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Noncentrosymmetric 2D superconductors with large spin-orbit coupling offer an opportunity to explore superconducting behaviors far beyond the Pauli limit. One such superconductor, few-layer T$_d$-MoTe$_2$, has large upper critical fields that can exceed the Pauli limit by up to 600%. However, the mechanisms governing this enhancement are still under debate, with theory pointing towards either spin-orbit parity coupling or tilted Ising spin-orbit coupling. Moreover, ferroelectricity concomitant with superconductivity has been recently observed in the bilayer, where strong changes to superconductivity can be observed throughout the ferroelectric transition pathway. Here, we report the superconducting behavior of bilayer T$_d$-MoTe$ _2$ under an in-plane magnetic field, while systematically varying magnetic field angle and out-of-plane electric field strength. We find that superconductivity in bilayer MoTe$_2$ exhibits a two-fold symmetry with an upper critical field maxima occurring along the b-axis and minima along the a-axis. The two-fold rotational symmetry remains robust throughout the entire superconducting region and ferroelectric hysteresis loop. Our experimental observations of the spin-orbit coupling strength (up to 16.4 meV) agree with the spin texture and spin splitting from first-principles calculations, indicating that tilted Ising spin-orbit coupling is the dominant underlying mechanism.

Two-dimensional materials are extraordinarily sensitive to external stimuli, making them ideal for studying fundamental properties and for engineering devices with new functionalities. One such stimulus, strain, affects the magnetic properties of the layered magnetic semiconductor CrSBr to such a degree that it can induce a reversible antiferromagnetic-to-ferromagnetic phase transition. Given the pervasiveness of non-uniform strain in exfoliated two-dimensional magnets, it is crucial to understand its impact on their magnetic behavior. Using scanning SQUID-on-lever microscopy, we directly image the effects of spatially inhomogeneous strain on the magnetization of layered CrSBr as it is polarized by a field applied along its easy axis. The evolution of this magnetization and the formation of domains is reproduced by a micromagnetic model, which incorporates the spatially varying strain and the corresponding changes in the local interlayer exchange stiffness. The observed sensitivity to small strain gradients along with similar images of a nominally unstrained CrSBr sample suggest that unintentional strain inhomogeneity influences the magnetic behavior of exfoliated samples and must be considered in the design of future devices., Comment: 15 pages, 4 figures, 1 supplementary section

Materials hosting flat electronic bands are a central focus of condensed matter physics as promising venues for novel electronic ground states. Two-dimensional (2D) geometrically frustrated lattices such as the kagome, dice, and Lieb lattices are attractive targets in this direction, anticipated to realize perfectly flat bands. Synthesizing these special structures, however, poses a formidable challenge, exemplified by the absence of solid-state materials realizing the dice and Lieb lattices. An alternative route leverages atomic orbitals to create the characteristic electron hopping of geometrically frustrated lattices. This strategy promises to expand the list of candidate materials to simpler structures, but is yet to be demonstrated experimentally. Here, we report the realization of frustrated hopping in the van der Waals (vdW) intermetallic Pd$_5$AlI$_2$, emerging from orbital decoration of a primitive square lattice. Using angle-resolved photoemission spectroscopy and quantum oscillations measurements, we demonstrate that the band structure of Pd$_5$AlI$_2$ includes linear Dirac-like bands intersected at their crossing point by a flat band, essential characteristics of frustrated hopping in the Lieb and dice lattices. Moreover, Pd$_5$AlI$_2$ is exceptionally stable, with the unusual bulk band structure and metallicity persisting in ambient conditions down to the monolayer limit. Our ability to realize an electronic structure characteristic of geometrically frustrated lattices establishes orbital decoration of primitive lattices as a new approach towards electronic structures that remain elusive to prevailing lattice-centric searches.

Graphene is a privileged 2D platform for hosting confined light-matter excitations known as surface plasmon-polaritons (SPPs), as it possesses low intrinsic losses with a high degree of optical confinement. However, the inherently isotropic optical properties of graphene limit its ability to guide and focus SPPs, making it less suitable than anisotropic elliptical and hyperbolic materials as a platform for polaritonic lensing and canalization. Here, we present the graphene/CrSBr heterostructure as an engineered 2D interface that hosts highly anisotropic SPP propagation over a wide range of frequencies in the mid-infrared and terahertz. Using a combination of scanning tunneling microscopy (STM), scattering-type scanning near-field optical microscopy (s-SNOM), and first-principles calculations, we demonstrate mutual doping in excess of 10$^{13}$ cm$^{-2}$ holes/electrons between the interfacial layers of graphene/CrSBr heterostructures. SPPs in graphene activated by charge transfer interact with charge-induced anisotropic intra- and interband transitions in the interfacial doped CrSBr, leading to preferential SPP propagation along the quasi-1D chains that compose each CrSBr layer. This multifaceted proximity effect both creates SPPs and endows them with anisotropic transport and propagation lengths that differ by an order-of-magnitude between the two in-plane crystallographic axes of CrSBr.

