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Josephson junctions (JJs) are ubiquitous superconducting devices, enabling high sensitivity magnetometers and voltage amplifiers, as well as forming the basis of high performance cryogenic computer and superconducting quantum computers. While JJ performance can be degraded by quasiparticles (QPs) formed from broken Cooper pairs, this phenomenon also opens opportunities to sensitively detect electromagnetic radiation. Here we demonstrate single near-infrared photon detection by coupling photons to the localized surface plasmons of a graphene-based JJ. Using the photon-induced switching statistics of the current-biased JJ, we reveal the critical role of QPs generated by the absorbed photon in the detection mechanism. The photon-sensitive JJ will enable a high-speed, low-power optical interconnect for future JJ-based computing architectures., Comment: 12 pages, 9 figures, and 4 tables

Combining various two-dimensional materials into novel van der Waals (vdW) heterostructures has been shown to lead to new emergent quantum systems. A novel heterostructure composed of a vdW topological insulator (TI) such as Bi$_{2}$Se$_{3}$ with a quantum spin liquid (QSL) such as $\alpha$-RuCl$_{3}$ is of great interest for the potential for the chiral Dirac electrons in the TI surface states to interact strongly with the fractionalized fermionic spin excitations in the QSL. We report the heteroepitaxial growth of Bi$_{2}$Se$_{3}$ thin films on $\alpha$-RuCl$_{3}$ as well as the characterization of their structural and electrical properties. Bi$_{2}$Se$_{3}$ thin films with an atomically smooth and uniform surface are grown by molecular beam epitaxy. The heterostructure exhibits a preferential epitaxial relationship corresponding to $(5 \times 5)-$Bi$_{2}$Se$_{3}/(2\sqrt{3} \times 2\sqrt{3})R30\deg-\alpha$-RuCl$_{3}$ commensurate supercells with a periodicity of 1.2 nm. The formation of the superlattice despite a lattice mismatch as large as 60% is attributed to the van der Waals heteroepitaxy. Magnetotransport measurements as a function of temperature show Bi$_{2}$Se$_{3}$ films grown on $\alpha$-RuCl$_{3}$ are heavily $n$-doped, $n_{e}$ ~10$^{14}$ cm$^{-2}$, with mobility $\mu$ ~450 cm$^{2}$ V$^{-1}$ s$^{-1}$ at low temperatures., Comment: 19 pages, 4 figures; accepted in Physical Review Materials

A Wigner crystal, a regular electron lattice arising from strong correlation effects, is one of the earliest predicted collective electronic states. This many-body state exhibits quantum and classical phase transitions and has been proposed as a basis for quantum information processing applications. In semiconductor platforms, two-dimensional Wigner crystals have been observed under magnetic field or moir\'e-based lattice potential where the electron kinetic energy is strongly suppressed. Here, we report bilayer Wigner crystal formation without a magnetic or confinement field in atomically thin MoSe$_2$ bilayers separated by hexagonal boron nitride. We observe optical signatures of robust correlated insulating states formed at symmetric (1:1) and asymmetric (4:1 and 7:1) electron doping of the two MoSe$_2$ layers at cryogenic temperatures. We attribute these features to the bilayer Wigner crystals formed from two commensurate triangular electron lattices in each layer, stabilized via inter-layer interaction. These bilayer Wigner crystal phases are remarkably stable and undergo quantum and thermal melting transitions above a critical electron density of up to $6 \times10^{12}$ cm$^{-2}$ and at temperatures of ~40 K. Our results demonstrate that atomically thin semiconductors provide a promising new platform for realizing strongly correlated electronic states, probing their electronic and magnetic phase transitions, and developing novel applications in quantum electronics and optoelectronics., Comment: 4 figures

We construct high-quality graphene-based van der Waals devices with narrow superconducting niobium nitride (NbN) electrodes, in which superconductivity and robust fqH coexist. We find crossed Andreev reflection (CAR) across the superconductor separating two fqH edges. Our observed CAR probabilities in the particle-like fractional fillings are markedly higher than those in the integer and hole-conjugate fractional fillings and depend strongly on temperature and magnetic field unlike the other fillings. Further, we find a filling-independent CAR probability in integer fillings, which we attribute to spin-orbit coupling in NbN allowing for Andreev reflection between spin-polarized edges. These results provide a route to realize novel topological superconducting phases in fqH-superconductor hybrid devices based on graphene and NbN., Comment: Revised text, additional main and appendix figures

We develop Johnson noise thermometry applicable to mesoscopic devices with variable source impedance with high bandwidth for fast data acquisition. By implementing differential noise measurement and two-stage impedance matching, we demonstrate noise measurement in the frequency range 120-250 MHz with a wide sample resistance range 30 {\Omega}-100 k{\Omega} tuned by gate voltages and temperature. We employ high-frequency, single-ended low noise amplifiers maintained at a constant cryogenic temperature in order to maintain the desired low noise temperature. We achieve thermometer calibration with temperature precision up to 650 mK on a 10 K background with 30 s of averaging. Using this differential noise thermometry technique, we measure thermal conductivity on a bilayer graphene sample spanning the metallic and semiconducting regimes in a wide resistance range, and we compare it to the electrical conductivity., Comment: 9 pages, 4 figures; submitted to Review of Scientific Instruments

