Two-dimensional heavy fermions in the van der Waals metal CeSiI.

Heavy-fermion metals are prototype systems for observing emergent quantum phases driven by electronic interactions1-6. A long-standing aspiration is the dimensional reduction of these materials to exert control over their quantum phases7-11, which remains a significant challenge because traditional intermetallic heavy-fermion compounds have three-dimensional atomic and electronic structures. Here we report comprehensive thermodynamic and spectroscopic evidence of an antiferromagnetically ordered heavy-fermion ground state in CeSiI, an intermetallic comprising two-dimensional (2D) metallic sheets held together by weak interlayer van der Waals (vdW) interactions. Owing to its vdW nature, CeSiI has a quasi-2D electronic structure, and we can control its physical dimension through exfoliation. The emergence of coherent hybridization of f and conduction electrons at low temperature is supported by the temperature evolution of angle-resolved photoemission and scanning tunnelling spectra near the Fermi level and by heat capacity measurements. Electrical transport measurements on few-layer flakes reveal heavy-fermion behaviour and magnetic order down to the ultra-thin regime. Our work establishes CeSiI and related materials as a unique platform for studying dimensionally confined heavy fermions in bulk crystals and employing 2D device fabrication techniques and vdW heterostructures12 to manipulate the interplay between Kondo screening, magnetic order and proximity effects.

Smectic pair-density-wave order in EuRbFe4As4.

The pair density wave (PDW) is a superconducting state in which Cooper pairs carry centre-of-mass momentum in equilibrium, leading to the breaking of translational symmetry1-4. Experimental evidence for such a state exists in high magnetic field5-8 and in some materials that feature density-wave orders that explicitly break translational symmetry9-13. However, evidence for a zero-field PDW state that exists independent of other spatially ordered states has so far been elusive. Here we show that such a state exists in the iron pnictide superconductor EuRbFe4As4, a material that features co-existing superconductivity (superconducting transition temperature (Tc) ≈ 37 kelvin) and magnetism (magnetic transition temperature (Tm) ≈ 15 kelvin)14,15. Using spectroscopic imaging scanning tunnelling microscopy (SI-STM) measurements, we show that the superconducting gap at low temperature has long-range, unidirectional spatial modulations with an incommensurate period of about eight unit cells. Upon increasing the temperature above Tm, the modulated superconductor disappears, but a uniform superconducting gap survives to Tc. When an external magnetic field is applied, gap modulations disappear inside the vortex halo. The SI-STM and bulk measurements show the absence of other density-wave orders, indicating that the PDW state is a primary, zero-field superconducting state in this compound. Both four-fold rotational symmetry and translation symmetry are recovered above Tm, indicating that the PDW is a smectic order.

Coupled ferroelectricity and superconductivity in bilayer Td-MoTe2.

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 semimetals such as WTe2 (refs. 1-5). 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 fields6-8. Here we show that bilayer Td-MoTe2 simultaneously exhibits ferroelectric switching and superconductivity. Notably, a field-driven, first-order superconductor-to-normal transition is observed at its ferroelectric transition. Bilayer Td-MoTe2 also has a maximum in its superconducting transition temperature (Tc) 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 Tc 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 two-dimensional superconductor is driven by an interband pairing interaction associated with nearly nested electron and hole Fermi pockets.

Quantum criticality in twisted transition metal dichalcogenides.

Near the boundary between ordered and disordered quantum phases, several experiments have demonstrated metallic behaviour that defies the Landau Fermi paradigm1-5. In moiré heterostructures, gate-tuneable insulating phases driven by electronic correlations have been recently discovered6-23. Here, we use transport measurements to characterize metal-insulator transitions (MITs) in twisted WSe2 near half filling of the first moiré subband. We find that the MIT as a function of both density and displacement field is continuous. At the metal-insulator boundary, the resistivity displays strange metal behaviour at low temperatures, with dissipation comparable to that at the Planckian limit. Further into the metallic phase, Fermi liquid behaviour is recovered at low temperature, and this evolves into a quantum critical fan at intermediate temperatures, before eventually reaching an anomalous saturated regime near room temperature. An analysis of the residual resistivity indicates the presence of strong quantum fluctuations in the insulating phase. These results establish twisted WSe2 as a new platform to study doping and bandwidth-controlled metal-insulator quantum phase transitions on the triangular lattice.