Electron hydrodynamics is an emerging framework that describes dynamics of interacting electron systems as conventional fluids. While evidence for hydrodynamic-like transport is reported in a variety of two-dimensional materials, precise quantitative measurement of the core parameter, electron viscosity, remains challenging. In this work, we demonstrate that magnetoresistance in Corbino-shaped graphene devices offers a simultaneous Ohmmeter/viscosometer, allowing us to disentangle the individual Ohmic and viscous contributions to the transport response, even in the mixed flow regime. Most surprising, we find that in both monolayer and bilayer graphene, the effective electron-electron scattering rate scales linearly with temperature, at odds with the expected $T$-squared dependence expected from conventional Fermi liquid theory, but consistent with a recently identified tomographic flow regime, which was theoretically conjectured to be generic for two-dimensional charged fluids.

Among expanding discoveries of quantum phases in moir\'e superlattices, correlated insulators stand out as both the most stable and most commonly observed. Despite the central importance of these states in moir\'e physics, little is known about their underlying nature. Here, we use pump-probe spectroscopy to show distinct time-domain signatures of correlated insulators at fillings of one (v = -1) and two (v = -2) holes per moir\'e unit cell in the angle-aligned WSe2/WS2 system. Following photo-doping, we find that the disordering time of the v = -1 state is independent of excitation density (n_ex), as expected from the characteristic phonon response time associated with a polaronic state. In contrast, the disordering time of the v = -2 state scales with (n_ex)^-0.5, in agreement with plasmonic screening from free holons and doublons. These states display disparate reordering behavior dominated either by first order (v = -1) or second order (v = -2) recombination, suggesting the presence of Hubbard excitons and free carrier-like holons/doublons, respectively. Our work delineates the roles of electron-phonon (e-ph) versus electron-electron (e-e) interactions in correlated insulators on the moir\'e landscape and establishes non-equilibrium responses as mechanistic signatures for distinguishing and discovering quantum phases., Comment: 18 pages, 4 figures, +10 Supporting figures. arXiv admin note: text overlap with arXiv:2307.16563

Kagome vanadates {\it A}V$_3$Sb$_5$ display unusual low-temperature electronic properties including charge density waves (CDW), whose microscopic origin remains unsettled. Recently, CDW order has been discovered in a new material ScV$_6$Sn$_6$, providing an opportunity to explore whether the onset of CDW leads to unusual electronic properties. Here, we study this question using angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM). The ARPES measurements show minimal changes to the electronic structure after the onset of CDW. However, STM quasiparticle interference (QPI) measurements show strong dispersing features related to the CDW ordering vectors. A plausible explanation is the presence of a strong momentum-dependent scattering potential peaked at the CDW wavevector, associated with the existence of competing CDW instabilities. Our STM results further indicate that the bands most affected by the CDW are near vHS, analogous to the case of {\it A}V$_3$Sb$_5$ despite very different CDW wavevectors., Comment: 33 pages, 4 figures

The discovery of superconductivity in twisted bilayer and twisted trilayer graphene has generated tremendous interest. The key feature of these systems is an interplay between interlayer coupling and a moir\'e superlattice that gives rise to low-energy flat bands with strong correlations. Flat bands can also be induced by moir\'e patterns in lattice-mismatched and or twisted heterostructures of other two-dimensional materials such as transition metal dichalcogenides (TMDs). Although a wide range of correlated phenomenon have indeed been observed in the moir\'e TMDs, robust demonstration of superconductivity has remained absent. Here we report superconductivity in 5 degree twisted bilayer WSe$_2$ (tWSe$_2$) with a maximum critical temperature of 426 mK. The superconducting state appears in a limited region of displacement field and density that is adjacent to a metallic state with Fermi surface reconstruction believed to arise from antiferromagnetic order. A sharp boundary is observed between the superconducting and magnetic phases at low temperature, reminiscent of spin-fluctuation mediated superconductivity. Our results establish that moir\'e flat-band superconductivity extends beyond graphene structures. Material properties that are absent in graphene but intrinsic among the TMDs such as a native band gap, large spin-orbit coupling, spin-valley locking, and magnetism offer the possibility to access a broader superconducting parameter space than graphene-only structures.

Moir\'e transition metal dichalcogenide (TMD) systems provide a tunable platform for studying electron-correlation driven quantum phases. Such phases have so far been found at rational fillings of the moir\'e superlattice, and it is believed that lattice commensurability plays a key role in their stability. In this work, we show via magnetotransport measurements on twisted WSe2 that new correlated electronic phases can exist away from commensurability. The first phase is an antiferromagnetic metal that is driven by proximity to the van Hove singularity. The second is a re-entrant magnetic field-driven insulator. This insulator is formed from a small and equal density of electrons and holes with opposite spin projections - an Ising excitonic insulator.

