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Flat band moiré superlattices have recently emerged as unique platforms for investigating the interplay between strong electronic correlations, nontrivial band topology, and multiple isospin ‘flavor’ symmetries. Twisted monolayer-bilayer graphene (tMBG) is an especially rich system owing to its low crystal symmetry and the tunability of its bandwidth and topology with an external electric field. Here, we find that orbital magnetism is abundant within the correlated phase diagram of tMBG, giving rise to the anomalous Hall effect in correlated metallic states nearby most odd integer fillings of the flat conduction band, as well as correlated Chern insulator states stabilized in an external magnetic field. The behavior of the states at zero field appears to be inconsistent with simple spin and valley polarization for the specific range of twist angles we investigate, and instead may plausibly result from an intervalley coherent (IVC) state with an order parameter that breaks time reversal symmetry. The application of a magnetic field further tunes the competition between correlated states, in some cases driving first-order topological phase transitions. Our results underscore the rich interplay between closely competing correlated ground states in tMBG, with possible implications for probing exotic IVC ordering. Twisted monolayer-bilayer graphene is an attractive platform to study the interplay between topology, magnetism and correlations in the flat bands. Here, using electrical transport measurements, the authors uncover a rich correlated phase diagram and identify a new insulating state that can be explained by intervalley coherence with broken time reversal symmetry.

Magic-angle twisted bilayer graphene (tBLG) displays a variety of symmetry-broken phases, correlated Chern insulators, orbital magnetism and superconductivity 1 – 8 . In particular, the anomalous Hall effect has been observed when the bands are filled with an odd number of electrons per moiré unit cell 5 , 6 , 9 , indicating the emergence of a zero-field orbital magnetic state with spontaneously broken time-reversal symmetry 10 – 12 . Here we present measurements of two tBLG devices with twist angles slightly away from the magic angle and report the observation of the anomalous Hall effect at half filling of both the electron and hole moiré bands. We suggest that two factors—the increased band dispersion away from the magic angle, and substrate potentials from the encapsulating boron nitride—probably play critical roles in stabilizing a valley-polarized ground state at half filling. Our findings further expand the rich correlated phase diagram of tBLG, and indicate the need to develop a more complete understanding of its manifold of closely competing symmetry-breaking orders. The anomalous Hall effect can signify that a material has a spontaneous magnetic order. Now, twisted bilayer graphene shows this effect at half filling, suggesting that the ground state is valley-polarized.

Combining atomically-thin van der Waals materials into heterostructures provides a powerful path towards the creation of designer electronic devices. The interaction strength between neighbouring layers, most easily controlled through their interlayer separation, can have significant influence on the electronic properties of these composite materials. Here, we demonstrate unprecedented control over interlayer interactions by locally modifying the interlayer separation between graphene and boron nitride, which we achieve by applying pressure with a scanning tunnelling microscopy tip. For the special case of aligned or nearly-aligned graphene on boron nitride, the graphene lattice can stretch and compress locally to compensate for the slight lattice mismatch between the two materials. We find that modifying the interlayer separation directly tunes the lattice strain and induces commensurate stacking underneath the tip. Our results motivate future studies tailoring the electronic properties of van der Waals heterostructures by controlling the interlayer separation of the entire device using hydrostatic pressure. Van der Waals heterostructures enable fabrication of materials with engineered functionalities. Here, the authors demonstrate precise control over the interaction between layers by application of pressure with a scanning tunnelling microscopy tip.

Moiré materials host a wealth of intertwined correlated and topological states of matter, all arising from flat electronic bands with nontrivial quantum geometry. A prominent example is the family of alternating-twist magic-angle graphene stacks, which exhibit symmetry-broken states at rational fillings of the moiré band and superconductivity close to half filling. Here, we introduce a second family of twisted graphene multilayers made up of twisted sheets of M - and N -layer Bernal-stacked graphene flakes. Calculations indicate that applying an electric displacement field isolates a flat and topological moiré conduction band that is primarily localized to a single graphene sheet below the moiré interface. Phenomenologically, the result is a striking similarity in the hierarchies of symmetry-broken phases across this family of twisted graphene multilayers. Our results show that this family of structures offers promising new opportunities for the discovery of exotic new correlated and topological phenomena, enabled by using the layer number to fine tune the flat moiré band and its screening environment. Twisted multilayer graphene structures composed of Bernal-stacked constituents are predicted to host flat moiré bands for several layer-number combinations. Here, the authors find an array of band insulators, correlated insulators, and topological states with notable similarities across different constructions.