Quantum interferometers are powerful tools for probing the wave-nature and exchange statistics of indistinguishable particles. Of particular interest are interferometers formed by the chiral, one-dimensional (1D) edge channels of the quantum Hall effect (QHE) that guide electrons without dissipation. Using quantum point contacts (QPCs) as beamsplitters, these 1D channels can be split and recombined, enabling interference of charged particles. Such quantum Hall interferometers (QHIs) can be used for studying exchange statistics of anyonic quasiparticles. In this study we develop a robust QHI fabrication technique in van der Waals (vdW) materials and realize a graphene-based Fabry-P\'erot (FP) QHI. By careful heterostructure design, we are able to measure pure Aharonov-Bohm (AB) interference effect in the integer QHE, a major technical challenge in finite size FP interferometers. We find that integer edge modes exhibit high visibility interference due to relatively large velocities and long phase coherence lengths. Our QHI with tunable QPCs presents a versatile platform for interferometer studies in vdW materials and enables future experiments in the fractional QHE.

In a Josephson junction (JJ), Cooper pairs are transported via Andreev bound states (ABSs) between superconductors. The ABSs in the weak link of multi-terminal (MT) JJs can coherently hybridize two Cooper pairs among different superconducting electrodes, resulting in the Cooper quartet (CQ) involving four fermions entanglement. The energy spectrum of these CQ-ABS can be controlled by biasing MT-JJs due to the AC Josephson effect. Here, using gate tunable four-terminal graphene JJs complemented with a flux loop, we construct CQs with a tunable spectrum. The critical quartet supercurrent exhibits magneto-oscillation associated with a charge of 4e; thereby presenting the evidence for interference between entangled CQ-ABS. At a finite bias voltage, we find the DC quartet supercurrent shows non-monotonic bias dependent behavior, attributed to Landau-Zener transitions between different Floquet bands. Our experimental demonstration of coherent non-equilibrium CQ-ABS sets a path for design of artificial topological materials based on MT-JJs.

Strong variations in superconducting critical temperatures in different families of the cuprate perovskites, even with similar hole doping in their copper-oxygen planes, suggest the importance of lattice modulation effects. The one-dimensional incommensurate lattice modulation (ILM) of Bi_2Sr_2CaCu_2O_{8+y}, with the average atomic positions perturbed beyond the unit cell, offers an ideal test ground for studying the interplay between superconductivity and the long-range incommensurate lattice fluctuations. Here we report Scanning nano X-ray Diffraction (SnXRD) imaging of incommensurate lattice modulations in Bi_{2.1}Sr_{1.9}CaCu_{2.0}O_{8+{\delta}} Van der Waals heterostructures of thicknesses down to two-unit cells. Using SnXRD, we probe that the long-range and short-range incommensurate lattice modulations in bulk sample surface with spatial resolution below 100 nm. We find that puddle-like domains of ILM of size uniformly evolving with dimensionality. In the 2-unit cell thin sample, it is observed that the wavevectors of the long- and short-range orders become anti-correlated with emerging spatial patterns having a directional gradient. The emerging patterns, originated by tiny tuning of lattice strain, induce static mesoscopic charge density waves. Our findings thus demonstrate that the strain can be used to tune and control the electromagnetic properties of two-dimensional high-temperature superconductors.

That one can stack van der Waals materials with atomically sharp interfaces has provided a new material platform of constructing heterostructures. The technical challenge of mechanical stacking is picking up the exfoliated atomically thin materials after mechanical exfoliation without chemical and mechanical degradation. Chemically inert hexagonal boron nitride (hBN) has been widely used for encapsulating and picking up vdW materials. However, due to the relatively weak adhesion of hBN, assembling vdW heterostructures based on hBN has been limited. We report a new dry transfer technique. We used two vdW semiconductors (ZnPS3 and CrPS4) to pick up and encapsulate layers for vdW heterostructures, which otherwise are known to be hard to fabricate. By combining with optimized polycaprolactone (PCL) providing strong adhesion, we demonstrated various vertical heterostructure devices, including quasi-2D superconducting NbSe2 Josephson junctions with atomically clean interface. The versatility of the PCL-based vdW stacking method provides a new route for assembling complex 2D vdW materials without interfacial degradation.