Understanding the thermoelastic response of a nanostructure is crucial for the choice of materials and interfaces in electronic devices with improved and tailored transport properties, at the length scales of the present technology. Here we show how the deposition of a $MoS_2$ monolayer can strongly modify the nanoscale thermoelastic dynamics of silicon substrates close to their interface. We achieve this result by creating a transient grating with extreme ultraviolet light, using ultrashort free-electron laser pulses, whose $\approx$84 nm period is comparable to the size of elements typically used in nanodevices, such as electric contacts and nanowires. The thermoelastic response, featured by coherent acoustic waves and an incoherent relaxation, is tangibly modified by the presence of monolayer $MoS_2$. Namely, we observed a major reduction of the amplitude of the surface mode, which is almost suppressed, while the longitudinal mode is basically unperturbed, aside from a faster decay of the acoustic modulations. We interpret this behavior as a selective modification of the surface elasticity and we discuss the conditions to observe such effect, which might be of immediate relevance for the design of Si-based nanoscale devices., Comment: 27 pages, 15 figures

Van der Waals (vdW) structures of two-dimensional materials host a broad range of physical phenomena. New opportunities arise if different functional layers may be remotely modulated or coupled in a device structure. Here we demonstrate the in-situ coherent modulation of moir\'e excitons and correlated Mott insulators in transition metal dichalcogenide (TMD) homo- or hetero-bilayers with on-chip terahertz (THz) waves. Using common dual-gated device structures, each consisting of a TMD moir\'e bilayer sandwiched between two few-layer graphene (fl-Gr) gates with hexagonal boron nitride (h-BN) spacers, we launch coherent phonon wavepackets at ~0.4-1 THz from the fl-Gr gates by femtosecond laser excitation. The waves travel through the h-BN spacer, arrive at the TMD bilayer with precise timing, and coherently modulate the moir\'e excitons or the Mott states. These results demonstrate that the fl-Gr gates, often used for electrical control of the material properties, can serve as effective on-chip opto-elastic transducers to generate THz waves for the coherent control and vibrational entanglement of functional layers in commonly used moir\'e devices., Comment: 11 pages, 4 figures, 12 pages SI. arXiv admin note: substantial text overlap with arXiv:2307.16563

Since their first observation in 2017, atomically thin van der Waals (vdW) magnets have attracted significant fundamental, and application-driven attention. However, their low ordering temperatures, $T_c$, sensitivity to atmospheric conditions and difficulties in preparing clean large-area samples still present major limitations to further progress. The remarkably stable high-$T_c$ vdW magnet CrSBr has the potential to overcome these key shortcomings, but its nanoscale properties and rich magnetic phase diagram remain poorly understood. Here we use single spin magnetometry to quantitatively characterise saturation magnetization, magnetic anisotropy constants, and magnetic phase transitions in few-layer CrSBr by direct magnetic imaging. We show pristine magnetic phases, devoid of defects on micron length-scales, and demonstrate remarkable air-stability down the monolayer limit. We address the spin-flip transition in bilayer CrSBr by direct imaging of the emerging antiferromagnetic (AFM) to ferromagnetic (FM) phase wall and elucidate the magnetic properties of CrSBr around its ordering temperature. Our work will enable the engineering of exotic electronic and magnetic phases in CrSBr and the realisation of novel nanomagnetic devices based on this highly promising vdW magnet., Comment: 8 pages, 4 figures, plus supplementary material. Questions and comments are welcome

Ultraclean graphene at charge neutrality hosts a quantum critical Dirac fluid of interacting electrons and holes. Interactions profoundly affect the charge dynamics of graphene, which is encoded in the properties of its electron-photon collective modes: surface plasmon polaritons (SPPs). Here we show that polaritonic interference patterns are particularly well suited to unveil the interactions in Dirac fluids by tracking polaritonic interference in time at temporal scales commensurate with the electronic scattering. Spacetime SPP interference patterns recorded in tera-hertz (THz) frequency range provided unobstructed readouts of the group velocity and lifetime of polariton that can be directly mapped onto the electronic spectral weight and the relaxation rate. Our data uncovered prominent departures of the electron dynamics from the predictions of the conventional Fermi-liquid theory. The deviations are particularly strong when the densities of electrons and holes are approximately equal. The proposed spacetime imaging methodology can be broadly applied to probe the electrodynamics of quantum materials.

Two-dimensional (2D) semiconductors, such as the transition metal dichalcogenides, have demonstrated tremendous promise for the development of highly tunable quantum devices. Realizing this potential requires low-resistance electrical contacts that perform well at low temperatures and low densities where quantum properties are relevant. Here we present a new device architecture for 2D semiconductors that utilizes a charge-transfer layer to achieve large hole doping in the contact region, and implement this technique to measure magneto-transport properties of high-purity monolayer WSe$_2$. We measure a record-high hole mobility of 80,000 cm$^2$/Vs and access channel carrier densities as low as $1.6\times10^{11}$ cm$^{-2}$, an order of magnitude lower than previously achievable. Our ability to realize transparent contact to high-mobility devices at low density enables transport measurement of correlation-driven quantum phases including observation of a low temperature metal-insulator transition in a density and temperature regime where Wigner crystal formation is expected, and observation of the fractional quantum Hall effect under large magnetic fields. The charge transfer contact scheme paves the way for discovery and manipulation of new quantum phenomena in 2D semiconductors and their heterostructures.

