Quick-connect scanning tunneling microscope head with nested piezoelectric coarse walkers.

To meet changing research demands, new scanning tunneling microscope (STM) features must constantly evolve. We describe the design, development, and performance of a modular plug-in STM, which is compact and stable. The STM head is equipped with a quick-connect socket that is matched to a universal connector plug, enabling it to be transferred between systems. This head can be introduced into a vacuum system via a load-lock and transferred to various sites equipped with the connector plug, permitting multi-site STM operation. Its design allows for reliable operation in a variety of experimental conditions, including a broad temperature range, ultra-high vacuum, high magnetic fields, and closed-cycle pulse-tube cooling. The STM's compact size is achieved by a novel nested piezoelectric coarse walker design, which allows for large orthogonal travel in the X, Y, and Z directions, ideal for studying both bulk and thin film samples ranging in size from mm to µm. Its stability and noise tolerance are demonstrated by achieving atomic resolution under ambient conditions on a laboratory desktop with no vibrational or acoustic isolation. The operation of the nested coarse walkers is demonstrated by successful navigation to a µm-sized 2D sample.

Spatial Interactions in Hydrogenated Perovskite Nickelate Synaptic Networks.

A key aspect of how the brain learns and enables decision-making processes is through synaptic interactions. Electrical transmission and communication in a network of synapses are modulated by extracellular fields generated by ionic chemical gradients. Emulating such spatial interactions in synthetic networks can be of potential use for neuromorphic learning and the hardware implementation of artificial intelligence. Here, we demonstrate that in a network of hydrogen-doped perovskite nickelate devices, electric bias across a single junction can tune the coupling strength between the neighboring cells. Electrical transport measurements and spatially resolved diffraction and nanoprobe X-ray and scanning microwave impedance spectroscopic studies suggest that graded proton distribution in the inhomogeneous medium of hydrogen-doped nickelate film enables this behavior. We further demonstrate signal integration through the coupling of various junctions.

Moiré Potential, Lattice Relaxation, and Layer Polarization in Marginally Twisted MoS2 Bilayers.

Artificially twisted heterostructures of semiconducting transition-metal dichalcogenides (TMDs) offer unprecedented control over their electronic and optical properties via the spatial modulation of interlayer interactions and structural reconstruction. Here we study twisted MoS2 bilayers in a wide range of twist angles near 0° using scanning tunneling microscopy/spectroscopy. We investigate the twist angle dependence of the moiré pattern, which is dominated by lattice reconstruction for small angles (<2°), leading to large triangular domains with rhombohedral stacking. Local spectroscopy measurements reveal a large moiré-potential strength of 100-200 meV for angles <3°. In reconstructed regions, we see a bias-dependent asymmetry between neighboring triangular domains, which we relate to the vertical polarization that is intrinsic to rhombohedral stacked TMDs. This viewpoint is further supported by spectroscopy maps and ambient piezoresponse measurements. Our results provide a microscopic perspective of this new class of interfacial ferroelectrics and can offer clues for designing novel heterostructures that harness this effect.

Intrinsic (Trap-Free) Transistors Based on Epitaxial Single-Crystal Perovskites.

The first experimental realization of the intrinsic (not dominated by defects) charge conduction regime in lead-halide perovskite field-effect transistors (FETs) is reported. The advance is enabled by: i) a new vapor-phase epitaxy technique that results in large-area single-crystalline cesium lead bromide (CsPbBr3 ) films with excellent structural and surface properties, including atomically flat surface morphology, essentially free from defects and traps at the level relevant to device operation; ii) an extensive materials analysis of these films using a variety of thin-film and surface probes certifying the chemical and structural quality of the material; and iii) the fabrication of nearly ideal (trap-free) FETs with characteristics superior to any reported to date. These devices allow the investigation of the intrinsic FET and (gated) Hall-effect carrier mobilities as functions of temperature. The intrinsic mobility is found to increase on cooling from ≈30 cm2 V-1 s-1 at room temperature to ≈250 cm2 V-1 s-1 at 50 K, revealing a band transport limited by phonon scattering. Establishing the intrinsic (phonon-limited) mobility provides a solid test for theoretical descriptions of carrier transport in perovskites, reveals basic limits to the technology, and points to a path for future high-performance perovskite electronic devices.

Charge Density Wave Vortex Lattice Observed in Graphene-Passivated 1T-TaS2 by Ambient Scanning Tunneling Microscopy.

The nearly commensurate charge density wave (CDW) excitations native to the transition-metal dichalcogenide crystal, 1T-TaS2, under ambient conditions are revealed by scanning tunneling microscopy (STM) and spectroscopy (STS) measurements of a graphene/TaS2 heterostructure. Surface potential measurements show that the graphene passivation layer prevents oxidation of the air-sensitive 1T-TaS2 surface. The graphene protective layer does not however interfere with probing the native electronic properties of 1T-TaS2 by STM/STS, which revealed that nearly commensurate CDW hosts an array of vortex-like topological defects. We find that these topological defects organize themselves to form a lattice with quasi-long-range order, analogous to the vortex Bragg glass in type-II superconductors but accessible in ambient conditions.

