing body of experimental work suggests that magic angle twisted bilayer graphene exhibits a "cascade" of spontaneous symmetry-breaking transitions, sparking interest in the potential relationship between symmetry breaking and superconductivity. However, it has proven difficult to find experimental probes which can unambiguously identify the nature of the symmetry breaking. Here, we show how atomically resolved scanning tunneling microscopy can be used as a fingerprint of symmetry-breaking order. By analyzing the pattern of sublattice polarization and "Kekulé" distortions in small magnetic fields, order parameters for each of the most competitive symmetry-breaking states can be identified. In particular, we show that the "Kramers intervalley coherent state," which theoretical work predicts to be the ground state at even integer fillings, shows a Kekulé distortion which emerges only in a magnetic field.

Mott correlations in ABC graphene trilayer aligned with hBN

ABC trilayer graphene aligned with hexagonal boron nitride (ABC/hBN) and other moir\'e systems have shown insulating phases at integer fillings of the moir\'e lattice. The role of Mott physics in these insulating states has been questioned by observations of correlated states in a nonaligned ABC trilayer, but recent photocurrent experiments in aligned samples are consistent with the existence of a Mott insulating state at half filling. Using dynamical mean-field theory we address the effect of Mott correlations in ABC/hBN. We show that, at experimentally relevant interaction values, the electronic states are strongly affected by a significant spectral weight transfer not present without alignment to hBN. This effect, which emerges at interactions considerably smaller than ${U}_{\mathrm{Mott}}$ (at which the Mott metal-insulator transition takes place) and does not require symmetry breaking, also impacts the electronic properties at temperatures above the ordering transitions producing anomalous temperature and doping dependencies. Close to the Mott transition, the intramoir\'e unit cell interactions promote an antiferromagnetic state, probably breaking the ${C}_{3}$ symmetry, that would compete with the ferromagnetic exchange interactions to determine the ground state.

Reentrant Correlated Insulators in Twisted Bilayer Graphene at 25T (2π Flux).

Twisted bilayer graphene (TBG) is remarkable for its topological flat bands, which drive strongly interacting physics at integer fillings, and its simple theoretical description facilitated by the Bistritzer-MacDonald Hamiltonian, a continuum model coupling two Dirac fermions. Because of the large moiré unit cell, TBG offers the unprecedented opportunity to observe reentrant Hofstadter phases in laboratory-strength magnetic fields near 25T. This Letter is devoted to magic angle TBG at 2π flux where the magnetic translation group commutes. We use a newly developed gauge-invariant formalism to determine the exact single-particle band structure and topology. We find that the characteristic TBG flat bands reemerge at 2π flux, but, due to the magnetic field breaking C_{2z}T, they split and acquire Chern number ±1. We show that reentrant correlated insulating states appear at 2π flux driven by the Coulomb interaction at integer fillings, and we predict the characteristic Landau fans from their excitation spectrum.