Maximized electron interactions at the magic angle in twisted bilayer graphene.

The electronic properties of heterostructures of atomically thin van der Waals crystals can be modified substantially by moiré superlattice potentials from an interlayer twist between crystals1,2. Moiré tuning of the band structure has led to the recent discovery of superconductivity3,4 and correlated insulating phases5 in twisted bilayer graphene (TBG) near the 'magic angle' of twist of about 1.1 degrees, with a phase diagram reminiscent of high-transition-temperature superconductors. Here we directly map the atomic-scale structural and electronic properties of TBG near the magic angle using scanning tunnelling microscopy and spectroscopy. We observe two distinct van Hove singularities (VHSs) in the local density of states around the magic angle, with an energy separation of 57 millielectronvolts that drops to 40 millielectronvolts with high electron/hole doping. Unexpectedly, the VHS energy separation continues to decrease with decreasing twist angle, with a lowest value of 7 to 13 millielectronvolts at a magic angle of 0.79 degrees. More crucial to the correlated behaviour of this material, we find that at the magic angle, the ratio of the Coulomb interaction to the bandwidth of each individual VHS (U/t) is maximized, which is optimal for electronic Cooper pairing mechanisms. When doped near the half-moiré-band filling, a correlation-induced gap splits the conduction VHS with a maximum size of 6.5 millielectronvolts at 1.15 degrees, dropping to 4 millielectronvolts at 0.79 degrees. We capture the doping-dependent and angle-dependent spectroscopy results using a Hartree-Fock model, which allows us to extract the on-site and nearest-neighbour Coulomb interactions. This analysis yields a U/t of order unity indicating that magic-angle TBG is moderately correlated. In addition, scanning tunnelling spectroscopy maps reveal an energy- and doping-dependent three-fold rotational-symmetry breaking of the local density of states in TBG, with the strongest symmetry breaking near the Fermi level and further enhanced when doped to the correlated gap regime. This indicates the presence of a strong electronic nematic susceptibility or even nematic order in TBG in regions of the phase diagram where superconductivity is observed.

Tunable Magnetic Domains in Ferrimagnetic MnSb2Te4.

Highly tunable properties make Mn(Bi,Sb)2Te4 a rich playground for exploring the interplay between band topology and magnetism: On one end, MnBi2Te4 is an antiferromagnetic topological insulator, while the magnetic structure of MnSb2Te4 (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 the 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.

Accelerated Nano-Optical Imaging through Sparse Sampling.

The integration time and signal-to-noise ratio are inextricably linked when performing scanning probe microscopy based on raster scanning. This often yields a large lower bound on the measurement time, for example, in nano-optical imaging experiments performed using a scanning near-field optical microscope (SNOM). Here, we utilize sparse scanning augmented with Gaussian process regression to bypass the time constraint. We apply this approach to image charge-transfer polaritons in graphene residing on ruthenium trichloride (α-RuCl3) and obtain key features such as polariton damping and dispersion. Critically, nano-optical SNOM imaging data obtained via sparse sampling are in good agreement with those extracted from traditional raster scans but require 11 times fewer sampled points. As a result, Gaussian process-aided sparse spiral scans offer a major decrease in scanning time.

Moiréless correlations in ABCA graphene.