Flat band carrier confinement in magic-angle twisted bilayer graphene.

Magic-angle twisted bilayer graphene has emerged as a powerful platform for studying strongly correlated electron physics, owing to its almost dispersionless low-energy bands and the ability to tune the band filling by electrostatic gating. Techniques to control the twist angle between graphene layers have led to rapid experimental progress but improving sample quality is essential for separating the delicate correlated electron physics from disorder effects. Owing to the 2D nature of the system and the relatively low carrier density, the samples are highly susceptible to small doping inhomogeneity which can drastically modify the local potential landscape. This potential disorder is distinct from the twist angle variation which has been studied elsewhere. Here, by using low temperature scanning tunneling spectroscopy and planar tunneling junction measurements, we demonstrate that flat bands in twisted bilayer graphene can amplify small doping inhomogeneity that surprisingly leads to carrier confinement, which in graphene could previously only be realized in the presence of a strong magnetic field.

Author Correction: Chern insulators, van Hove singularities and topological flat bands in magic-angle twisted bilayer graphene.

A Correction to this paper has been published: https://doi.org/10.1038/s41563-021-00997-2.

Chern insulators, van Hove singularities and topological flat bands in magic-angle twisted bilayer graphene.

Magic-angle twisted bilayer graphene exhibits intriguing quantum phase transitions triggered by enhanced electron-electron interactions when its flat bands are partially filled. However, the phases themselves and their connection to the putative non-trivial topology of the flat bands are largely unexplored. Here we report transport measurements revealing a succession of doping-induced Lifshitz transitions that are accompanied by van Hove singularities, which facilitate the emergence of correlation-induced gaps and topologically non-trivial subbands. In the presence of a magnetic field, well-quantized Hall plateaus at a filling of 1,2,3 carriers per moiré cell reveal the subband topology and signal the emergence of Chern insulators with Chern numbers, C = 3,2,1, respectively. Surprisingly, for magnetic fields exceeding 5 T we observe a van Hove singularity at a filling of 3.5, suggesting the possibility of a fractional Chern insulator. This van Hove singularity is accompanied by a crossover from low-temperature metallic, to high-temperature insulating behaviour, characteristic of entropically driven Pomeranchuk-like transitions.

Graphene bilayers with a twist.

Near a magic twist angle, bilayer graphene transforms from a weakly correlated Fermi liquid to a strongly correlated two-dimensional electron system with properties that are extraordinarily sensitive to carrier density and to controllable environmental factors such as the proximity of nearby gates and twist-angle variation. Among other phenomena, magic-angle twisted bilayer graphene hosts superconductivity, interaction-induced insulating states, magnetism, electronic nematicity, linear-in-temperature low-temperature resistivity and quantized anomalous Hall states. We highlight some key research results in this field, point to important questions that remain open and comment on the place of magic-angle twisted bilayer graphene in the strongly correlated quantum matter world.

Evidence of flat bands and correlated states in buckled graphene superlattices.

Two-dimensional atomic crystals can radically change their properties in response to external influences, such as substrate orientation or strain, forming materials with novel electronic structure1-5. An example is the creation of weakly dispersive, 'flat' bands in bilayer graphene for certain 'magic' angles of twist between the orientations of the two layers6. The quenched kinetic energy in these flat bands promotes electron-electron interactions and facilitates the emergence of strongly correlated phases, such as superconductivity and correlated insulators. However, the very accurate fine-tuning required to obtain the magic angle in twisted-bilayer graphene poses challenges to fabrication and scalability. Here we present an alternative route to creating flat bands that does not involve fine-tuning. Using scanning tunnelling microscopy and spectroscopy, together with numerical simulations, we demonstrate that graphene monolayers placed on an atomically flat substrate can be forced to undergo a buckling transition7-9, resulting in a periodically modulated pseudo-magnetic field10-14, which in turn creates a 'post-graphene' material with flat electronic bands. When we introduce the Fermi level into these flat bands using electrostatic doping, we observe a pseudogap-like depletion in the density of states, which signals the emergence of a correlated state15-17. This buckling of two-dimensional crystals offers a strategy for creating other superlattice systems and, in particular, for exploring interaction phenomena characteristic of flat bands.

Charge order and broken rotational symmetry in magic-angle twisted bilayer graphene.