Highly tunable properties make Mn(Bi,Sb)$_2$Te$_4$ a rich playground for exploring the interplay between band topology and magnetism: On one end, MnBi$_2$Te$_4$ is an antiferromagnetic topological insulator, while the magnetic structure of MnSb$_2$Te$_4$ (MST) can be tuned between antiferromagnetic and ferrimagnetic. Motivated to control electronic properties through real-space magnetic textures, we use magnetic force microscopy (MFM) to image the domains of ferrimagnetic MST. We find that magnetic field tunes between stripe and bubble domain morphologies, raising the possibility of topological spin textures. Moreover, we combine in situ transport with domain manipulation and imaging to both write MST device properties and directly measure the scaling of the Hall response with domain area. This work demonstrates measurement of the local anomalous Hall response using MFM, and opens the door to reconfigurable domain-based devices in the M(B,S)T family.

Two-dimensional moir\'e materials have emerged as the most versatile platforms for realizing quantum phases of electrons. Here, we explore the stability origins of correlated states in WSe2/WS2 moir\'e superlattices. We find that ultrafast electronic excitation leads to melting of the Mott states on time scales five times longer than predictions from the charge hopping integrals and the melting rates are thermally activated, with activation energies of 18 and 13 meV for the one- and two-hole Mott states, respectively, suggesting significant electron-phonon coupling. DFT calculation of the one-hole Mott state confirms polaron formation and yields a hole-polaron binding energy of 16 meV. These findings reveal a close interplay of electron-electron and electron-phonon interactions in stabilizing the polaronic Mott insulators at transition metal dichalcogenide moir\'e interfaces., Comment: 14 pages, 4 figures, 11 SI figures

Two-dimensional (2D) antiferromagnets have garnered considerable interest for the next generation of functional spintronics. However, many available bulk materials from which 2D antiferromagnets are isolated are limited by their sensitivity to air, low ordering temperatures, and insulating transport properties. TaFe$_{1+y}$Te$_3$ offers unique opportunities to address these challenges with increased air stability, metallic transport properties, and robust antiferromagnetic order. Here, we synthesize TaFe$_{1+y}$Te$_3$ ($y$ = 0.14), identify its structural, magnetic, and electronic properties, and elucidate the relationships between them. Axial-dependent high-field magnetization measurements on TaFe$_{1.14}$Te$_3$ reveal saturation magnetic fields ranging between 27-30 T with a saturation magnetic moment of 2.05-2.12 $\mu_B$. Magnetotransport measurements confirm TaFe$_{1.14}$Te$_3$ is metallic with strong coupling between magnetic order and electronic transport. Angle-resolved photoemission spectroscopy measurements across the magnetic transition uncover a complex interplay between itinerant electrons and local magnetic moments that drives the magnetic transition. We further demonstrate the ability to isolate few-layer sheets of TaFe$_{1.14}$Te$_3$ through mechanical exfoliation, establishing TaFe$_{1.14}$Te$_3$ as a potential platform for 2D spintronics based on metallic layered antiferromagnets., Comment: 30 pages, 5 main figures, 23 supporting figures, and 3 supporting tables

Material systems that exhibit tunable spin-selective conductivity are key components of spintronic technologies. Here we demonstrate a novel type of spin-selective transport, based on the unusual Landau level (LL) sequence observed in bilayer WSe$_2$ under large applied magnetic fields. We find that the conductivity depends strongly on the relative iso-spin ordering between conducting electrons in a partially filled LL and the localized electrons of lower energy filled LLs, with conductivity observed to be almost completely suppressed when the spin-ratio and field-tuned Coulomb energy exceed a critical threshold. Switching between "on/off" states is achievable through either modulation of the external magnetic or electric fields, with many-body interaction driving a collective switching mechanism. In contrast to magnetoresistive heterostructures, this system achieves electrically tunable spin filtering within a single material, driven by interaction between free and localized spins residing in energy-separated spin/valley polarized bands. Similar spin-selective conductivity may be realizable in multi-flat band systems at zero magnetic field.

Achieving electrostatic control of quantum phases is at the frontier of condensed matter research. Recent investigations have revealed superconductivity tunable by electrostatic doping in twisted graphene heterostructures and in two-dimensional (2D) semimetals such as WTe$_2$. Some of these systems have a polar crystal structure that gives rise to ferroelectricity, in which the interlayer polarization exhibits bistability driven by external electric fields. Here we show that bilayer $T_d$-MoTe$_2$ simultaneously exhibits ferroelectric switching and superconductivity. Remarkably, a field-driven, first-order superconductor-to-normal transition is observed at its ferroelectric transition. Bilayer $T_d$-MoTe$_2$ also has a maximum in its superconducting transition temperature ($T_\textrm{c}$) as a function of carrier density and temperature, allowing independent control of the superconducting state as a function of both doping and polarization. We find that the maximum $T_\textrm{c}$ is concomitant with compensated electron and hole carrier densities and vanishes when one of the Fermi pockets disappears with doping. We argue that this unusual polarization-sensitive 2D superconductor is driven by an interband pairing interaction associated with nearly nested electron and hole Fermi pockets.

