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.

Kagome Quantum Oscillations in Graphene Superlattices.

Electronic spectra of solids subjected to a magnetic field are often discussed in terms of Landau levels and Hofstadter-butterfly-style Brown-Zak minibands manifested by magneto-oscillations in two-dimensional electron systems. Here, we present the semiclassical precursors of these quantum magneto-oscillations which appear in graphene superlattices at low magnetic field near the Lifshitz transitions and persist at elevated temperatures. These oscillations originate from Aharonov-Bohm interference of electron waves following open trajectories that belong to a kagome-shaped network of paths characteristic for Lifshitz transitions in the moire superlattice minibands of twistronic graphenes.

Mixing of moiré-surface and bulk states in graphite.

Van der Waals assembly enables the design of electronic states in two-dimensional (2D) materials, often by superimposing a long-wavelength periodic potential on a crystal lattice using moiré superlattices1-9. This twistronics approach has resulted in numerous previously undescribed physics, including strong correlations and superconductivity in twisted bilayer graphene10-12, resonant excitons, charge ordering and Wigner crystallization in transition-metal chalcogenide moiré structures13-18 and Hofstadter's butterfly spectra and Brown-Zak quantum oscillations in graphene superlattices19-22. Moreover, twistronics has been used to modify near-surface states at the interface between van der Waals crystals23,24. Here we show that electronic states in three-dimensional (3D) crystals such as graphite can be tuned by a superlattice potential occurring at the interface with another crystal-namely, crystallographically aligned hexagonal boron nitride. This alignment results in several Lifshitz transitions and Brown-Zak oscillations arising from near-surface states, whereas, in high magnetic fields, fractal states of Hofstadter's butterfly draw deep into the bulk of graphite. Our work shows a way in which 3D spectra can be controlled using the approach of 2D twistronics.

Giant orbital magnetic moments and paramagnetic shift in artificial relativistic atoms and molecules.

Materials such as graphene and topological insulators host massless Dirac fermions that enable the study of relativistic quantum phenomena. Single quantum dots and coupled quantum dots formed with massless Dirac fermions can be viewed as artificial relativistic atoms and molecules, respectively. Such structures offer a unique testbed to study atomic and molecular physics in the ultrarelativistic regime (particle speed close to the speed of light). Here we use a scanning tunnelling microscope to create and probe single and coupled electrostatically defined graphene quantum dots to unravel the magnetic-field responses of artificial relativistic nanostructures. We observe a giant orbital Zeeman splitting and orbital magnetic moment up to ~70 meV T-1 and ~600µB (µB, Bohr magneton) in single graphene quantum dots. For coupled graphene quantum dots, Aharonov-Bohm oscillations and a strong Van Vleck paramagnetic shift of ~20 meV T-2 are observed. Our findings provide fundamental insights into relativistic quantum dot states, which can be potentially leveraged for use in quantum information science.

Out-of-equilibrium criticalities in graphene superlattices.

In thermodynamic equilibrium, current in metallic systems is carried by electronic states near the Fermi energy, whereas the filled bands underneath contribute little to conduction. Here, we describe a very different regime in which carrier distribution in graphene and its superlattices is shifted so far from equilibrium that the filled bands start playing an essential role, leading to a critical-current behavior. The criticalities develop upon the velocity of electron flow reaching the Fermi velocity. Key signatures of the out-of-equilibrium state are current-voltage characteristics that resemble those of superconductors, sharp peaks in differential resistance, sign reversal of the Hall effect, and a marked anomaly caused by the Schwinger-like production of hot electron-hole plasma. The observed behavior is expected to be common to all graphene-based superlattices.

Control of Giant Topological Magnetic Moment and Valley Splitting in Trilayer Graphene.