We report a combined nano-photocurrent and infrared nanoscopy study of twisted bilayer graphene (TBG) enabling access to the local electronic phenomena at length scales as short as 20 nm. We show that the photocurrent changes sign at carrier densities tracking the local superlattice density of states of TBG. We use this property to identify domains of varying local twist angle by local photo-thermoelectric effect. Consistent with the photocurrent study, infrared nano-imaging experiments reveal optical conductivity features dominated by twist-angle dependent interband transitions. Our results provide a fast and robust method for mapping the electronic structure of TBG and suggest that similar methods can be broadly applied to probe electronic inhomogeneities of moir\'e superlattices in other van der Waals heterostructures.

The artificial stacking of atomically thin crystals suffers from intrinsic limitations in terms of control and reproducibility of the relative orientation of exfoliated flakes. This drawback is particularly severe when the properties of the system critically depend on the twist angle, as in the case of the dodecagonal quasicrystal formed by two graphene layers rotated by 30$^\circ$. Here we show that large-area 30$^\circ$-rotated bilayer graphene can be grown deterministically by chemical vapor deposition on Cu, eliminating the need of artificial assembly. The quasicrystals are easily transferred to arbitrary substrates and integrated in high-quality hBN-encapsulated heterostructures, which we process into dual-gated devices exhibiting carrier mobility up to $10^5$ cm$^2$/Vs. From low-temperature magnetotransport, we find that the graphene quasicrystals effectively behave as uncoupled graphene layers, showing 8-fold degenerate quantum Hall states: this result indicates that the Dirac cones replica detected by previous photo-emission experiments do not contribute to the electrical transport., Comment: This is the unedited authors' version of the submitted article, published in its final form on Nano Letters 2020 https://doi.org/10.1021/acs.nanolett.0c00172 , 21 pages, 3 figures and supporting information

Structural engineering of van der Waals heterostructures via stacking and twisting has recently been used to create moir\'e superlattices, enabling the realization of new optical and electronic properties in solid-state systems. In particular, moir\'e lattices in twisted bilayers of transition metal dichalcogenides (TMDs) have been shown to lead to exciton trapping, host Mott insulating and superconducting states, and act as unique Hubbard systems whose correlated electronic states can be detected and manipulated optically. Structurally, these twisted heterostructures also feature atomic reconstruction and domain formation. Unfortunately, due to the nanoscale sizes (~10 nm) of typical moir\'e domains, the effects of atomic reconstruction on the electronic and excitonic properties of these heterostructures could not be investigated systematically and have often been ignored. Here, we use near-0$^o$ twist angle MoSe$_2$/MoSe$_2$ bilayers with large rhombohedral AB/BA domains to directly probe excitonic properties of individual domains with far-field optics. We show that this system features broken mirror/inversion symmetry, with the AB and BA domains supporting interlayer excitons with out-of-plane (z) electric dipole moments in opposite directions. The dipole orientation of ground-state $\Gamma$-K interlayer excitons (X$_{I,1}$) can be flipped with electric fields, while higher-energy K-K interlayer excitons (X$_{I,2}$) undergo field-asymmetric hybridization with intralayer K-K excitons (X$_0$). Our study reveals the profound impacts of crystal symmetry on TMD excitons and points to new avenues for realizing topologically nontrivial systems, exotic metasurfaces, collective excitonic phases, and quantum emitter arrays via domain-pattern engineering., Comment: 29 pages, 4 figures in main text, 6 figures in supplementary information

A beam of holes formed in graphene by a collimating contact is imaged using a liquid-He cooled scanning probe microscope (SPM). The mean free path of holes is greater than the device dimensions. A zigzag shaped pattern on both sides of the collimating contact absorb holes that enter at large angles. The image charge beneath the SPM tip defects holes, and the pattern of flow is imaged by displaying the change in conductance between contacts on opposite sides, as the tip is raster scanned across the sample. Collimation is confirmed by bending hole trajectories away from the receiving contact with an applied magnetic field. The SPM images agree well with ray-tracing simulations., Comment: 11 pages, 3 figures

The twist degree of freedom provides a powerful new tool for engineering the electrical and optical properties of van der Waals heterostructures. Here, we show that the twist angle can be used to control the spin-valley properties of transition metal dichalcogenide bilayers by changing the momentum alignment of the valleys in the two layers. Specifically, we observe that the interlayer excitons in twisted WSe$_2$/WSe$_2$ bilayers exhibit a high (>60%) degree of circular polarization (DOCP) and long valley lifetimes (>40 ns) at zero electric and magnetic fields. The valley lifetime can be tuned by more than three orders of magnitude via electrostatic doping, enabling switching of the DOCP from ~80% in the n-doped regime to <5% in the p-doped regime. These results open up new avenues for tunable chiral light-matter interactions, enabling novel device schemes that exploit the valley degree of freedom., Comment: 31 pages, 4 figures in main text, 5 figures in supplemental materials

