van der Waals heterostructures constitute a new class of artificial materials formed by stacking atomically thin planar crystals. We demonstrated band structure engineering in a van der Waals heterostructure composed of a monolayer graphene flake coupled to a rotationally aligned hexagonal boron nitride substrate. The spatially varying interlayer atomic registry results in both a local breaking of the carbon sublattice symmetry and a long-range moiré superlattice potential in the graphene. In our samples, this interplay between short- and long-wavelength effects resulted in a band structure described by isolated superlattice minibands and an unexpectedly large band gap at charge neutrality. This picture is confirmed by our observation of fractional quantum Hall states at ± 5/3 filling and features associated with the Hofstadter butterfly at ultrahigh magnetic fields.

Electrons moving through a spatially periodic lattice potential develop a quantized energy spectrum consisting of discrete Bloch bands. In two dimensions, electrons moving through a magnetic field also develop a quantized energy spectrum, consisting of highly degenerate Landau energy levels. When subject to both a magnetic field and a periodic electrostatic potential, two-dimensional systems of electrons exhibit a self-similar recursive energy spectrum. Known as Hofstadter's butterfly, this complex spectrum results from an interplay between the characteristic lengths associated with the two quantizing fields, and is one of the first quantum fractals discovered in physics. In the decades since its prediction, experimental attempts to study this effect have been limited by difficulties in reconciling the two length scales. Typical atomic lattices (with periodicities of less than one nanometre) require unfeasibly large magnetic fields to reach the commensurability condition, and in artificially engineered structures (with periodicities greater than about 100 nanometres) the corresponding fields are too small to overcome disorder completely. Here we demonstrate that moiré superlattices arising in bilayer graphene coupled to hexagonal boron nitride provide a periodic modulation with ideal length scales of the order of ten nanometres, enabling unprecedented experimental access to the fractal spectrum. We confirm that quantum Hall features associated with the fractal gaps are described by two integer topological quantum numbers, and report evidence of their recursive structure. Observation of a Hofstadter spectrum in bilayer graphene means that it is possible to investigate emergent behaviour within a fractal energy landscape in a system with tunable internal degrees of freedom.

We theoretically study the optical absorption property of twisted bilayer graphenes with various stacking geometries, and demonstrate that the spectroscopic characteristics serve as a fingerprint to identify the rotation angle between two layers. We find that the absorption spectrum almost continuously evolves in changing the rotation angle, regardless of the lattice commensurability. The spectrum is characterized by series of peaks associated with the van Hove singularity, and the peak energies systematically shift with the rotation angle. We calculate the optical absorption in two different frameworks; the tight-binding model and the effective continuum model based on the Dirac equation. For small rotation angles less than 10 • , the effective model well reproduces the lowenergy band structure and the optical conductivity of the tight-binding model, and also explains the optical selection rule analytically in terms of the symmetry of the effective Hamiltonian.

We investigate the electronic structure and the quantum Hall effect in twisted bilayer graphenes with various rotation angles in the presence of magnetic field. Using a low-energy approximation, which incorporates the rigorous interlayer interaction, we computed the energy spectrum and the quantized Hall conductivity in a wide range of magnetic field from the semi-classical regime to the fractal spectrum regime. In weak magnetic fields, the low-energy conduction band is quantized into electronlike and holelike Landau levels at energies below and above the van Hove singularity, respectively, and the Hall conductivity sharply drops from positive to negative when the Fermi energy goes through the transition point. In increasing magnetic field, the spectrum gradually evolves into a fractal band structure called Hofstadter's butterfly, where the Hall conductivity exhibits a nonmonotonic behavior as a function of Fermi energy. The typical electron density and magnetic field amplitude characterizing the spectrum monotonically decrease as the rotation angle is reduced, indicating that the rich electronic structure may be observed in a moderate condition.