Here, we describe synthesis of TMD crystals using a two-step flux growth method that eliminates a major potential source of contamination. Detailed characterization of TMDs grown by this two-step method reveals charged and isovalent defects with densities an order of magnitude lower than in TMDs grown by a single-step flux technique. Initial temperature-dependent electrical transport measurements of monolayer WSe2 yield room-temperature hole mobility above 840 cm2/Vs and low-temperature disorder-limited mobility above 44,000 cm2/Vs. Electrical transport measurements of graphene-WSe2 heterostructures fabricated from the two-step flux grown WSe2 also show superior performance: higher graphene mobility, lower charged impurity density, and well-resolved integer quantum Hall states.

Massive Dirac fermions are low-energy electronic excitations characterized by a hyperbolic band dispersion. They play a central role in several emerging physical phenomena such as topological phase transitions, anomalous Hall effects and superconductivity. This work demonstrates that massive Dirac fermions can be controllably induced by lithographically patterning superstructures of nanoscale holes in a graphene device. Their band dispersion is systematically visualized using angle-resolved photoemission spectroscopy with nanoscale spatial resolution. A linear scaling of effective mass with feature sizes is discovered, underlining the Dirac nature of the superstructures. In situ electrostatic doping dramatically enhances the effective hole mass and leads to the direct observation of an electronic band gap that results in a peak-to-peak band separation of (0.64 $\pm$ 0.03) eV, which is shown via first-principles calculations to be strongly renormalized by carrier-induced screening. The presented methodology outlines a new approach for band structure engineering guided by directly viewing structurally- and electrically-tunable massive Dirac quasiparticles in lithographic superstructures at the nanoscale., Comment: 37 pages, 12 figures (includes supporting information). A revised version has been published in ACS Nano

Forming a hetero-interface is a materials-design strategy that can access an astronomically large phase space. However, the immense phase space necessitates a high-throughput approach for optimal interface design. Here we introduce a high-throughput computational framework, InterMatch, for efficiently predicting charge transfer, strain, and superlattice structure of an interface by leveraging the databases of individual bulk materials. Specifically, the algorithm reads in the lattice vectors, density of states, and the stiffness tensors for each material in their isolated form from the Materials Project. From these bulk properties, InterMatch estimates the interfacial properties. We benchmark InterMatch predictions for the charge transfer against experimental measurements and supercell density-functional theory calculations. We then use InterMatch to predict promising interface candidates for doping transition metal dichalcogenide MoSe$_2$. Finally, we explain experimental observation of factor of 10 variation in the supercell periodicity within a few microns in graphene/$\alpha$-RuCl$_3$ by exploring low energy superlattice structures as a function of twist angle using InterMatch. We anticipate our open-source InterMatch algorithm accelerating and guiding ever-growing interfacial design efforts. Moreover, the interface database resulting from the InterMatch searches presented in this paper can be readily accessed through https://contribs.materialsproject.org/projects/intermatch/ .

The ability to control magnetic properties of materials is crucial for fundamental research and underpins many information technologies. In this context, two-dimensional materials are a particularly exciting platform due to their high degree of tunability and ease of implementation into nanoscale devices. Here we report two approaches for manipulating the A-type antiferromagnetic properties of the layered semiconductor CrSBr through hydrostatic pressure and ligand substitution. Hydrostatic pressure compresses the unit cell, increasing the interlayer exchange energy while lowering the N\'eel temperature. Ligand substitution, realized synthetically through Cl alloying, anisotropically compresses the unit cell and suppresses the Cr-halogen covalency, reducing the magnetocrystalline anisotropy energy and decreasing the N\'eel temperature. A detailed structural analysis combined with first-principles calculations reveal that alterations in the magnetic properties are intricately related to changes in direct Cr-Cr exchange interactions and the Cr-anion superexchange pathways. Further, we demonstrate that Cl alloying enables chemical tuning of the interlayer coupling from antiferromagnetic to ferromagnetic, which is unique amongst known two-dimensional magnets. The magnetic tunability, combined with a high ordering temperature, chemical stability, and functional semiconducting properties, make CrSBr an ideal candidate for pre- and post-synthetic design of magnetism in two-dimensional materials., Comment: Main text: 17 pages, 4 figures. Supporting Information: 34 pages, 32 figures, 4 tables

Twisted van der Waals multilayers are widely regarded as a rich platform to access novel electronic phases, thanks to the multiple degrees of freedom such as layer thickness and twist angle that allow control of their electronic and chemical properties. Here, we propose that the stacking domains that form naturally due to the relative twist between successive layers act as an additional "knob" for controlling the behavior of these systems, and report the emergence and engineering of stacking domain-dependent surface chemistry in twisted few-layer graphene. Using mid-infrared near-field optical microscopy and atomic force microscopy, we observe a selective adhesion of metallic nanoparticles and liquid water at the domains with rhombohedral stacking configurations of minimally twisted double bi- and tri-layer graphene. Furthermore, we demonstrate that the manipulation of nanoparticles located at certain stacking domains can locally reconfigure the moir\'e superlattice in their vicinity at the {\mu}m-scale. In addition, we report first-principles simulations of the energetics of adhesion of metal atoms and water molecules on the stacking domains in an attempt to elucidate the origin of the observed selective adhesion. Our findings establish a new approach to controlling moir\'e-assisted chemistry and nanoengineering., Comment: 11 pages, 3 figures