Excitons are composite bosons that can feature spin singlet and triplet states. In usual semiconductors, without an additional spin-flip mechanism, triplet excitons are extremely inefficient optical emitters. Large spin-orbit coupling in transition metal dichalcogenides (TMDs) couples circularly polarized light to excitons with selective valley and spin. Here, we demonstrate electrically controlled brightening of spin-triplet interlayer excitons in a MoSe$_2$/WSe$_2$ TMD van der Waals (vdW) heterostructure. The atomic registry of vdW layers in TMD heterostructures provides a quasi-angular momentum to interlayer excitons, enabling emission from otherwise dark spin-triplet excitons. Employing magnetic field, we show that photons emitted by triplet and singlet excitons in the same valley have opposite chirality. We also measure effective exciton g-factors, presenting direct and quantitative evidence of triplet interlayer excitons. We further demonstrate gate tuning of the relative photoluminescence intensity between singlet and triplet charged excitons. Electrically controlled emission between singlet and triplet excitons enables a route for optoelectronic devices that can configure excitonic chiral, spin, and valley quantum states.

The optical and electronic properties of van der Waals (vdW) heterostructures depend strongly on the atomic stacking order of the constituent layers. This is exemplified by periodic variation of the local atomic registry, known as moire patterns, giving rise to superconductivity and ferromagnetism in twisted bilayer graphene and novel exciton states in transition metal dichalcogenides (TMD) heterobilayers. However, the presence of the nanometer-scale moire superlattices is typically deduced indirectly, because conventional imaging techniques, such as transmission electron microscopy (TEM), require special sample preparation that is incompatible with most optical and transport measurements. Here, we demonstrate a method that uses a secondary electron microscope to directly image the local stacking order in fully hexagonal boron nitride (hBN) encapsulated, gated vdW heterostructure devices on standard Si-substrates. Using this method, we demonstrate imaging of reconstructed moire patterns in stacked TMDs, ABC/ABA stacking order in graphene multilayers, and AB/BA boundaries in bilayer graphene. Furthermore, we show that the technique is non-destructive, thus unlocking the possibility of directly correlating local stacking order with optical and electronic properties, crucial to the development of vdW heterostructure devices with precisely controlled functionality.

Moir\'e superlattices in twisted van der Waals materials constitute a promising platform for engineering electronic and optical properties. However, a major obstacle to fully understanding these systems and harnessing their potential is the limited ability to correlate the local moir\'e structure with optical properties. By using a recently developed scanning electron microscopy technique to image twisted WSe$_2$/WSe$_2$ bilayers, we directly correlate increasing moir\'e periodicity with the emergence of two distinct exciton species. These can be tuned individually through electrostatic gating, and feature different valley coherence properties. Our observations can be understood as resulting from an array of two intralayer exciton species residing in alternating locations in the superlattice, and illuminate the influence of the moir\'e potential on lateral exciton motion. They open up new avenues for controlling exciton arrays in twisted TMDs, with applications in quantum optoelectronics and explorations of novel many body systems., Comment: 25 pages, 4 figures in main text, 4 figures in supplementary materials

The Sachdev-Ye-Kitaev (SYK) model describes electrons with random and all-to-all interactions, and realizes a many-body state without quasiparticle excitations, and a non-vanishing extensive entropy $S_0$ in the zero temperature limit. Its low energy theory coincides the low energy theory of the near-extremal charged black holes with Bekenstein-Hawking entropy $S_0$. Several mesoscopic experimental configurations realizing SYK quantum dynamics over a significant intermediate temperature scale have been proposed. We investigate quantum thermoelectric transport in such configurations, and describe the low temperature crossovers out of SYK criticality into regimes with either Fermi liquid behavior, a Coulomb blockade, or criticality associated with Schwarzian quantum gravity fluctuations. Our results show that thermopower measurements can serve as a direct probe for $S_0$., Comment: 11 pages, 4 figures; (v2) rewritten, with new results on charging energy and Schwarzian fluctuations

Relativistic massless charged particles in a two-dimensional conductor can be guided by a one-dimensional electrostatic potential, in an analogous manner to light guided by an optical fiber. We use a carbon nanotube to generate such a guiding potential in graphene and create a single mode electronic waveguide. The nanotube and graphene are separated by a few nanometers and can be controlled and measured independently. As we charge the nanotube, we observe the formation of a single guided mode in graphene that we detect using the same nanotube as a probe. This single electronic guided mode in graphene is sufficiently isolated from other electronic states of linear Dirac spectrum continuum, allowing the transmission of information with minimal distortion., Comment: The manuscript includes Supplementary Information