Bilayer graphene can be modified by rotating (twisting) one layer with respect to the other. The interlayer twist gives rise to a moiré superlattice that affects the electronic motion and alters the band structure1-4. Near a 'magic angle' of twist2,4, where the emergence of a flat band causes the charge carriers to slow down3, correlated electronic phases including Mott-like insulators and superconductors were recently discovered5-8 by using electronic transport. These measurements revealed an intriguing similarity between magic-angle twisted bilayer graphene and high-temperature superconductors, which spurred intensive research into the underlying physical mechanism9-14. Essential clues to this puzzle, such as the symmetry and spatial distribution of the spectral function, can be accessed through scanning tunnelling spectroscopy. Here we use scanning tunnelling microscopy and spectroscopy to visualize the local density of states and charge distribution in magic-angle twisted bilayer graphene. Doping the sample to partially fill the flat band, we observe a pseudogap phase accompanied by a global stripe charge order that breaks the rotational symmetry of the moiré superlattice. Both the pseudogap and the stripe charge order disappear when the band is either empty or full. The close resemblance to similar observations in high-temperature superconductors15-21 provides new evidence of a deeper link underlying the phenomenology of these systems.

Inducing Kondo screening of vacancy magnetic moments in graphene with gating and local curvature.

In normal metals the magnetic moment of impurity-spins disappears below a characteristic Kondo temperature which marks the formation of a cloud of conduction-band electrons that screen the local-moment. In contrast, moments embedded in insulators remain unscreened at all temperatures. What then is the fate of magnetic-moments in intermediate, pseudogap systems, such as graphene? Theory predicts that coupling to the conduction-band electrons will drive a quantum phase transition between a local-moment phase and a Kondo-screened phase. However, attempts to experimentally confirm this prediction and its intriguing consequences, such as electrostatically tunable magnetic-moments, have been elusive. Here we report the observation of Kondo-screening and the quantum phase-transition between screened and unscreened phases of vacancy magnetic moments in graphene. Using scanning tunneling spectroscopy and numerical renormalization-group calculations we show that this transition enables to control the screening of local moments by tuning the gate voltage and the local curvature of the graphene membrane.

Tuning a circular p-n junction in graphene from quantum confinement to optical guiding.

The photon-like propagation of the Dirac electrons in graphene, together with its record-high electronic mobility, can lead to applications based on ultrafast electronic response and low dissipation. However, the chiral nature of the charge carriers that is responsible for the high mobility also makes it difficult to control their motion and prevents electronic switching. Here, we show how to manipulate the charge carriers by using a circular p-n junction whose size can be continuously tuned from the nanometre to the micrometre scale. The junction size is controlled with a dual-gate device consisting of a planar back gate and a point-like top gate made by decorating a scanning tunnelling microscope tip with a gold nanowire. The nanometre-scale junction is defined by a deep potential well created by the tip-induced charge. It traps the Dirac electrons in quantum-confined states, which are the graphene equivalent of the atomic collapse states (ACSs) predicted to occur at supercritically charged nuclei. As the junction size increases, the transition to the optical regime is signalled by the emergence of whispering-gallery modes, similar to those observed at the perimeter of acoustic or optical resonators, and by the appearance of a Fabry-Pérot interference pattern for junctions close to a boundary.

Visualizing Strain-Induced Pseudomagnetic Fields in Graphene through an hBN Magnifying Glass.

Graphene's remarkable properties are inherent to its two-dimensional honeycomb lattice structure. Its low dimensionality, which makes it possible to rearrange the atoms by applying an external force, offers the intriguing prospect of mechanically controlling the electronic properties. In the presence of strain, graphene develops a pseudomagnetic field (PMF) that reconstructs the band structure into pseudo Landau levels (PLLs). However, a feasible route to realizing, characterizing and controlling PMFs is still lacking. Here we report on a method to generate and characterize PMFs in a graphene membrane supported on nanopillars. A direct measure of the local strain is achieved by using the magnifying effect of the moiré pattern formed against a hexagonal boron nitride substrate under scanning tunneling microscopy. We quantify the strain-induced PMF through the PLLs spectra observed in scanning tunneling spectroscopy. This work provides a pathway to strain induced engineering and electro-mechanical graphene-based devices.

High thermoelectricpower factor in graphene/hBN devices.

Fast and controllable cooling at nanoscales requires a combination of highly efficient passive cooling and active cooling. Although passive cooling in graphene-based devices is quite effective due to graphene's extraordinary heat conduction, active cooling has not been considered feasible due to graphene's low thermoelectric power factor. Here, we show that the thermoelectric performance of graphene can be significantly improved by using hexagonal boron nitride (hBN) substrates instead of SiO2 We find the room temperature efficiency of active cooling in the device, as gauged by the power factor times temperature, reaches values as high as 10.35 W⋅m-1⋅K-1, corresponding to more than doubling the highest reported room temperature bulk power factors, 5 W⋅m-1⋅K-1, in YbAl3, and quadrupling the best 2D power factor, 2.5 W⋅m-1⋅K-1, in MoS2 We further show that the Seebeck coefficient provides a direct measure of substrate-induced random potential fluctuations and that their significant reduction for hBN substrates enables fast gate-controlled switching of the Seebeck coefficient polarity for applications in integrated active cooling devices.

