Twisted Double Bilayer Graphene Research Articles

Landau Levels as a Probe for Band Topology in Graphene Moiré Superlattices.

We propose Landau levels as a probe for the topological character of electronic bands in two-dimensional moiré superlattices. We consider two configurations of twisted double bilayer graphene (TDBG) that have very similar band structures, but show different valley Chern numbers of the flat bands. These differences between the AB-AB and AB-BA configurations of TDBG clearly manifest as different Landau level sequences in the Hofstadter butterfly spectra calculated using the tight-binding model. The Landau level sequences are explained from the point of view of the distribution of orbital magnetization in momentum space that is governed by the rotational C_{2} and time-reversal T symmetries. Our results can be readily extended to other twisted graphene multilayers and h-BN/graphene heterostructures thus establishing the Hofstadter butterfly spectra as a powerful tool for detecting the nontrivial valley band topology.

Gate-Tunable Fractional Chern Insulators in Twisted Double Bilayer Graphene.

We predict twisted double bilayer graphene to be a versatile platform for the realization of fractional Chern insulators readily targeted by tuning the gate potential and the twist angle. Remarkably, these topologically ordered states of matter, including spin singlet Halperin states and spin polarized states in Chern number C=1 and C=2 bands, occur at high temperatures and without the need for an external magnetic field.

Bulk valley transport and Berry curvature spreading at the edge of flat bands

2D materials based superlattices have emerged as a promising platform to modulate band structure and its symmetries. In particular, moiré 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 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.

Effect of bilayer stacking on the atomic and electronic structure of twisted double bilayer graphene

Twisted double bilayer graphene has recently emerged as an interesting moir\'e material that exhibits strong correlation phenomena that are tunable by an applied electric field. Here we study the atomic and electronic properties of three different graphene double bilayers: double bilayers composed of two AB stacked bilayers (AB/AB), double bilayers composed of two AA stacked bilayers (AA/AA) as well as heterosystems composed of one AB and one AA bilayer (AB/AA). The atomic structure is determined using classical force fields. We find that the inner layers of the double bilayer exhibit significant in-plane and out-of-plane relaxations, similar to twisted bilayer graphene. The relaxations of the outer layers depend on the stacking: atoms in AB bilayers follow the relaxations of the inner layers, while atoms in AA bilayers attempt to avoid higher-energy AA stacking. For the relaxed structures, we calculate the electronic band structures using the tight-binding method. All double bilayers exhibit flat bands at small twist angles, but the shape of the bands depends sensitively on the stacking of the outer layers. To gain further insight, we study the evolution of the band structure as the outer layers are rigidly moved away from the inner layers, while preserving their atomic relaxations. This reveals that the hybridization with the outer layers results in an additional flattening of the inner-layer flat band manifold. Our results establish AA/AA and AB/AA twisted double bilayers as interesting moir\'e materials with different flat band physics compared to the widely studied AB/AB system.

Combined Minivalley and Layer Control in Twisted Double Bilayer Graphene.

Control over minivalley polarization and interlayer coupling is demonstrated in double bilayer graphene twisted with an angle of 2.37°. This intermediate angle is small enough for the minibands to form and large enough such that the charge carrier gases in the layers can be tuned independently. Using a dual-gated geometry we identify and control all possible combinations of minivalley polarization via the population of the two bilayers. An applied displacement field opens a band gap in either of the two bilayers, allowing us to even obtain full minivalley polarization. In addition, the carriers, formerly separated by their minivalley character, are mixed by tuning through a Lifshitz transition, where the Fermi surface topology changes. The high degree of control over the minivalley character of the bulk charge transport in twisted double bilayer graphene offers new opportunities for realizing valleytronics devices such as valley valves, filters, and logic gates.

Floquet engineering of twisted double bilayer graphene

Motivated by the recent experimental realization of twisted double bilayer graphene (TDBG) samples, we study, both analytically and numerically, the effects of circularly polarized light propagating in free space and confined in a waveguide on the band structure and topological properties of these systems. These two complementary Floquet protocols allow us to selectively tune different parameters of the system by varying the intensity and light frequency. For the drive protocol in free space, in the high-frequency regime, we find that in TDBG with AB/BA stacking, we can selectively close the zone-center quasienergy gaps around one valley while increasing the gaps near the opposite valley by tuning the parameters of the drive. In TDBG with AB/AB stacking, a similar effect can be obtained upon the application of a perpendicular static electric field. Furthermore, we study the topological properties of the driven system in different settings, provide accurate effective Floquet Hamiltonians, and show that relatively strong drives can generate flat bands. On the other hand, longitudinal light confined in a waveguide couples to the components of the interlayer hopping that are perpendicular to the TDBG sheet, allowing for selective engineering of the bandwidth of Floquet zone-center quasienergy bands without breaking the symmetries of the static system.5 MoreReceived 15 June 2020Accepted 1 September 2020DOI:https://doi.org/10.1103/PhysRevResearch.2.033494Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasElectronic structureTwist deformationValleytronicsPhysical SystemsFloquet systemsGrapheneTopological insulatorsTechniquesBand structure methodsCondensed Matter, Materials & Applied Physics

Tunable spin-polarized correlated states in twisted double bilayer graphene.