Sensitive microwave detectors are critical instruments in radioastronomy, dark matter axion searches, and superconducting quantum information science. The conventional strategy towards higher-sensitivity bolometry is to nanofabricate an ever-smaller device to augment the thermal response. However, this direction is increasingly more difficult to obtain efficient photon coupling and maintain the material properties in a device with a large surface-to-volume ratio. Here we advance this concept to an ultimately thin bolometric sensor based on monolayer graphene. To utilize its minute electronic specific heat and thermal conductivity, we develop a superconductor-graphene-superconductor (SGS) Josephson junction bolometer embedded in a microwave resonator of resonant frequency 7.9 GHz with over 99\% coupling efficiency. From the dependence of the Josephson switching current on the operating temperature, charge density, input power, and frequency, we demonstrate a noise equivalent power (NEP) of 7 $\times 10^{-19}$ W/Hz$^{1/2}$, corresponding to an energy resolution of one single photon at 32 GHz and reaching the fundamental limit imposed by intrinsic thermal fluctuation at 0.19 K., Comment: 8 pages, 4 figures

We respond to P. Ao's comment in arXiv:1907.09263, which suggests that vortex many-body effects are the origin of Hall sign reversal in few-unit-cell thick Bi-2212 cuprate crystals (Phys. Rev. Lett. 122, 247001 (2019)). Our experimental results are incompatible with the theoretical predictions detailed in Ao's comment., Comment: 1 page, 1 figure with inset

The growth of single crystals of MoS2 and WS2 by materials transport through a liquid salt flux made from a low melting mixture of NaCl and CsCl is described. The crystals are characterized by single crystal X-ray diffraction, which reveals that they are 2H-MoS2 with a small percentage (about 3%) of 3R intergrowths. The 2H-WS2 crystals display less than 1% of 3R intergrowths. Photoluminescence spectra of exfoliated monolayers suggest that MoS2 grown by this method has superior crystallinity in comparison to commercially-available MoS2 crystals., Comment: 24 pages, 8 figures. SI: 4 tables

The electron-hole plasma in charge-neutral graphene is predicted to realize a quantum critical system whose transport features a universal hydrodynamic description, even at room temperature. This quantum critical "Dirac fluid" is expected to have a shear viscosity close to a minimum bound, with an inter-particle scattering rate saturating at the Planckian time $\hbar/(k_B T)$. While electrical transport measurements at finite carrier density are consistent with hydrodynamic electron flow in graphene, a "smoking gun" of viscous behavior remains elusive. In this work, we directly image viscous Dirac fluid flow in graphene at room temperature via measurement of the associated stray magnetic field. Nanoscale magnetic imaging is performed using quantum spin magnetometers realized with nitrogen vacancy (NV) centers in diamond. Scanning single-spin and wide-field magnetometry reveals a parabolic Poiseuille profile for electron flow in a graphene channel near the charge neutrality point, establishing the viscous transport of the Dirac fluid. This measurement is in contrast to the conventional uniform flow profile imaged in an Ohmic conductor. Via combined imaging-transport measurements, we obtain viscosity and scattering rates, and observe that these quantities are comparable to the universal values expected at quantum criticality. This finding establishes a nearly-ideal electron fluid in neutral graphene at room temperature. Our results pave the way to study hydrodynamic transport in quantum critical fluids relevant to strongly-correlated electrons in high-$T_c$ superconductors. This work also highlights the capability of quantum spin magnetometers to probe correlated-electronic phenomena at the nanoscale., Comment: Author list and title have been updated in published version

Polaritons formed by the coupling of light and material excitations such as plasmons, phonons, or excitons enable light-matter interactions at the nanoscale beyond what is currently possible with conventional optics. Recently, significant interest has been attracted by polaritons in van der Waals materials, which could lead to applications in sensing, integrated photonic circuits and detectors. However, novel techniques are required to control the propagation of polaritons at the nanoscale and to implement the first practical devices. Here we report the experimental realization of polariton refractive and meta-optics in the mid-infrared by exploiting the properties of low-loss phonon polaritons in isotopically pure hexagonal boron nitride (hBN), which allow it to interact with the surrounding dielectric environment comprising the low-loss phase change material, Ge$_3$Sb$_2$Te$_6$ (GST). We demonstrate waveguides which confine polaritons in a 1D geometry, and refractive optical elements such as lenses and prisms for phonon polaritons in hBN, which we characterize using scanning near field optical microscopy. Furthermore, we demonstrate metalenses, which allow for polariton wavefront engineering and sub-wavelength focusing. Our method, due to its sub-diffraction and planar nature, will enable the realization of programmable miniaturized integrated optoelectronic devices, and will lay the foundation for on-demand biosensors., Comment: 15 pages, 4 figures, typos corrected in v2

Two monolayers of graphene twisted by a small `magic' angle exhibit nearly flat bands leading to correlated electronic states and superconductivity, whose precise nature including possible broken symmetries, remain under debate. Here we theoretically study a related but different system with reduced symmetry - twisted {\em double} bilayer graphene (TDBLG), consisting of {\em two} Bernal stacked bilayer graphene sheets, twisted with respect to one another. Unlike the monolayer case, we show that isolated flat bands only appear on application of a vertical displacement field $D$. We construct a phase diagram as a function of twist angle and $D$, incorporating interactions via a Hartree-Fock approximation. At half filling, ferromagnetic insulators are stabilized, typically with valley Chern number $C_v=2$. Ferromagnetic fluctuations in the metallic state are argued to lead to spin triplet superconductivity from pairing between electrons in opposite valleys. Response of these states to a magnetic field applied either perpendicular or parallel to the graphene sheets is obtained, and found to compare favorably with a recent experiment. We highlight a novel orbital effect arising from in-plane fields that can exceed the Zeeman effect and plays an important role in interpreting experiments., Comment: main 15 pages, appendix 11 pages