Bloch states of electrons in honeycomb two-dimensional crystals with multivalley band structure and broken inversion symmetry have orbital magnetic moments of a topological nature. In crystals with two degenerate valleys, a perpendicular magnetic field lifts the valley degeneracy via a Zeeman effect due to these magnetic moments, leading to magnetoelectric effects which can be leveraged for creating valleytronic devices. In this work, we demonstrate that trilayer graphene with Bernal stacking (ABA TLG), hosts topological magnetic moments with a large and widely tunable valley g factor (g_{ν}), reaching a value g_{ν}∼1050 at the extreme of the studied parametric range. The reported experiment consists in sublattice-resolved scanning tunneling spectroscopy under perpendicular electric and magnetic fields that control the TLG bands. The tunneling spectra agree very well with the results of theoretical modeling that includes the full details of the TLG tight-binding model and accounts for a quantum-dot-like potential profile formed electrostatically under the scanning tunneling microscope tip.

Out-of-Plane Dielectric Susceptibility of Graphene in Twistronic and Bernal Bilayers.

We describe how the out-of-plane dielectric polarizability of monolayer graphene influences the electrostatics of bilayer graphene-both Bernal (BLG) and twisted (tBLG). We compare the polarizability value computed using density functional theory with the output from previously published experimental data on the electrostatically controlled interlayer asymmetry potential in BLG and data on the on-layer density distribution in tBLG. We show that monolayers in tBLG are described well by polarizability αexp = 10.8 Å3 and effective out-of-plane dielectric susceptibility ϵz = 2.5, including their on-layer electron density distribution at zero magnetic field and the interlayer Landau level pinning at quantizing magnetic fields.

Electronic phase separation in multilayer rhombohedral graphite.

Of the two stable forms of graphite, hexagonal and rhombohedral, the former is more common and has been studied extensively. The latter is less stable, which has so far precluded its detailed investigation, despite many theoretical predictions about the abundance of exotic interaction-induced physics1-6. Advances in van der Waals heterostructure technology7 have now allowed us to make high-quality rhombohedral graphite films up to 50 graphene layers thick and study their transport properties. Here we show that the bulk electronic states in such rhombohedral graphite are gapped8 and, at low temperatures, electron transport is dominated by surface states. Because of their proposed topological nature, the surface states are of sufficiently high quality to observe the quantum Hall effect, whereby rhombohedral graphite exhibits phase transitions between a gapless semimetallic phase and a gapped quantum spin Hall phase with giant Berry curvature. We find that an energy gap can also be opened in the surface states by breaking their inversion symmetry by applying a perpendicular electric field. Moreover, in rhombohedral graphite thinner than four nanometres, a gap is present even without an external electric field. This spontaneous gap opening shows pronounced hysteresis and other signatures characteristic of electronic phase separation, which we attribute to emergence of strongly correlated electronic surface states.

Spectroscopic Signatures of Electronic Excitations in Raman Scattering in Thin Films of Rhombohedral Graphite.

Rhombohedral graphite features peculiar electronic properties, including persistence of low-energy surface bands of a topological nature. Here, we study the contribution of electron-hole excitations toward inelastic light scattering in thin films of rhombohedral graphite. We show that, in contrast to the featureless electron-hole contribution toward Raman spectrum of graphitic films with Bernal stacking, the inelastic light scattering accompanied by electron-hole excitations in crystals with rhombohedral stacking produces distinct features in the Raman signal which can be used both to identify the stacking and to determine the number of layers in the film.

Transport Through a Network of Topological Channels in Twisted Bilayer Graphene.

We explore a network of electronic quantum valley Hall states in the moiré crystal of minimally twisted bilayer graphene. In our transport measurements, we observe Fabry-Pérot and Aharanov-Bohm oscillations that are robust in magnetic fields ranging from 0 to 8 T, which is in strong contrast to more conventional two-dimensional systems where trajectories in the bulk are bent by the Lorentz force. This persistence in magnetic field and the linear spacing in density indicate that charge carriers in the bulk flow in topologically protected, one-dimensional channels. With this work, we demonstrate coherent electronic transport in a lattice of topologically protected states.