Reducing the energy bandwidth of electrons in a lattice below the long-range Coulomb interaction energy promotes correlation effects. Moiré superlattices-which are created by stacking van der Waals heterostructures with a controlled twist angle1-3-enable the engineering of electron band structure. Exotic quantum phases can emerge in an engineered moiré flat band. The recent discovery of correlated insulator states, superconductivity and the quantum anomalous Hall effect in the flat band of magic-angle twisted bilayer graphene4-8 has sparked the exploration of correlated electron states in other moiré systems9-11. The electronic properties of van der Waals moiré superlattices can further be tuned by adjusting the interlayer coupling6 or the band structure of constituent layers9. Here, using van der Waals heterostructures of twisted double bilayer graphene (TDBG), we demonstrate a flat electron band that is tunable by perpendicular electric fields in a range of twist angles. Similarly to magic-angle twisted bilayer graphene, TDBG shows energy gaps at the half- and quarter-filled flat bands, indicating the emergence of correlated insulator states. We find that the gaps of these insulator states increase with in-plane magnetic field, suggesting a ferromagnetic order. On doping the half-filled insulator, a sudden drop in resistivity is observed with decreasing temperature. This critical behaviour is confined to a small area in the density-electric-field plane, and is attributed to a phase transition from a normal metal to a spin-polarized correlated state. The discovery of spin-polarized correlated states in electric-field-tunable TDBG provides a new route to engineering interaction-driven quantum phases.

Phonon scattering induced carrier resistivity in twisted double-bilayer graphene

In this work we carry out a theoretical study of the phonon-induced resistivity in twisted double bilayer graphene (TDBG), in which two Bernal-stacked bilayer graphene devices are rotated relative to each other by a small angle $\theta$. We show that at small twist angles ($\theta\sim 1^\circ$) the effective mass of the TDBG system is greatly enhanced, leading to a drastically increased phonon-induced resistivity in the high-temperature limit where phonon scattering leads to a linearly increasing resistivity with increasing temperature. We also discuss possible implications of our theory on superconductivity in such a system, and provide an order of magnitude estimation of the superconducting transition temperature.

Anomalous Hall effect, magneto-optical properties, and nonlinear optical properties of twisted graphene systems

We study the anomalous Hall effect, magneto-optical properties, and nonlinear optical properties of twisted bilayer graphene aligned with hexagonal boron nitride substrate, as well as twisted double bilayer graphene systems. We show that non-vanishing valley polarizations in twisted graphene systems would give rise to the anomalous Hall effect, which can be tuned by in-plane magnetic fields. The valley polarized states are also associated with giant Faraday and Kerr rotations in the terahertz frequency regime. Moreover, we propose that the twisted graphene systems exhibit colossal nonlinear optical responses by virtue of the inversion-symmetry breaking, the small bandwidth, and the small excitation gaps of the systems. In twisted double bilayer graphene, we find that certain components of the nonlinear photo-conductivity tensor are directly proportional to the orbital magnetization of the system, which would exhibit remarkable hysteresis behavior in response to perpendicular magnetic fields.

Ferromagnetism and superconductivity in twisted double bilayer graphene

Twisted double bilayer graphene is a highly tunable moir\'e system to study strongly interacting physics. Here, the authors present a theory of competing ferromagnetic and superconducting orders in this system. They show that the single-particle moir\'e bands can be drastically modified by a perpendicular electric displacement field. As a result, the ferromagnetic insulating gap driven by Coulomb interaction has a dome shape dependence on the layer potential difference, as observed in several experiments. The stability of the ferromagnetic insulator against collective excitations, including spin and valley magnons, is theoretically verified. Furthermore, the authors investigate the possibility of phonon-mediated intervalley equal-spin pairing, using the property that the acoustic phonon mediated attraction respects an enlarged SU(2)\ifmmode\times\else\texttimes\fi{}SU(2) symmetry.

Tunable bandwidths and gaps in twisted double bilayer graphene on the verge of correlations

We use temperature-dependent resistivity in small-angle twisted double bilayer graphene to measure bandwidths and gaps of the bands. This electron-hole asymmetric system has one set of non-dispersing bands that splits into two flat bands with the electric field - distinct from the twisted bilayer system. With electric field, the gap between two emergent flat bands increases monotonically and bandwidth is tuned from 1 meV to 15 meV. These two flat bands with gap result in a series of thermally induced insulator to metal transitions - we use a model, at charge neutrality, to measure the bandwidth using only transport measurements. Having two flat bands with tunable gap and bandwidth offers an opportunity to probe the emergence of correlations.