Ferromagnetism and superconductivity typically compete with each other since the internal magnetic field generated in a magnet suppresses the formation of spin-singlet Cooper pairs in conventional superconductors. Only a handful of ferromagnetic superconductors are known in heavy fermion systems, where many-body electron interactions promoted by the narrow energy bands play a key role in stabilizing these emergent states. Recently, interaction-driven superconductivity and ferromagnetism have been demonstrated as separate phenomena in different density regimes of flat bands enabled by graphene moire superlattices. Combining superconductivity and magnetism in a single ground state may lead to more exotic quantum phases. Here, employing van der Waals heterostructures of twisted double bilayer graphene (TDBG), we realize a flat electron band that is tunable by perpendicular electric fields. Similar to the magic angle twisted bilayer graphene, TDBG exhibits energy gaps at the half and quarter filled flat bands, indicating the emergence of correlated insulating states. We find that the gaps of these insulating states increase with in-plane magnetic field, suggesting a ferromagnetic order. Upon doping the ferromagnetic half-filled insulator, superconductivity emerges with a critical temperature controlled by both density and electric fields. We observe that the in-plane magnetic field enhances the superconductivity in the low field regime, suggesting spin-polarized electron pairing. Spin-polarized superconducting states discovered in TDBG provide a new route to engineering interaction-driven topological superconductivity., Comment: 13 pages, 3 figures and supplementary information

We demonstrate a new approach for dynamically manipulating the optical response of an atomically thin semiconductor, a monolayer of MoSe2, by suspending it over a metallic mirror. First, we show that suspended van der Waals heterostructures incorporating a MoSe2 monolayer host spatially homogeneous, lifetime-broadened excitons. Then, we interface this nearly ideal excitonic system with a metallic mirror and demonstrate control over the exciton-photon coupling. Specifically, by electromechanically changing the distance between the heterostructure and the mirror, thereby changing the local photonic density of states in a controllable and reversible fashion, we show that both the absorption and emission properties of the excitons can be dynamically modulated. This electromechanical control over exciton dynamics in a mechanically flexible, atomically thin semiconductor opens up new avenues in cavity quantum optomechanics, nonlinear quantum optics, and topological photonics., Comment: accepted version

Excitons in semiconductors, bound pairs of excited electrons and holes, can form the basis for new classes of quantum optoelectronic devices. A van der Waals heterostructure built from atomically thin semiconducting transition metal dichalcogenides (TMDs) enables the formation of excitons from electrons and holes in distinct layers, producing interlayer excitons with large binding energy and a long lifetime. Employing heterostructures of monolayer TMDs, we realize optical and electrical generation of long-lived neutral and charged interlayer excitons. We demonstrate the transport of neutral interlayer excitons across the whole sample that can be controlled by excitation power and gate electrodes. We also realize the drift motion of charged interlayer excitons using Ohmic-contacted devices. The electrical generation and control of excitons provides a new route for realizing quantum manipulation of bosonic composite particles with complete electrical tunability.

In two-dimensional (2D) electron systems under strong magnetic fields, interactions can cause fractional quantum Hall (FQH) effects. Bringing two 2D conductors to proximity, a new set of correlated states can emerge due to interactions between electrons in the same and opposite layers. Here we report interlayer correlated FQH states in a system of two parallel graphene layers separated by a thin insulator. Current flow in one layer generates different quantized Hall signals in the two layers. This result is interpreted by composite fermion (CF) theory with different intralayer and interlayer Chern-Simons gauge-field coupling. We observe FQH states corresponding to integer values of CF Landau level (LL) filling in both layers, as well as "semi-quantized" states, where a full CF LL couples to a continuously varying partially filled CF LL. Remarkably, we also recognize a quantized state between two coupled half-filled CF LLs, attributable to an interlayer CF exciton condensate., Comment: 14 pages, 3 figures, one table and supplementary information

We articulate the challenges and opportunities of unconventional devices using the photon like flow of electrons in graphene, such as Graphene Klein Tunnel (GKT) transistors. The underlying physics is the employment of momentum rather than energy filtering to engineer a gate tunable transport gap in a 2D Dirac cone bandstructure. In the ballistic limit, we get a clean tunable gap that implies subthermal switching voltages below the Boltzmann limit, while maintaining a high saturating current in the output characteristic. In realistic structures, detailed numerical simulations and experiments show that momentum scattering, especially from the edges, bleeds leakage paths into the transport gap and turns it into a pseudogap. We quantify the importance of reducing edge roughness and overall geometry on the low-bias transfer characteristics of GKT transistors and benchmark against experimental data. We find that geometry plays a critical role in determining the performance of electron optics based devices that utilize angular resolution of electrons.