Atomically thin van der Waals materials stacked with an interlayer twist have proven to be an excellent platform toward achieving gate-tunable correlated phenomena linked to the formation of flat electronic bands. In this work we demonstrate the formation of emergent correlated phases in multilayer rhombohedral graphene--a simple material that also exhibits a flat electronic band edge but without the need of having a moiré superlattice induced by twisted van der Waals layers. We show that two layers of bilayer graphene that are twisted by an arbitrary tiny angle host large (micrometer-scale) regions of uniform rhombohedral four-layer (ABCA) graphene that can be independently studied. Scanning tunneling spectroscopy reveals that ABCA graphene hosts an unprecedentedly sharp van Hove singularity of 3-5-meV half-width. We demonstrate that when this van Hove singularity straddles the Fermi level, a correlated many-body gap emerges with peak-to-peak value of 9.5 meV at charge neutrality. Mean-field theoretical calculations for model with short-ranged interactions indicate that two primary candidates for the appearance of this broken symmetry state are a charge-transfer excitonic insulator and a ferrimagnet. Finally, we show that ABCA graphene hosts surface topological helical edge states at natural interfaces with ABAB graphene which can be turned on and off with gate voltage, implying that small-angle twisted double-bilayer graphene is an ideal programmable topological quantum material.

Polaritonic Probe of an Emergent 2D Dipole Interface.

The use of work-function-mediated charge transfer has recently emerged as a reliable route toward nanoscale electrostatic control of individual atomic layers. Using α-RuCl3 as a 2D electron acceptor, we are able to induce emergent nano-optical behavior in hexagonal boron nitride (hBN) that arises due to interlayer charge polarization. Using scattering-type scanning near-field optical microscopy (s-SNOM), we find that a thin layer of α-RuCl3 adjacent to an hBN slab reduces the propagation length of hBN phonon polaritons (PhPs) in significant excess of what can be attributed to intrinsic optical losses. Concomitant nano-optical spectroscopy experiments reveal a novel resonance that aligns energetically with the region of excess PhP losses. These experimental observations are elucidated by first-principles density-functional theory and near-field model calculations, which show that the formation of a large interfacial dipole suppresses out-of-plane PhP propagation. Our results demonstrate the potential utility of charge-transfer heterostructures for tailoring optoelectronic properties of 2D insulators.

Quenched Excitons in WSe2/α-RuCl3 Heterostructures Revealed by Multimessenger Nanoscopy.

We investigate heterostructures composed of monolayer WSe2 stacked on α-RuCl3 using a combination of Terahertz (THz) and infrared (IR) nanospectroscopy and imaging, scanning tunneling spectroscopy (STS), and photoluminescence (PL). Our observations reveal itinerant carriers in the heterostructure prompted by charge transfer across the WSe2/α-RuCl3 interface. Local STS measurements show the Fermi level is shifted to the valence band edge of WSe2 which is consistent with p-type doping and verified by density functional theory (DFT) calculations. We observe prominent resonances in near-IR nano-optical and PL spectra, which are associated with the A-exciton of WSe2. We identify a concomitant, near total, quenching of the A-exciton resonance in the WSe2/α-RuCl3 heterostructure. Our nano-optical measurements show that the charge-transfer doping vanishes while excitonic resonances exhibit near-total recovery in "nanobubbles", where WSe2 and α-RuCl3 are separated by nanometer distances. Our broadband nanoinfrared inquiry elucidates local electrodynamics of excitons and an electron-hole plasma in the WSe2/α-RuCl3 system.

Interplay between Local Moment and Itinerant Magnetism in the Layered Metallic Antiferromagnet TaFe1.14Te3.

Two-dimensional antiferromagnets have garnered considerable interest for the next generation of functional spintronics. However, many bulk materials from which two-dimensional antiferromagnets are isolated are limited by their air sensitivity, low ordering temperatures, and insulating transport properties. TaFe1+yTe3 aims to address these challenges with increased air stability, metallic transport, and robust antiferromagnetism. Here, we synthesize TaFe1+yTe3 (y = 0.14), identify its structural, magnetic, and electronic properties, and elucidate the relationships between them. Axial-dependent high-field magnetization measurements on TaFe1.14Te3 reveal saturation magnetic fields ranging between 27 and 30 T with saturation magnetic moments of 2.05-2.12 µB. Magnetotransport measurements confirm that TaFe1.14Te3 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 demonstrate the ability to isolate few-layer sheets of TaFe1.14Te3, establishing TaFe1.14Te3 as a potential platform for two-dimensional spintronics.

Coupling between magnetic order and charge transport in a two-dimensional magnetic semiconductor.