Moiré Flat Bands in Twisted Double Bilayer Graphene.

We investigate twisted double bilayer graphene (TDBG), a four-layer system composed of two AB-stacked graphene bilayers rotated with respect to each other by a small angle. Our ab initio band structure calculations reveal a considerable energy gap at the charge-neutrality point that we assign to the intrinsic symmetric polarization (ISP). We then introduce the ISP effect into the tight-binding parametrization and perform calculations on TDBG models that include lattice relaxation effects down to very small twist angles. We identify a narrow region around the magic angle characterized by a manifold of remarkably flat bands gapped out from other states even without external electric fields. To understand the fundamental origin of the magic angle in TDBG, we construct a continuum model that points to a hidden mathematical link to the twisted bilayer graphene model, thus indicating that the band flattening is a fundamental feature of TDBG and is not a result of external fields.

Theory of correlated insulating behaviour and spin-triplet superconductivity in twisted double bilayer graphene

Two graphene monolayers twisted by a small magic angle exhibit nearly flat bands, leading to correlated electronic states. Here we study a related but different system with reduced symmetry - twisted double bilayer graphene (TDBG), consisting of two Bernal stacked bilayer graphenes, twisted with respect to one another. Unlike the monolayer case, we show that isolated flat bands only appear on application of a vertical displacement field. We construct a phase diagram as a function of twist angle and displacement field, incorporating interactions via a Hartree-Fock approximation. At half-filling, ferromagnetic insulators are stabilized with valley Chern number {C}_{{rm{v}}}=pm 2. Upon doping, ferromagnetic fluctuations are argued to lead to spin-triplet superconductivity from pairing between opposite valleys. We highlight a novel orbital effect arising from in-plane fields plays an important role in interpreting experiments. Combined with recent experimental findings, our results establish TDBG as a tunable platform to realize rare phases in conventional solids.

Intrinsic band gap and electrically tunable flat bands in twisted double bilayer graphene

We present atomistic calculations on structural and electronic properties of twisted double bilayer graphene (TDBG) consisting of two sets of rotationally misaligned Bernal-stacked bilayer graphene. Obtained equilibrium atomic structures exhibit in-plane strains and the modulation of the interlayer distances at the rotationally mismatched interface layers. We find that the electronic structure of TDBG can have an intrinsic band gap at the charge neutral point for a large range of the twist angle theta. Near theta = 1.25 degree, the intrinsic band gap disappears and TDBG hosts flat bands at the Fermi level that are energetically well separated from higher and lower energy bands. We also show that the flat bands are easily tunable by applying vertical electric fields, and extremely narrow bandwidths less than 10 meV can be achieved for the electron-side flat bands in a wide range of the twist angle. Our results serve as a theoretical guide for exploring emergent correlated electron physics in this versatile moire superlattice system.

Correlated Insulating States in Twisted Double Bilayer Graphene.

We present a combined experimental and theoretical study of twisted double bilayer graphene with twist angles between 1° and 1.35°. Consistent with moiré band structure calculations, we observe insulators at integer moiré band fillings one and three, but not two. An applied transverse electric field separates the first moiré conduction band from neighboring bands, and favors the appearance of correlated insulators at 1/4, 1/2, and 3/4 band filling. Insulating states at 1/4 and 3/4 band filling emerge only in a parallel magnetic field (B_{||}), whereas the resistivity at half band filling is weakly dependent on B_{||}. Our findings suggest that correlated insulators are favored when a moiré flat band is spectrally isolated, and are consistent with a mean-field picture in which insulating states are established by breaking both spin and valley symmetries at 1/4 and 3/4 band filling and valley polarization alone at 1/2 band filling.

Gap Opening in Twisted Double Bilayer Graphene by Crystal Fields.

Crystal fields occur due to a potential difference between chemically different atomic species. In van der Waals heterostructures such fields are naturally present perpendicular to the planes. It has been realized recently that twisted graphene multilayers provide powerful playgrounds to engineer electronic properties by the number of layers, the twist angle, applied electric biases, electronic interactions, and elastic relaxations, but crystal fields have not received the attention they deserve. Here, we show that the band structure of large-angle twisted double bilayer graphene is strongly modified by crystal fields. In particular, we experimentally demonstrate that twisted double bilayer graphene, encapsulated between hBN layers, exhibits an intrinsic band gap. By the application of an external field, the gaps in the individual bilayers can be closed, allowing to determine the crystal fields. We find that crystal fields point from the outer to the inner layers with strengths in the bottom/top bilayer [Formula: see text] = 0.13 V/nm ≈ [Formula: see text] = 0.12 V/nm. We show both by means of first-principles calculations and low energy models that crystal fields open a band gap in the ground state. Our results put forward a physical scenario in which a crystal field effect in carbon substantially impacts the low energy properties of twisted double bilayer graphene, suggesting that such contributions must be taken into account in other regimes to faithfully predict the electronic properties of twisted graphene multilayers.