Van der Waals isotope heterostructures for engineering phonon polariton dispersions.

Element isotopes are characterized by distinct atomic masses and nuclear spins, which can significantly influence material properties. Notably, however, isotopes in natural materials are homogenously distributed in space. Here, we propose a method to configure material properties by repositioning isotopes in engineered van der Waals (vdW) isotopic heterostructures. We showcase the properties of hexagonal boron nitride (hBN) isotopic heterostructures in engineering confined photon-lattice waves-hyperbolic phonon polaritons. By varying the composition, stacking order, and thicknesses of h10BN and h11BN building blocks, hyperbolic phonon polaritons can be engineered into a variety of energy-momentum dispersions. These confined and tailored polaritons are promising for various nanophotonic and thermal functionalities. Due to the universality and importance of isotopes, our vdW isotope heterostructuring method can be applied to engineer the properties of a broad range of materials.

Single-photon detection using high-temperature superconductors.

The detection of individual quanta of light is important for quantum communication, fluorescence lifetime imaging, remote sensing and more. Due to their high detection efficiency, exceptional signal-to-noise ratio and fast recovery times, superconducting-nanowire single-photon detectors (SNSPDs) have become a critical component in these applications. However, the operation of conventional SNSPDs requires costly cryocoolers. Here we report the fabrication of two types of high-temperature superconducting nanowires. We observe linear scaling of the photon count rate on the radiation power at the telecommunications wavelength of 1.5 µm and thereby reveal single-photon operation. SNSPDs made from thin flakes of Bi2Sr2CaCu2O8+δ exhibit a single-photon response up to 25 K, and for SNSPDs from La1.55Sr0.45CuO4/La2CuO4 bilayer films, this response is observed up to 8 K. While the underlying detection mechanism is not fully understood yet, our work expands the family of materials for SNSPD technology beyond the liquid helium temperature limit and suggests that even higher operation temperatures may be reached using other high-temperature superconductors.

Interlayer Electron-Hole Friction in Tunable Twisted Bilayer Graphene Semimetal.

Charge-neutral conducting systems represent a class of materials with unusual properties governed by electron-hole (e-h) interactions. Depending on the quasiparticle statistics, band structure, and device geometry these semimetallic phases of matter can feature unconventional responses to external fields that often defy simple interpretations in terms of single-particle physics. Here we show that small-angle twisted bilayer graphene (SA TBG) offers a highly tunable system in which to explore interactions-limited electron conduction. By employing a dual-gated device architecture we tune our devices from a nondegenerate charge-neutral Dirac fluid to a compensated two-component e-h Fermi liquid where spatially separated electrons and holes experience strong mutual friction. This friction is revealed through the T^{2} resistivity that accurately follows the e-h drag theory we develop. Our results provide a textbook illustration of a smooth transition between different interaction-limited transport regimes and clarify the conduction mechanisms in charge-neutral SA TBG.

Strong Interminivalley Scattering in Twisted Bilayer Graphene Revealed by High-Temperature Magneto-Oscillations.

Twisted bilayer graphene (TBG) provides an example of a system in which the interplay of interlayer interactions and superlattice structure impacts electron transport in a variety of nontrivial ways and gives rise to a plethora of interesting effects. Understanding the mechanisms of electron scattering in TBG has, however, proven challenging, raising many questions about the origins of resistivity in this system. Here we show that TBG exhibits high-temperature magneto-oscillations originating from the scattering of charge carriers between TBG minivalleys. The amplitude of these oscillations reveals that interminivalley scattering is strong, and its characteristic timescale is comparable to that of its intraminivalley counterpart. Furthermore, by exploring the temperature dependence of these oscillations, we estimate the electron-electron collision rate in TBG and find that it exceeds that of monolayer graphene. Our study demonstrates the consequences of the relatively small size of the superlattice Brillouin zone and Fermi velocity reduction on lateral transport in TBG.

Fizeau drag in graphene plasmonics.

Dragging of light by moving media was predicted by Fresnel1 and verified by Fizeau's celebrated experiments2 with flowing water. This momentous discovery is among the experimental cornerstones of Einstein's special relativity theory and is well understood3,4 in the context of relativistic kinematics. By contrast, experiments on dragging photons by an electron flow in solids are riddled with inconsistencies and have so far eluded agreement with the theory5-7. Here we report on the electron flow dragging surface plasmon polaritons8,9 (SPPs): hybrid quasiparticles of infrared photons and electrons in graphene. The drag is visualized directly through infrared nano-imaging of propagating plasmonic waves in the presence of a high-density current. The polaritons in graphene shorten their wavelength when propagating against the drifting carriers. Unlike the Fizeau effect for light, the SPP drag by electrical currents defies explanation by simple kinematics and is linked to the nonlinear electrodynamics of Dirac electrons in graphene. The observed plasmonic Fizeau drag enables breaking of time-reversal symmetry and reciprocity10 at infrared frequencies without resorting to magnetic fields11,12 or chiral optical pumping13,14. The Fizeau drag also provides a tool with which to study interactions and nonequilibrium effects in electron liquids.