Nanoscale Internal Fields in a Biased Graphene-Insulator-Semiconductor Structure.

Measuring and understanding electric fields in multilayered materials at the nanoscale remains a challenging problem impeding the development of novel devices. At this scale, it is far from obvious that materials can be accurately described by their intrinsic bulk properties, and considerations of the interfaces between layered materials become unavoidable for a complete description of the system's electronic properties. Here, a general approach to the direct measurement of nanoscale internal fields is proposed. Small spot X-ray photoemission was performed on a biased graphene/SiO2/Si structure in order to experimentally determine the potential profile across the system, including discontinuities at the interfaces. Core levels provide a measure of the local potential and are used to reconstruct the potential profile as a function of the depth through the stack. It is found that each interface plays a critical role in establishing the potential across the dielectric, and the origin of the potential discontinuities at each interface is discussed.

Local, global, and nonlinear screening in twisted double-layer graphene.

One-atom-thick crystalline layers and their vertical heterostructures carry the promise of designer electronic materials that are unattainable by standard growth techniques. To realize their potential it is necessary to isolate them from environmental disturbances, in particular those introduced by the substrate. However, finding and characterizing suitable substrates, and minimizing the random potential fluctuations they introduce, has been a persistent challenge in this emerging field. Here we show that Landau-level (LL) spectroscopy offers the unique capability to quantify both the reduction of the quasiparticles' lifetime and the long-range inhomogeneity due to random potential fluctuations. Harnessing this technique together with direct scanning tunneling microscopy and numerical simulations we demonstrate that the insertion of a graphene buffer layer with a large twist angle is a very effective method to shield a 2D system from substrate interference that has the additional desirable property of preserving the electronic structure of the system under study. We further show that owing to its remarkable nonlinear screening capability a single graphene buffer layer provides better shielding than either increasing the distance to the substrate or doubling the carrier density and reduces the amplitude of the potential fluctuations in graphene to values even lower than the ones in AB-stacked bilayer graphene.

MoS 2 MoS2: choice substrate for accessing and tuning the electronic properties of graphene.

One of the enduring challenges in graphene research and applications is the extreme sensitivity of its charge carriers to external perturbations, especially those introduced by the substrate. The best available substrates to date, graphite and hexagonal boron nitride (h-BN), still pose limitations: graphite being metallic does not allow gating, while both h-BN and graphite, having lattice structures closely matched to that of graphene, may cause significant band structure reconstruction. Here we show that the atomically smooth surface of exfoliated MoS(2) provides access to the intrinsic electronic structure of graphene without these drawbacks. Using scanning tunneling microscopy and Landau-level (LL) spectroscopy in a device configuration that allows tuning of the carrier concentration, we find that graphene on MoS(2) is ultraflat, producing long mean free paths, while avoiding band structure reconstruction. Importantly, the screening of the MoS(2) substrate can be tuned by changing the position of the Fermi energy with relatively low gate voltages. We show that shifting the Fermi energy from the gap to the edge of the conduction band gives rise to enhanced screening and to a substantial increase in the mean free path and quasiparticle lifetime. MoS(2) substrates thus provide unique opportunities to access the intrinsic electronic properties of graphene and to study in situ the effects of screening on electron-electron interactions and transport.

Bandgap, mid-gap states, and gating effects in MoS2.

The discovery of graphene has put the spotlight on other layered materials including transition metal dichalcogenites (TMD) as building blocks for novel heterostructures assembled from stacked atomic layers. Molybdenum disulfide, MoS2, a semiconductor in the TMD family, with its remarkable thermal and chemical stability and high mobility, has emerged as a promising candidate for postsilicon applications such as switching, photonics, and flexible electronics. Because these rely on controlling the position of the Fermi energy (EF), it is crucial to understand its dependence on doping and gating. To elucidate these questions we carried out gated scanning tunneling microscopy (STM) and spectroscopy (STS) measurements and compared them with transport measurements in a field effect transistor (FET) device configuration. This made it possible to measure the bandgap and the position of EF in MoS2 and to track its evolution with gate voltage. For bulk samples, the measured bandgap (∼ 1.3 eV) is comparable to the value obtained by photoluminescence, and the position of EF (∼ 0.35 eV) below the conduction band, is consistent with N-doping reported in this material. We show that the N-doping in bulk samples can be attributed to S vacancies. In contrast, the significantly higher N-doping observed in thin MoS2 films deposited on SiO2 is dominated by charge traps at the sample-substrate interface.