A new spectroscopic technique takes advantage of overlapping electronic bands to probe the strongly correlated states of magic-angle twisted trilayer graphene.

The electronic band structure of twisted bilayer graphene develops van Hove singularities whose energy depends on the twist angle between the two layers. Using Raman spectroscopy, we monitor the evolution of the electronic band structure upon doping using the G peak area which is enhanced when the laser photon energy is resonant with the energy separation of the van Hove singularities. Upon charge doping, the Raman G peak area initially increases for twist angles larger than a critical angle and decreases for smaller angles. To explain this behavior with twist angle, the energy separation of the van Hove singularities must decrease with increasing charge density demonstrating the ability to modify the electronic and optical properties of twisted bilayer graphene with doping.

Materials with flat electronic bands often exhibit exotic quantum phenomena owing to strong correlations. An isolated low-energy flat band can be induced in bilayer graphene by simply rotating the layers by 1.1°, resulting in the appearance of gate-tunable superconducting and correlated insulating phases. In this study, we demonstrate that in addition to the twist angle, the interlayer coupling can be varied to precisely tune these phases. We induce superconductivity at a twist angle larger than 1.1°—in which correlated phases are otherwise absent—by varying the interlayer spacing with hydrostatic pressure. Our low-disorder devices reveal details about the superconducting phase diagram and its relationship to the nearby insulator. Our results demonstrate twisted bilayer graphene to be a distinctively tunable platform for exploring correlated states.

Twisted bilayer graphene has recently emerged as a platform for hosting correlated phenomena. For twist angles near θ ≈ 1.1°, the low-energy electronic structure of twisted bilayer graphene features isolated bands with a flat dispersion1,2. Recent experiments have observed a variety of low-temperature phases that appear to be driven by electron interactions, including insulating states, superconductivity and magnetism3–6. Here we report electrical transport measurements up to room temperature for twist angles varying between 0.75° and 2°. We find that the resistivity, ρ, scales linearly with temperature, T, over a wide range of T before falling again owing to interband activation. The T-linear response is much larger than observed in monolayer graphene for all measured devices, and in particular increases by more than three orders of magnitude in the range where the flat band exists. Our results point to the dominant role of electron–phonon scattering in twisted bilayer graphene, with possible implications for the origin of the observed superconductivity.

The flat bands that appear in some twisted van der Waals heterostructures provide a setting in which strong interactions between electrons lead to a variety of correlated phases1–20. In particular, heterostructures of twisted double bilayer graphene host correlated insulating states that can be tuned by both the twist angle and an external electric field11–14. Here, we report electrical transport measurements of twisted double bilayer graphene with which we examine the fundamental role of spontaneous symmetry breaking in its phase diagram. The metallic states near each of the correlated insulators exhibit abrupt drops in their resistivity as the temperature is lowered, along with associated nonlinear current–voltage characteristics. Despite qualitative similarities to superconductivity, the simultaneous reversals in the sign of the Hall coefficient point instead to spontaneous symmetry breaking as the origin of the abrupt resistivity drops, whereas Joule heating seems to underlie the nonlinear transport. Our results suggest that similar mechanisms are probably relevant across a broader class of semiconducting flat band van der Waals heterostructures.Transport measurements show that spontaneous symmetry breaking plays a crucial role in the correlated insulating and metallic states in twisted double bilayer graphene.

As the first in a large family of 2D van der Waals (vdW) materials, graphene has attracted enormous attention owing to its remarkable properties. The recent development of simple experimental techniques for combining graphene with other atomically thin vdW crystals to form heterostructures has enabled the exploration of the properties of these so-called vdW heterostructures. Hexagonal boron nitride is the second most popular vdW material after graphene, owing to the new physics and device properties of vdW heterostructures combining the two. Hexagonal boron nitride can act as a featureless dielectric substrate for graphene, enabling devices with ultralow disorder that allow access to the intrinsic physics of graphene, such as the integer and fractional quantum Hall effects. Additionally, under certain circumstances, hexagonal boron nitride can modify the optical and electronic properties of graphene in new ways, inducing the appearance of secondary Dirac points or driving new plasmonic states. Integrating other vdW materials into these heterostructures and tuning their new degrees of freedom, such as the relative rotation between crystals and their interlayer spacing, provide a path for engineering and manipulating nearly limitless new physics and device properties.This is an overview of the new physics that emerges in van der Waals heterostructures consisting of graphene and hexagonal boron nitride, including the integer and fractional quantum Hall effects, novel plasmonic states and the effects of emergent moiré superlattices.