We fabricate van der Waals heterostructure devices using few unit cell thick Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$ for magnetotransport measurements. The superconducting transition temperature and carrier density in atomically thin samples can be maintained to close to that of the bulk samples. As in the bulk sample, the sign of the Hall conductivity is found to be opposite to the normal state near the transition temperature but with a drastic enlargement of the region of Hall sign reversal in the temperature-magnetic field phase diagram as the thickness of samples decreases. Quantitative analysis of the Hall sign reversal based on the excess charge density in the vortex core and superconducting fluctuations suggests a renormalized superconducting gap in atomically thin samples at the 2-dimensional limit., Comment: 5 pages, 3 figures. Supplementary information is not included

The linear energy-momentum dispersion, coupled with pseudo-spinors, makes graphene an ideal solid-state material platform to realize an electronic device based on Dirac-Fermionic relativistic quantum mechanics. Employing local gate control, several examples of electronic devices based on Dirac fermion dynamics have been demonstrated, including Klein tunneling, negative refraction and specular Andreev reflection. In this work, we present a quantum switch based on analogous Dirac-fermion-optics (DFO), in which the angle dependence of Klein tunneling is explicitly utilized to build tunable collimators and reflectors for the quantum wave function of Dirac fermions. We employ a novel dual-source design with a single flat reflector, which minimizes diffusive edge scattering and suppresses the background incoherent transmission. Our gate-tunable collimator-reflector device design enables measurement of the net DFO contribution in the switching device operation. We measure a full set of transmission coefficients of DFO wavefunction between multiple leads of the device, separating the classical contribution from that of any disorder in the channel. Since the DFO quantum switch demonstrated in this work requires no explicit energy gap, the switching operation is expected to be robust against thermal fluctuations and inhomogeneity length scales comparable to the Fermi wavelength. We find our quantum switch works at an elevated temperature up to 230 K and large bias current density up to 102 A/m, over a wide range of carrier densities. The tunable collimator-reflector coupled with the conjugated source electrodes developed in this work provides an additional component to build more efficient DFO electronic devices., Comment: 27 pages, 9 figures

Van der Waals heterostructures assembled from layers of 2D materials have attracted considerable interest due to their novel optical and electrical properties. Here we report a scattering-type scanning near field optical microscopy study of hexagonal boron nitride on black phosphorous (h-BN/BP) heterostructures, demonstrating the first direct observation of in-plane anisotropic phonon polariton modes in vdW heterostructures. Strikingly, the measured in-plane optical anisotropy along armchair and zigzag crystal axes exceeds the ratio of refractive indices of BP in the x-y plane. We explain that this enhancement is due to the high confinement of the phonon polaritons in h-BN. We observe a maximum in-plane optical anisotropy of {\alpha}_max=1.25 in the 1405-1440 cm-1 frequency spectrum. These results provide new insights on the behavior of polaritons in vdW heterostructures, and the observed anisotropy enhancement paves the way to novel nanophotonic devices and to a new way to characterize optical anisotropy in thin films.

The properties of Van der Waals heterostructures are determined by the twist angle and the interface between adjacent layers as well as their polytype and stacking. Here we describe the use of spectroscopic Low Energy Electron Microscopy (LEEM) and micro Low Energy Electron Diffraction ({\mu}LEED) methods to measure these properties locally. We present results on a MoS$_{2}$/hBN heterostructure, but the methods are applicable to other materials. Diffraction spot analysis is used to assess the benefits of using hBN as a substrate. In addition, by making use of the broken rotational symmetry of the lattice, we determine the cleaving history of the MoS$_{2}$ flake, i.e., which layer stems from where in the bulk.

Quantum states of quasiparticles in solids are dictated by symmetry. Thus, a discovery of unconventional symmetry can provide a new opportunity to reach a novel quantum state. Recently, Dirac and Weyl electrons have been observed in crystals with discrete translational symmetry. Here we experimentally demonstrate Dirac electrons in a two-dimensional quasicrystal without translational symmetry. A dodecagonal quasicrystal was realized by epitaxial growth of twisted bilayer graphene rotated exactly 30 degree. The graphene quasicrystal was grown up to a millimeter scale on SiC(0001) surface while maintaining the single rotation angle over an entire sample and was successfully isolated from a substrate, demonstrating its structural and chemical stability under ambient conditions. Multiple Dirac cone replicated with the 12-fold rotational symmetry were observed in angle resolved photoemission spectra, showing its unique electronic structures with anomalous strong interlayer coupling with quasi-periodicity. Our study provides a new way to explore physical properties of relativistic fermions with controllable quasicrystalline orders., Comment: 20 pages, 4 figures