Cascade of phase transitions and Dirac revivals in magic-angle graphene.

Twisted bilayer graphene near the magic angle1-4 exhibits rich electron-correlation physics, displaying insulating3-6, magnetic7,8 and superconducting phases4-6. The electronic bands of this system were predicted1,2 to narrow markedly9,10 near the magic angle, leading to a variety of possible symmetry-breaking ground states11-17. Here, using measurements of the local electronic compressibility, we show that these correlated phases originate from a high-energy state with an unusual sequence of band population. As carriers are added to the system, the four electronic 'flavours', which correspond to the spin and valley degrees of freedom, are not filled equally. Rather, they are populated through a sequence of sharp phase transitions, which appear as strong asymmetric jumps of the electronic compressibility near integer fillings of the moiré lattice. At each transition, a single spin/valley flavour takes all the carriers from its partially filled peers, 'resetting' them to the vicinity of the charge neutrality point. As a result, the Dirac-like character observed near charge neutrality reappears after each integer filling. Measurement of the in-plane magnetic field dependence of the chemical potential near filling factor one reveals a large spontaneous magnetization, further substantiating this picture of a cascade of symmetry breaking. The sequence of phase transitions and Dirac revivals is observed at temperatures well above the onset of the superconducting and correlated insulating states. This indicates that the state that we report here, with its strongly broken electronic flavour symmetry and revived Dirac-like electronic character, is important in the physics of magic-angle graphene, forming the parent state out of which the more fragile superconducting and correlated insulating ground states emerge.

Mapping the twist-angle disorder and Landau levels in magic-angle graphene.

The recently discovered flat electronic bands and strongly correlated and superconducting phases in magic-angle twisted bilayer graphene (MATBG)1,2 crucially depend on the interlayer twist angle, θ. Although control of the global θ with a precision of about 0.1 degrees has been demonstrated1-7, little information is available on the distribution of the local twist angles. Here we use a nanoscale on-tip scanning superconducting quantum interference device (SQUID-on-tip)8 to obtain tomographic images of the Landau levels in the quantum Hall state9 and to map the local θ variations in hexagonal boron nitride (hBN)-encapsulated MATBG devices with relative precision better than 0.002 degrees and a spatial resolution of a few moiré periods. We find a correlation between the degree of θ disorder and the quality of the MATBG transport characteristics and show that even state-of-the-art devices-which exhibit correlated states, Landau fans and superconductivity-display considerable local variation in θ of up to 0.1 degrees, exhibiting substantial gradients and networks of jumps, and may contain areas with no local MATBG behaviour. We observe that the correlated states in MATBG are particularly fragile with respect to the twist-angle disorder. We also show that the gradients of θ generate large gate-tunable in-plane electric fields, unscreened even in the metallic regions, which profoundly alter the quantum Hall state by forming edge channels in the bulk of the sample and may affect the phase diagram of the correlated and superconducting states. We thus establish the importance of θ disorder as an unconventional type of disorder enabling the use of twist-angle gradients for bandstructure engineering, for realization of correlated phenomena and for gate-tunable built-in planar electric fields for device applications.

Electronic Compressibility of Magic-Angle Graphene Superlattices.

We report the first electronic compressibility measurements of magic-angle twisted bilayer graphene. The evolution of the compressibility with carrier density offers insights into the interaction-driven ground state that have not been accessible in prior transport and tunneling studies. From capacitance measurements, we determine the chemical potential as a function of carrier density and find the widths of the energy gaps at fractional filling of the moiré lattice. In the electron-doped regime, we observe unexpectedly large gaps at quarter- and half-filling and strong electron-hole asymmetry. Moreover, we measure a ∼35 meV minibandwidth that is much wider than most theoretical estimates. Finally, we explore the field dependence up to the quantum Hall regime and observe significant differences from transport measurements.

Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling.

Magnetic insulators are a key resource for next-generation spintronic and topological devices. The family of layered metal halides promises varied magnetic states, including ultrathin insulating multiferroics, spin liquids, and ferromagnets, but device-oriented characterization methods are needed to unlock their potential. Here, we report tunneling through the layered magnetic insulator CrI3 as a function of temperature and applied magnetic field. We electrically detect the magnetic ground state and interlayer coupling and observe a field-induced metamagnetic transition. The metamagnetic transition results in magnetoresistances of 95, 300, and 550% for bilayer, trilayer, and tetralayer CrI3 barriers, respectively. We further measure inelastic tunneling spectra for our junctions, unveiling a rich spectrum consistent with collective magnetic excitations (magnons) in CrI3.