Transport measurement of electron optics in monolayer graphene p-n junction devices has been traditionally studied with negative refraction and chiral transmission experiments in Hallbar magnetic focusing set-ups. We show direct signatures of Klein (monolayer) and anti-Klein (bilayer) tunneling with a circular 'edgeless' Corbino geometry made out of gated graphene p-n junctions. Noticeable in particular is the appearance of angular sweet spots (Brewster angles) in the magnetoconductance data of bilayer graphene, which minimizes head-on transmission, contrary to conventional Fresnel optics or monolayer graphene which shows instead a sharpened collimation of transmission paths. The local maxima on the bilayer magnetoconductance plots migrate to higher fields with increasing doping density. These experimental results are in good agreement with detailed numerical simulations and analytical predictions.

Moir\'e superlattices in twisted two-dimensional materials have generated tremendous excitement as a platform for achieving quantum properties on demand. However, the moir\'e pattern is highly sensitive to the interlayer atomic registry, and current assembly techniques suffer from imprecise control of the average twist angle, spatial inhomogeneity in the local twist angle, and distortions due to random strain. Here, we demonstrate a new way to manipulate the moir\'e patterns in hetero- and homo-bilayers through in-plane bending of monolayer ribbons, using the tip of an atomic force microscope. This technique achieves continuous variation of twist angles with improved twist-angle homogeneity and reduced random strain, resulting in moir\'e patterns with highly tunable wavelength and ultra-low disorder. Our results pave the way for detailed studies of ultra-low disorder moir\'e systems and the realization of precise strain-engineered devices.

Two-dimensional (2D) transition metal dichalcogenides (TMDC) and their moir\'e interfaces have been demonstrated for correlated electron states, including Mott insulators and electron/hole crystals commensurate with moir\'e superlattices. Here we present spectroscopic evidences for ordered bosons - interlayer exciton crystals in a WSe2/MoSe2/WSe2 trilayer, where the enhanced Coulomb interactions over those in heterobilayers have been predicted to result in exciton ordering. While the dipolar interlayer excitons in the heterobilayer may be ordered by the periodic moir\'e traps, their mutual repulsion results in de-trapping at exciton density n_ex larger than 10^11 cm^-2 to form mobile exciton gases and further to electron-hole plasmas, both accompanied by broadening in photoluminescence (PL) peaks and large increases in mobility. In contrast, ordered interlayer excitons in the trilayer are characterized by negligible mobility and by sharper PL peaks persisting to n_ex approximately 10^12 cm^-2. We present evidences for the predicted quadrupolar exciton crystal and its transitions to dipolar excitons either with increasing n_ex or by an applied electric field. These ordered interlayer excitons may serve as models for the exploration of quantum phase transitions and quantum coherent phenomena., Comment: 19 pages, 4 figures, SI

Plasmon polaritons in van der Waals (vdW) materials hold promise for next-generation photonics. The ability to deterministically imprint spatial patterns of high carrier density in cavities and circuitry with nanoscale features underlies future progress in nonlinear nanophotonics and strong light-matter interactions. Here, we demonstrate a general strategy to atomically imprint low-loss graphene plasmonic structures using oxidation-activated charge transfer (OCT). We cover graphene with a monolayer of WSe$_2$, which is subsequently oxidized into high work-function WOx to activate charge transfer. Nano-infrared imaging reveals low-loss plasmon polaritons at the WOx/graphene interface. We insert WSe$_2$ spacers to precisely control the OCT-induced carrier density and achieve a near-intrinsic quality factor of plasmons. Finally, we imprint canonical plasmonic cavities exhibiting laterally abrupt doping profiles with single-digit nanoscale precision via programmable OCT. Specifically, we demonstrate technologically appealing but elusive plasmonic whispering-gallery resonators based on free-standing graphene encapsulated in WOx. Our results open avenues for novel quantum photonic architectures incorporating two-dimensional materials., Comment: 17 pages, 4 figures

We introduce a novel planar tunneling architecture for van der Waals heterostructures based on via contacts, namely metallic contacts embedded into through-holes in hexagonal boron nitride ($h$BN). We use the via-based tunneling method to study the single-particle density of states of two different two-dimensional (2D) materials, NbSe$_2$ and graphene. In NbSe$_2$ devices, we characterize the barrier strength and interface disorder for barrier thicknesses of 0, 1 and 2 layers of $h$BN and study the dependence on tunnel-contact area down to $(44 \pm 14)^2 $ nm$^2$. For 0-layer $h$BN devices, we demonstrate a crossover from diffusive to point contacts in the small-contact-area limit. In graphene, we show that reducing the tunnel barrier thickness and area can suppress effects due to phonon-assisted tunneling and defects in the $h$BN barrier. This via-based architecture overcomes limitations of other planar tunneling designs and produces high-quality, ultra-clean tunneling structures from a variety of 2D materials.