Control of the interlayer twist angle in two-dimensional (2D) van der Waals (vdW) heterostructures enables one to engineer a quasiperiodic moir\'e superlattice of tunable length scale. In twisted bilayer graphene (TBG), the simple moir\'e superlattice band description suggests that the electronic band width can be tuned to be comparable to the vdW interlayer interaction at a 'magic angle', exhibiting strongly correlated behavior. However, the vdW interlayer interaction can also cause significant structural reconstruction at the interface by favoring interlayer commensurability, which competes with the intralayer lattice distortion. Here we report the atomic scale reconstruction in TBG and its effect on the electronic structure. We find a gradual transition from incommensurate moir\'e structure to an array of commensurate domain structures as we decrease the twist angle across the characteristic crossover angle, $\theta_c$ ~1\deg. In the twist regime smaller than $\theta_c$ where the atomic and electronic reconstruction become significant, a simple moir\'e band description breaks down. Upon applying a transverse electric field, we observe electronic transport along the network of one-dimensional (1D) topological channels that surround the alternating triangular gapped domains, providing a new pathway to engineer the system with continuous tunability.

We report magnetotransport measurements on magnetically doped (Bi,Sb)$_2$Te$_3$ films grown by molecular beam epitaxy. In Hallbar devices, logarithmic dependence on temperature and bias voltage are obseved in both the longitudinal and anomalous Hall resistance. The interplay of disorder and electron-electron interactions is found to explain quantitatively the observed logarithmic singularities and is a dominant scattering mechanism in these samples. Submicron scale devices exhibit intriguing quantum oscillations at high magnetic fields with dependence on bias voltage. The observed quantum oscillations can be attributed to bulk and surface transport., Comment: 10 pages, 13 figures

Polaritons in 2D and van der Waals (vdW) materials have been investigated in several recent works as an innovative platform for light-matter interaction, rich of new physical phenomena.Hexagonal Boron Nitride (h-BN), in particular, is an out of plane anisotropic material (while it is in-plane isotropic) with two very strong phonon polaritons bands where the permittivity becomes negative. In the first restrahlen band (RS1, 780-830 cm-1) the relative out of plane permittivity is negative, while in the second restrahlen band (RS2, 1370-1610 cm-1) the relative in-plane permittivity is negative. Due to these optical properties, thin h-BN flakes support guided modes which have been observed experimentally both via far field and near field methods. In this work, we show how selectively excite the more confined modes in the RS1 and RS2 bands. The supported guided modes have phase and group velocities respectively tens and hundreds of times slower than the speed of light. We also show the possibility of full hyperspectral nano-imaging of modes in RS1 band by means of photo-induced force microscopy (PiFM). Moreover, a direct comparison of (PiFM) and scattering-type near-field microscopy (s-SNOM) is obtained by imaging the modes of the RS2 band with both techniques implemented on the same platform. The possibility of addressing ultraslow (ultraconfined) polaritonic modes of h-BN crystal flakes together with the possibility of optical nano-imaging in both the restrahlen bands have many innovative aspects that can lead to unprecedented schemes for strong light-matter interaction, slow and confined light.

Molecular-scale manipulation of electronic/ionic charge accumulation in materials is a preeminent challenge, particularly in electrochemical energy storage. Layered van der Waals (vdW) crystals exemplify a diverse family of materials that permit ions to reversibly associate with a host atomic lattice by intercalation into interlamellar gaps. Motivated principally by the search for high-capacity battery anodes, ion intercalation in composite materials is a subject of intense study. Yet the precise role and ability of heterolayers to modify intercalation reactions remains elusive. Previous studies of vdW hybrids represented ensemble measurements at macroscopic films/powders, which do not permit the isolation and investigation of the chemistry at individual 2-dimensional (2D) interfaces. Here, we demonstrate the intercalation of lithium at the level of individual atomic interfaces of dissimilar vdW layers. Electrochemical devices based on vdW heterostructures comprised of deterministically stacked hexagonal boron nitride, graphene (G) and molybdenum dichalcogenide (MoX2; X = S, Se) layers are fabricated, enabling the direct resolution of intermediate stages in the intercalation of discrete heterointerfaces and the extent of charge transfer to individual layers. Operando magnetoresistance and optical spectroscopy coupled with low-temperature quantum magneto-oscillation measurements show that the creation of intimate vdW heterointerfaces between G and MoX2 engenders over 10-fold accumulation of charge in MoX2 compared to MoX2/MoX2 homointerfaces, while enforcing a more negative intercalation potential than that of bulk MoX2 by at least 0.5 V. Beyond energy storage, our new combined experimental and computational methodology to manipulate and characterize the electrochemical behavior of layered systems opens up new pathways to control the charge density in 2D (opto)electronic devices., Comment: 10 pages, 5 Figures, Methods, and Supplementary Information