Semiconductors, featuring tunable electrical transport, and magnets, featuring tunable spin configurations, form the basis of many information technologies. A long-standing challenge has been to realize materials that integrate and connect these two distinct properties. Two-dimensional (2D) materials offer a platform to realize this concept, but known 2D magnetic semiconductors are electrically insulating in their magnetic phase. Here we demonstrate tunable electron transport within the magnetic phase of the 2D semiconductor CrSBr and reveal strong coupling between its magnetic order and charge transport. This provides an opportunity to characterize the layer-dependent magnetic order of CrSBr down to the monolayer via magnetotransport. Exploiting the sensitivity of magnetoresistance to magnetic order, we uncover a second regime characterized by coupling between charge carriers and magnetic defects. The magnetoresistance within this regime can be dynamically and reversibly tuned by varying the carrier concentration using an electrostatic gate, providing a mechanism for controlling charge transport in 2D magnets.

Ultralocalized Optoelectronic Properties of Nanobubbles in 2D Semiconductors.

The optical properties of transition-metal dichalcogenides have previously been modified at the nanoscale by using mechanical and electrical nanostructuring. However, a clear experimental picture relating the local electronic structure with emission properties in such structures has so far been lacking. Here, we use a combination of scanning tunneling microscopy (STM) and near-field photoluminescence (nano-PL) to probe the electronic and optical properties of single nanobubbles in bilayer heterostructures of WSe2 on MoSe2. We show from tunneling spectroscopy that there are electronic states deeply localized in the gap at the edge of such bubbles, which are independent of the presence of chemical defects in the layers. We also show a significant change in the local band gap on the bubble, with a continuous evolution to the edge of the bubble over a length scale of ∼20 nm. Nano-PL measurements observe a continuous redshift of the interlayer exciton on entering the bubble, in agreement with the band-to-band transitions measured by STM. We use self-consistent Schrödinger-Poisson simulations to capture the essence of the experimental results and find that strong doping in the bubble region is a key ingredient to achieving the observed localized states, together with mechanical strain.

Nanoscale Femtosecond Dynamics of Mott Insulator (Ca0.99Sr0.01)2RuO4.

Ca2RuO4 is a transition-metal oxide that exhibits a Mott insulator-metal transition (IMT) concurrent with a symmetry-preserving Jahn-Teller distortion (JT) at 350 K. The coincidence of these two transitions demonstrates a high level of coupling between the electronic and structural degrees of freedom in Ca2RuO4. Using spectroscopic measurements with nanoscale spatial resolution, we interrogate the interplay of the JT and IMT through the temperature-driven transition. Then, we introduce photoexcitation with subpicosecond temporal resolution to explore the coupling of the JT and IMT via electron-hole injection under ambient conditions. Through the temperature-driven IMT, we observe phase coexistence in the form of a stripe phase existing at the domain wall between macroscopic insulating and metallic domains. Through ultrafast carrier injection, we observe the formation of midgap states via enhanced optical absorption. We propose that these midgap states become trapped by lattice polarons originating from the local perturbation of the JT.

Nanometer-Scale Lateral p-n Junctions in Graphene/α-RuCl3 Heterostructures.

The ability to create nanometer-scale lateral p-n junctions is essential for the next generation of two-dimensional (2D) devices. Using the charge-transfer heterostructure graphene/α-RuCl3, we realize nanoscale lateral p-n junctions in the vicinity of graphene nanobubbles. Our multipronged experimental approach incorporates scanning tunneling microscopy (STM) and spectroscopy (STS) and scattering-type scanning near-field optical microscopy (s-SNOM) to simultaneously probe the electronic and optical responses of nanobubble p-n junctions. Our STM/STS results reveal that p-n junctions with a band offset of ∼0.6 eV can be achieved with widths of ∼3 nm, giving rise to electric fields of order 108 V/m. Concurrent s-SNOM measurements validate a point-scatterer formalism for modeling the interaction of surface plasmon polaritons (SPPs) with nanobubbles. Ab initio density functional theory (DFT) calculations corroborate our experimental data and reveal the dependence of charge transfer on layer separation. Our study provides experimental and conceptual foundations for generating p-n nanojunctions in 2D materials.