Two-dimensional (2D) magnetic semiconductors feature both tightly-bound excitons with large oscillator strength and potentially long-lived coherent magnons due to the presence of bandgap and spatial confinement. While magnons and excitons are energetically mismatched by orders of magnitude, their coupling can lead to efficient optical access to spin information. Here we report strong magnon-exciton coupling in the 2D van der Waals (vdW) antiferromagnetic (AFM) semiconductor CrSBr. Coherent magnons launched by above-gap excitation modulate the interlayer hybridization, which leads to dynamic modulation of excitonic energies. Time-resolved exciton sensing reveals magnons that can coherently travel beyond 7 micrometer, with coherence time above 5 ns. We observe this exciton-coupled coherent magnons in both even and odd number of layers, with and without compensated magnetization, down to the bilayer limit. Given the versatility of vdW heterostructures, these coherent 2D magnons may be basis for optically accessible magnonics and quantum interconnects., Comment: 14 pages, 5 figures, 30 pages Supporting Info

Two-dimensional (2D) materials can host stable, long-range magnetic phases in the presence of underlying magnetic anisotropy. The ability to realize the full potential of 2D magnets necessitates systematic investigation of the role of individual atomic layers and nanoscale inhomogeneity ($\textit{i.e.}$, strain) on the emergence and stability of both intra- and interlayer magnetic phases. Here, we report multifaceted spatial-dependent magnetism in few-layer CrSBr using magnetic force microscopy (MFM) and Monte Carlo-based magnetic simulations. We perform nanoscale visualization of the magnetic sheet susceptibility from raw MFM data and force-distance curves, revealing a characteristic onset of both intra- and interlayer magnetic correlations as a function of temperature and layer-thickness. We demonstrate that the presence of a single uncompensated layer in odd-layer terraces significantly reduces the stability of the low-temperature antiferromagnetic (AFM) phase and gives rise to multiple coexisting magnetic ground states at temperatures close to the bulk N\'eel temperature ($\textit{T}$$_N$). Furthermore, the AFM phase can be reliably suppressed using modest fields (~300 Oe) from the MFM probe, behaving as a nanoscale magnetic switch. Our prototypical study of few-layer CrSBr demonstrates the critical role of layer parity on field-tunable 2D magnetism and provides vital design criteria for future nanoscale magnetic devices. Moreover, we provide a roadmap for using MFM for nano-magnetometry of 2D materials, despite the ubiquitous absence of bulk zero-field magnetism in magnetized sheets., Comment: Main text: 30 pages, 4 figures. Supporting Information: 19 pages, 8 figures

The ability to create high-quality lateral p-n junctions at nanometer length scales is essential for the next generation of two-dimensional (2D) electronic and plasmonic devices. Using a charge-transfer heterostructure consisting of graphene on $\alpha$-RuCl$_3$, we conduct a proof-of-concept study demonstrating the existence of intrinsic nanoscale lateral p-n junctions in the vicinity of graphene nanobubbles. Our multi-pronged experimental approach incorporates scanning tunneling microscopy (STM) and spectroscopy (STS) and scattering-type scanning near-field optical microscopy ($\textit{s}$-SNOM) in order to simultaneously probe both the electronic and optical responses of nanobubble p-n junctions. Our STM and STS results reveal that p-n junctions with a band offset of more than 0.6 eV can be achieved over lateral length scale of less than 3 nm, giving rise to a staggering effective in-plane field in excess of 10$^8$ V/m. Concurrent $\textit{s}$-SNOM measurements confirm the utility of these nano-junctions in plasmonically-active media, and validate the use of a point-scatterer formalism for modeling surface plasmon polaritons (SPPs). Model $\textit{ab initio}$ density functional theory (DFT) calculations corroborate our experimental data and reveal a combination of sub-angstrom and few-angstrom decay processes dictating the dependence of charge transfer on layer separation. Our study provides experimental and conceptual foundations for the use of charge-transfer interfaces such as graphene/$\alpha$-RuCl$_3$ to generate p-n nano-junctions., Comment: D.J.R., S.S., B.S.J., and J.Z. contributed equally. File contains main manuscript (14 pages, 4 figures) and supplementary information (13 pages, 4 figures)

Magic angle twisted trilayer graphene (TTG) has recently emerged as a new platform to engineer strongly correlated flat bands. Here, we reveal the structural and electronic properties of TTG using low temperature scanning tunneling microscopy at twist angles for which superconductivity has been observed. Real trilayer samples deviate from their idealized structure due to a strong reconstruction of the moir\'e lattice, which locks layers into near-magic angle, mirror symmetric domains comparable in size to the superconducting coherence length. The price for this magic relaxation is the introduction of an array of localized twist angle faults, termed twistons. These novel, gate-tunable moir\'e defects offer a natural explanation for the superconducting dome observed in transport and provide an avenue to probe superconducting pairing mechanisms through disorder tuning.