We theoretically investigate the electronic structures of moiré superlattices arising in monolayer / bilayer graphene stacked on hexagonal boron nitride (hBN) in presence and absence of magnetic field. We develop an effective continuum model from a microscopic tight-binding lattice Hamiltonian, and calculate the electronic structures of graphene-hBN systems with different rotation angles. Using the effective model, we explain the characteristic band properties such as the gap opening at the corners of the superlattice Brillouin zone (mini-Dirac point). We also investigate the energy spectrum and quantum Hall effect of graphene-hBN systems in uniform magnetic field and demonstrate the evolution of the fractal spectrum as a function of the magnetic field. The spectrum generally splits in the valley degrees of freedom (K and K ′ ) due to the lack of the inversion symmetry, and the valley splitting is more significant in bilayer graphene on hBN than in monolayer graphene on hBN because of the stronger inversion-symmetry breaking in bilayer.

The emergence of flat electronic bands and of the recently discovered strongly correlated and superconducting phases in twisted bilayer graphene crucially depends on the interlayer twist angle upon approaching the magic angle ߠ ெ ≈ 1.1°. Although advanced fabrication methods allow alignment of graphene layers with global twist angle control of about 0.1°, little information is currently available on the distribution of the local twist angles in actual magic angle twisted bilayer graphene (MATBG) transport devices. Here we map the local ߠ variations in hBN encapsulated devices with relative precision better than 0.002° and spatial resolution of a few moiré periods. Utilizing a scanning nanoSQUID-on-tip, we attain tomographic imaging of the Landau levels in the quantum Hall state in MATBG, which provides a highly sensitive probe of the charge disorder and of the local band structure determined by the local ߠ. We find a correlation between the degree of twist angle disorder and the quality of the typical MATBG transport characteristics. However, even state-of-the-art transport devices, exhibiting pronounced global MATBG features, such as multiple correlated insulator states, high-quality Landau fan diagrams, and superconductivity, display significant variations in the local ߠ with a span that can be close to 0.1°. Devices may even have substantial areas where no local MATBG behavior is detected, yet still display global MATBG characteristics in transport, highlighting the importance of percolation physics. The derived ߠ maps reveal substantial gradients and a network of jumps. We show that the twist angle gradients generate large unscreened electric fields that drastically change the quantum Hall state by forming edge states in the bulk of the sample, and may also significantly affect the phase diagram of correlated and superconducting states. The findings call for exploration of band structure engineering utilizing twist-angle gradients and gate-tunable built-in planar electric fields for novel correlated phenomena and applications.

Quantum states of quasiparticles in solids are dictated by symmetry. We have experimentally demonstrated quantum states of Dirac electrons in a two-dimensional quasicrystal without translational symmetry. A dodecagonal quasicrystalline order was realized by epitaxial growth of twisted bilayer graphene rotated exactly 30°. We grew the graphene quasicrystal up to a millimeter scale on a silicon carbide surface while maintaining the single rotation angle over an entire sample and successfully isolated the quasicrystal from a substrate, demonstrating its structural and chemical stability under ambient conditions. Multiple Dirac cones replicated with the 12-fold rotational symmetry were observed in angle-resolved photoemission spectra, which revealed anomalous strong interlayer coupling with quasi-periodicity. Our study provides a way to explore physical properties of relativistic fermions with controllable quasicrystalline orders.

The ability to manipulate electrons in two-dimensional materials with external electric fields provides a route to synthetic band engineering. By imposing artificially designed and spatially periodic superlattice potentials, electronic properties can be further altered beyond the constraints of naturally occurring atomic crystals. Here, we report a new approach to fabricate high-mobility superlattice devices by integrating surface dielectric patterning with atomically thin van der Waals materials. By separating the device assembly and superlattice fabrication processes, we address the intractable trade-off between device processing and mobility degradation that constrains superlattice engineering in conventional systems. The improved electrostatics of atomically thin materials allows smaller wavelength superlattice patterns relative to previous demonstrations. Moreover, we observe the formation of replica Dirac cones in ballistic graphene devices with sub-40 nm wavelength superlattices and report fractal Hofstadter spectra under large magnetic fields from superlattices with designed lattice symmetries that differ from that of the host crystal. Our results establish a robust and versatile technique for band structure engineering of graphene and related van der Waals materials with dynamic tunability.