Magnetoresistance in Co-hBN-NiFe Tunnel Junctions Enhanced by Resonant Tunneling through Single Defects in Ultrathin hBN Barriers.

Hexagonal boron nitride (hBN) is a prototypical high-quality two-dimensional insulator and an ideal material to study tunneling phenomena, as it can be easily integrated in vertical van der Waals devices. For spintronic devices, its potential has been demonstrated both for efficient spin injection in lateral spin valves and as a barrier in magnetic tunnel junctions (MTJs). Here we reveal the effect of point defects inevitably present in mechanically exfoliated hBN on the tunnel magnetoresistance of Co-hBN-NiFe MTJs. We observe a clear enhancement of both the conductance and magnetoresistance of the junction at well-defined bias voltages, indicating resonant tunneling through magnetic (spin-polarized) defect states. The spin polarization of the defect states is attributed to exchange coupling of a paramagnetic impurity in the few-atomic-layer thick hBN to the ferromagnetic electrodes. This is confirmed by excellent agreement with theoretical modeling. Our findings should be taken into account in analyzing tunneling processes in hBN-based magnetic devices. More generally, our study shows the potential of using atomically thin hBN barriers with defects to engineer the magnetoresistance of MTJs and to achieve spin filtering, opening the door toward exploiting the spin degree of freedom in current studies of point defects as quantum emitters.

Electrostatically Induced Quantum Point Contacts in Bilayer Graphene.

We report the fabrication of electrostatically defined nanostructures in encapsulated bilayer graphene, with leakage resistances below depletion gates as high as R ∼ 10 GΩ. This exceeds previously reported values of R = 10-100 kΩ.1-3 We attribute this improvement to the use of a graphite back gate. We realize two split gate devices which define an electronic channel on the scale of the Fermi-wavelength. A channel gate covering the gap between the split gates varies the charge carrier density in the channel. We observe device-dependent conductance quantization of ΔG = 2e2/h and ΔG = 4e2/h. In quantizing magnetic fields normal to the sample plane, we recover the four-fold Landau level degeneracy of bilayer graphene. Unexpected mode crossings appear at the crossover between zero magnetic field and the quantum Hall regime.

Magnetic fluctuations and specific heat in Na(x)CoO2 near a Lifshitz transition.

We analyze the temperature and doping dependence of the specific heat C(T) in Na(x)CoO(2). This material was conjectured to undergo a Lifshitz-type topological transition at x=x(c)=0.62, in which a new electron Fermi pocket emerges at the Γ point, in addition to the existing hole pocket with large k(F). The data show that near x=x(c), the temperature dependence of C(T)/T at low T gets stronger as x approaches x(c) from below and then reverses the trend and changes sign at x≥x(c). We argue that this behavior can be quantitatively explained within the spin-fluctuation theory. We show that magnetic fluctuations are enhanced near x(c) at momenta around k(F), and their dynamics changes between x≤x(c) and x>x(c), when the new pocket forms. We demonstrate that this explains the temperature dependence of C(T)/T. We show that at larger x (x>0.65) the system enters a magnetic quantum critical regime where C(T)/T roughly scales as logT. This behavior extends to progressively lower T as x increases towards a magnetic instability at x≈0.75.

Charging of graphene by a magnetic field and the mechanical effect of magnetic oscillations.

We discuss the fact that the quantum capacitance of graphene-based devices leads to variation of graphene charge density under changes of external magnetic field. The charge is conserved, but redistributes to the substrate or other graphene sheets. We derive an exact analytic expression for charge redistribution in the case of ideal graphene in a strong magnetic field. When we account for impurities and temperature, the effect decreases and the formulas reduce to standard quantum capacitance expressions. The importance of quantum capacitance for potential Casimir force experiments is emphasized and the corresponding corrections are worked out.