Observation of Exciton Redshift-Blueshift Crossover in Monolayer WS2.

We report a rare atom-like interaction between excitons in monolayer WS2, measured using ultrafast absorption spectroscopy. At increasing excitation density, the exciton resonance energy exhibits a pronounced redshift followed by an anomalous blueshift. Using both material-realistic computation and phenomenological modeling, we attribute this observation to plasma effects and an attraction-repulsion crossover of the exciton-exciton interaction that mimics the Lennard-Jones potential between atoms. Our experiment demonstrates a strong analogy between excitons and atoms with respect to interparticle interaction, which holds promise to pursue the predicted liquid and crystalline phases of excitons in two-dimensional materials.

Superlattice-Induced Insulating States and Valley-Protected Orbits in Twisted Bilayer Graphene.

Twisted bilayer graphene (TBLG) is one of the simplest van der Waals heterostructures, yet it yields a complex electronic system with intricate interplay between moiré physics and interlayer hybridization effects. We report on electronic transport measurements of high mobility small angle TBLG devices showing clear evidence for insulating states at the superlattice band edges, with thermal activation gaps several times larger than theoretically predicted. Moreover, Shubnikov-de Haas oscillations and tight binding calculations reveal that the band structure consists of two intersecting Fermi contours whose crossing points are effectively unhybridized. We attribute this to exponentially suppressed interlayer hopping amplitudes for momentum transfers larger than the moiré wave vector.

TOPOLOGICAL MATTER. Observation of chiral currents at the magnetic domain boundary of a topological insulator.

A magnetic domain boundary on the surface of a three-dimensional topological insulator is predicted to host a chiral edge state, but direct demonstration is challenging. We used a scanning superconducting quantum interference device to show that current in a magnetized topological insulator heterostructure (EuS/Bi2Se3) flows at the edge when the Fermi level is gate-tuned to the surface band gap. We further induced micrometer-scale magnetic structures on the heterostructure and detected a chiral edge current at the magnetic domain boundary. The chirality of the current was determined by magnetization of the surrounding domain, and its magnitude by the local chemical potential rather than the applied current. Such magnetic structures provide a platform for detecting topological magnetoelectric effects and may enable progress in quantum information processing and spintronics.

Graphene on hexagonal boron nitride as a tunable hyperbolic metamaterial.

Hexagonal boron nitride (h-BN) is a natural hyperbolic material, in which the dielectric constants are the same in the basal plane (ε(t) ≡ ε(x) = ε(y)) but have opposite signs (ε(t)ε(z) < 0) in the normal plane (ε(z)). Owing to this property, finite-thickness slabs of h-BN act as multimode waveguides for the propagation of hyperbolic phonon polaritons--collective modes that originate from the coupling between photons and electric dipoles in phonons. However, control of these hyperbolic phonon polaritons modes has remained challenging, mostly because their electrodynamic properties are dictated by the crystal lattice of h-BN. Here we show, by direct nano-infrared imaging, that these hyperbolic polaritons can be effectively modulated in a van der Waals heterostructure composed of monolayer graphene on h-BN. Tunability originates from the hybridization of surface plasmon polaritons in graphene with hyperbolic phonon polaritons in h-BN, so that the eigenmodes of the graphene/h-BN heterostructure are hyperbolic plasmon-phonon polaritons. The hyperbolic plasmon-phonon polaritons in graphene/h-BN suffer little from ohmic losses, making their propagation length 1.5-2.0 times greater than that of hyperbolic phonon polaritons in h-BN. The hyperbolic plasmon-phonon polaritons possess the combined virtues of surface plasmon polaritons in graphene and hyperbolic phonon polaritons in h-BN. Therefore, graphene/h-BN can be classified as an electromagnetic metamaterial as the resulting properties of these devices are not present in its constituent elements alone.

Subdiffractional focusing and guiding of polaritonic rays in a natural hyperbolic material.

Uniaxial materials whose axial and tangential permittivities have opposite signs are referred to as indefinite or hyperbolic media. In such materials, light propagation is unusual leading to novel and often non-intuitive optical phenomena. Here we report infrared nano-imaging experiments demonstrating that crystals of hexagonal boron nitride, a natural mid-infrared hyperbolic material, can act as a 'hyper-focusing lens' and as a multi-mode waveguide. The lensing is manifested by subdiffractional focusing of phonon-polaritons launched by metallic disks underneath the hexagonal boron nitride crystal. The waveguiding is revealed through the modal analysis of the periodic patterns observed around such launchers and near the sample edges. Our work opens new opportunities for anisotropic layered insulators in infrared nanophotonics complementing and potentially surpassing concurrent artificial hyperbolic materials with lower losses and higher optical localization.

Hot-carrier photocurrent effects at graphene-metal interfaces.