Hybrid superconductor/graphene (SC/g) junctions are excellent candidates for investigating correlations between Cooper pairs and quantum Hall (QH) edge modes. Experimental studies are challenging as Andreev reflections are extremely sensitive to junction disorder and high magnetic fields are required to form QH edge states. We fabricated low-resistance SC/g interfaces, composed of graphene edge contacted with NbN with a barrier strength of $Z\approx 0.4$, that remain superconducting under magnetic fields larger than $18$ T. We establish the role of graphene's Dirac band structure on zero-field Andreev reflections and demonstrate dynamic tunability of the Andreev reflection spectrum by moving the boundary between specular and retro Andreev reflections with parallel magnetic fields. Through the application of perpendicular magnetic fields, we observe an oscillatory suppression of the 2-probe conductance in the $\nu = 4$ Landau level attributed to the reduced efficiency of Andreev processes at the NbN/g interface, consistent with theoretical predictions.

Exciton condensates (EC) are macroscopic coherent states arising from condensation of electron-hole pairs. Bilayer heterostructures, consisting of two-dimensional electron and hole layers separated by a tunnel barrier, provide a versatile platform to realize and study EC. The tunnel barrier suppresses recombination yielding long-lived excitons. However, this separation also reduces interlayer Coulomb interactions, limiting the exciton binding strength. Here, we report the observation of EC in naturally occurring 2H-stacked bilayer WSe$_2$. In this system, the intrinsic spin-valley structure suppresses interlayer tunneling even when the separation is reduced to the atomic limit, providing access to a previously unattainable regime of strong interlayer coupling. Using capacitance spectroscopy, we investigate magneto-EC, formed when partially filled Landau levels (LL) couple between the layers. We find that the strong-coupling EC show dramatically different behaviour compared with previous reports, including an unanticipated variation of the EC robustness with the orbital number, and find evidence for a transition between two types of low-energy charged excitations. Our results provide a demonstration of tuning EC properties by varying the constituent single-particle wavefunctions.

Deep learning (DL) is an emerging analysis tool across sciences and engineering. Encouraged by the successes of DL in revealing quantitative trends in massive imaging data, we applied this approach to nano-scale deeply sub-diffractional images of propagating polaritonic waves in complex materials. We developed a practical protocol for the rapid regression of images that quantifies the wavelength and the quality factor of polaritonic waves utilizing the convolutional neural network (CNN). Using simulated near-field images as training data, the CNN can be made to simultaneously extract polaritonic characteristics and materials parameters in a timescale that is at least three orders of magnitude faster than common fitting/processing procedures. The CNN-based analysis was validated by examining the experimental near-field images of charge-transfer plasmon polaritons at Graphene/{\alpha}-RuCl3 interfaces. Our work provides a general framework for extracting quantitative information from images generated with a variety of scanning probe methods.

Magnetic semiconductors are a powerful platform for understanding, utilizing and tuning the interplay between magnetic order and electronic transport. Compared to bulk crystals, two-dimensional magnetic semiconductors have greater tunability, as illustrated by the gate modulation of magnetism in exfoliated CrI$_3$ and Cr$_2$Ge$_2$Te$_6$, but their electrically insulating properties limit their utility in devices. Here we report the simultaneous electrostatic and magnetic control of electronic transport in atomically-thin CrSBr, an A-type antiferromagnetic semiconductor. Through magnetotransport measurements, we find that spin-flip scattering from the interlayer antiferromagnetic configuration of multilayer flakes results in giant negative magnetoresistance. Conversely, magnetoresistance of the ferromagnetic monolayer CrSBr vanishes below the Curie temperature. A second transition ascribed to the ferromagnetic ordering of magnetic defects manifests in a large positive magnetoresistance in the monolayer and a sudden increase of the bulk magnetic susceptibility. We demonstrate this magnetoresistance is tunable with an electrostatic gate, revealing that the ferromagnetic coupling of defects is carrier mediated.

We present transport measurements of bilayer graphene with 1.38{\deg} interlayer twist and apparent additional alignment to its hexagonal boron nitride cladding. As with other devices with twist angles substantially larger than the magic angle of 1.1{\deg}, we do not observe correlated insulating states or band reorganization. However, we do observe several highly unusual behaviors in magnetotransport. For a large range of densities around half filling of the moir\'e bands, magnetoresistance is large and quadratic. Over these same densities, the magnetoresistance minima corresponding to gaps between Landau levels split and bend as a function of density and field. We reproduce the same splitting and bending behavior in a simple tight-binding model of Hofstadter's butterfly on a square lattice with anisotropic hopping terms. These features appear to be a generic class of experimental manifestations of Hofstadter's butterfly and may provide insight into the emergent states of twisted bilayer graphene., Comment: 8 pages, 4 figures; updated supplemental material; added additional device measurements and updated toy model