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In recent years, correlated insulating states, unconventional superconductivity, and topologically non-trivial phases have all been observed in several moiré heterostructures. However, understanding of the physical mechanisms behind these phenomena is hampered by the lack of local electronic structure data. Here, we use scanning tunnelling microscopy and spectroscopy to demonstrate how the interplay between correlation, topology, and local atomic structure determines the behaviour of electron-doped twisted monolayer–bilayer graphene. Through gate- and magnetic field-dependent measurements, we observe local spectroscopic signatures indicating a quantum anomalous Hall insulating state with a total Chern number of ±2 at a doping level of three electrons per moiré unit cell. We show that the sign of the Chern number and associated magnetism can be electrostatically switched only over a limited range of twist angle and sample hetero-strain values. This results from a competition between the orbital magnetization of filled bulk bands and chiral edge states, which is sensitive to strain-induced distortions in the moiré superlattice.

 

Interacting electrons in flat bands give rise to a variety of quantum phases. One fundamental aspect of such states is the ordering of the various flavours—such as spin or valley—that the electrons can possess and the excitation spectrum of the broken-symmetry states that they form. These properties cannot be probed directly with electrical transport measurements. The zeroth Landau level of monolayer graphene with fourfold spin–valley degeneracy is a model system for such investigations, but the nature of its broken-symmetry states—particularly at partial fillings—is still not understood. Here we demonstrate a non-invasive spectroscopic technique with a scanning tunnelling microscope and use it to perform measurements of the valley polarization of the electronic wavefunctions and their excitation spectrum in the partially filled zeroth Landau level of graphene. We can extract information such as the strength of the Haldane pseudopotentials that characterize the repulsive interactions underlying the fractional quantum states. Our experiments also demonstrate that fractional quantum Hall phases are built upon broken-symmetry states that persist at partial filling. Our experimental approach quantifies the valley phase diagram of the partially filled Landau level as a model flat-band platform, which is applicable to other graphene-based electronic systems. 

Scanning tunneling spectroscopy is used to image valley ordering in graphene in the presence of a magnetic field. 

Abstract The discovery of interaction-driven insulating and superconducting phases in moiré van der Waals heterostructures has sparked considerable interest in understanding the novel correlated physics of these systems. While a significant number of studies have focused on twisted bilayer graphene, correlated insulating states and a superconductivity-like transition up to 12 K have been reported in recent transport measurements of twisted double bilayer graphene. Here we present a scanning tunneling microscopy and spectroscopy study of gate-tunable twisted double bilayer graphene devices. We observe splitting of the van Hove singularity peak by ~20 meV at half-filling of the conduction flat band, with a corresponding reduction of the local density of states at the Fermi level. By mapping the tunneling differential conductance we show that this correlated system exhibits energetically split states that are spatially delocalized throughout the different regions in the moiré unit cell, inconsistent with order originating solely from onsite Coulomb repulsion within strongly-localized orbitals. We have performed self-consistent Hartree-Fock calculations that suggest exchange-driven spontaneous symmetry breaking in the degenerate conduction flat band is the origin of the observed correlated state. Our results provide new insight into the nature of electron-electron interactions in twisted double bilayer graphene and related moiré systems.