Photoexcitation of graphene leads to an interesting sequence of phenomena, some of which can be exploited in optoelectronic devices based on graphene. In particular, the efficient and ultrafast generation of an electron distribution with an elevated electron temperature and the concomitant generation of a photo-thermoelectric voltage at symmetry-breaking interfaces is of interest for photosensing and light harvesting. Here, we experimentally study the generated photocurrent at the graphene-metal interface, focusing on the time-resolved photocurrent, the effects of photon energy, Fermi energy and light polarization. We show that a single framework based on photo-thermoelectric photocurrent generation explains all experimental results.

Generation of photovoltage in graphene on a femtosecond timescale through efficient carrier heating.

Graphene is a promising material for ultrafast and broadband photodetection. Earlier studies have addressed the general operation of graphene-based photothermoelectric devices and the switching speed, which is limited by the charge carrier cooling time, on the order of picoseconds. However, the generation of the photovoltage could occur at a much faster timescale, as it is associated with the carrier heating time. Here, we measure the photovoltage generation time and find it to be faster than 50 fs. As a proof-of-principle application of this ultrafast photodetector, we use graphene to directly measure, electrically, the pulse duration of a sub-50 fs laser pulse. The observation that carrier heating is ultrafast suggests that energy from absorbed photons can be efficiently transferred to carrier heat. To study this, we examine the spectral response and find a constant spectral responsivity of between 500 and 1,500 nm. This is consistent with efficient electron heating. These results are promising for ultrafast femtosecond and broadband photodetector applications.

Tunable phonon polaritons in atomically thin van der Waals crystals of boron nitride.

van der Waals heterostructures assembled from atomically thin crystalline layers of diverse two-dimensional solids are emerging as a new paradigm in the physics of materials. We used infrared nanoimaging to study the properties of surface phonon polaritons in a representative van der Waals crystal, hexagonal boron nitride. We launched, detected, and imaged the polaritonic waves in real space and altered their wavelength by varying the number of crystal layers in our specimens. The measured dispersion of polaritonic waves was shown to be governed by the crystal thickness according to a scaling law that persists down to a few atomic layers. Our results are likely to hold true in other polar van der Waals crystals and may lead to new functionalities.

Tunable symmetry breaking and helical edge transport in a graphene quantum spin Hall state.

Low-dimensional electronic systems have traditionally been obtained by electrostatically confining electrons, either in heterostructures or in intrinsically nanoscale materials such as single molecules, nanowires and graphene. Recently, a new method has emerged with the recognition that symmetry-protected topological (SPT) phases, which occur in systems with an energy gap to quasiparticle excitations (such as insulators or superconductors), can host robust surface states that remain gapless as long as the relevant global symmetry remains unbroken. The nature of the charge carriers in SPT surface states is intimately tied to the symmetry of the bulk, resulting in one- and two-dimensional electronic systems with novel properties. For example, time reversal symmetry endows the massless charge carriers on the surface of a three-dimensional topological insulator with helicity, fixing the orientation of their spin relative to their momentum. Weakly breaking this symmetry generates a gap on the surface, resulting in charge carriers with finite effective mass and exotic spin textures. Analogous manipulations have yet to be demonstrated in two-dimensional topological insulators, where the primary example of a SPT phase is the quantum spin Hall state. Here we demonstrate experimentally that charge-neutral monolayer graphene has a quantum spin Hall state when it is subjected to a very large magnetic field angled with respect to the graphene plane. In contrast to time-reversal-symmetric systems, this state is protected by a symmetry of planar spin rotations that emerges as electron spins in a half-filled Landau level are polarized by the large magnetic field. The properties of the resulting helical edge states can be modulated by balancing the applied field against an intrinsic antiferromagnetic instability, which tends to spontaneously break the spin-rotation symmetry. In the resulting canted antiferromagnetic state, we observe transport signatures of gapped edge states, which constitute a new kind of one-dimensional electronic system with a tunable bandgap and an associated spin texture.

Observation of Floquet-Bloch states on the surface of a topological insulator.

The unique electronic properties of the surface electrons in a topological insulator are protected by time-reversal symmetry. Circularly polarized light naturally breaks time-reversal symmetry, which may lead to an exotic surface quantum Hall state. Using time- and angle-resolved photoemission spectroscopy, we show that an intense ultrashort midinfrared pulse with energy below the bulk band gap hybridizes with the surface Dirac fermions of a topological insulator to form Floquet-Bloch bands. These photon-dressed surface bands exhibit polarization-dependent band gaps at avoided crossings. Circularly polarized photons induce an additional gap at the Dirac point, which is a signature of broken time-reversal symmetry on the surface. These observations establish the Floquet-Bloch bands in solids and pave the way for optical manipulation of topological quantum states of matter.

Massive Dirac fermions and Hofstadter butterfly in a van der Waals heterostructure.

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.