Nonmonotonic Temperature-Dependent Dissipation at Nonequilibrium in Atomically Thin Clean-Limit Superconductors.

Resistance in superconductors arises from the motion of vortices driven by flowing supercurrents or external electromagnetic fields and may be strongly affected by thermal or quantum fluctuations. The common expectation is that as the temperature is lowered, vortex motion is suppressed, leading to a decreased resistance. We show experimentally that in clean-limit atomically thin 2H-NbSe2 the resistance below the superconducting transition temperature may be nonmonotonic, passing through a minimum before increasing again as the temperature is decreased further. The effect is most pronounced in monolayer devices and cannot be understood in terms of known mechanisms. We propose a qualitative two-fluid vortex model in which thermal fluctuations of pinned vortices control the mobility of the free vortices. The findings provide a new perspective on fundamental questions of vortex mobility and dissipation in superconductors.

Andreev Reflections in NbN/Graphene Junctions under Large Magnetic Fields.

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 ≈ 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 ν = 4 Landau level attributed to the reduced efficiency of Andreev processes at the NbN/g interface, consistent with theoretical predictions.

Enhanced Superconductivity in Monolayer Td-MoTe2.

Crystalline two-dimensional (2D) superconductors (SCs) with low carrier density are an exciting new class of materials in which electrostatic gating can tune superconductivity, electronic interactions play a prominent role, and electrical transport properties may directly reflect the topology of the Fermi surface. Here, we report the dramatic enhancement of superconductivity with decreasing thickness in semimetallic Td-MoTe2, with critical temperature (Tc) increasing up to 7.6 K for monolayers, a 60-fold increase with respect to the bulk Tc. We show that monolayers possess a similar electronic structure and density of states (DOS) as the bulk, implying that electronic interactions play a strong role in the enhanced superconductivity. Reflecting the low carrier density, the critical temperature, magnetic field, and current density are all tunable by an applied gate voltage. The response to high in-plane magnetic fields is distinct from that of other 2D SCs and reflects the canted spin texture of the electron pockets.

Excitons in strain-induced one-dimensional moiré potentials at transition metal dichalcogenide heterojunctions.

The possibility of confining interlayer excitons in interfacial moiré patterns has recently gained attention as a strategy to form ordered arrays of zero-dimensional quantum emitters and topological superlattices in transition metal dichalcogenide heterostructures. Strain is expected to play an important role in the modulation of the moiré potential landscape, tuning the array of quantum dot-like zero-dimensional traps into parallel stripes of one-dimensional quantum wires. Here, we present real-space imaging of unstrained zero-dimensional and strain-induced one-dimensional moiré patterns along with photoluminescence measurements of the corresponding excitonic emission from WSe2/MoSe2 heterobilayers. Whereas excitons in zero-dimensional moiré traps display quantum emitter-like sharp photoluminescence peaks with circular polarization, the photoluminescence emission from excitons in one-dimensional moiré potentials shows linear polarization and two orders of magnitude higher intensity. These results establish strain engineering as an effective method to tailor moiré potentials and their optoelectronic response on demand.

Correlated electronic phases in twisted bilayer transition metal dichalcogenides.

In narrow electron bands in which the Coulomb interaction energy becomes comparable to the bandwidth, interactions can drive new quantum phases. Such flat bands in twisted graphene-based systems result in correlated insulator, superconducting and topological states. Here we report evidence of low-energy flat bands in twisted bilayer WSe2, with signatures of collective phases observed over twist angles that range from 4 to 5.1°. At half-band filling, a correlated insulator appeared that is tunable with both twist angle and displacement field. At a 5.1° twist, zero-resistance pockets were observed on doping away from half filling at temperatures below 3 K, which indicates a possible transition to a superconducting state. The observation of tunable collective phases in a simple band, which hosts only two holes per unit cell at full filling, establishes twisted bilayer transition metal dichalcogenides as an ideal platform to study correlated physics in two dimensions on a triangular lattice.