Visualizing moiré ferroelectricity via plasmons and nano-photocurrent in graphene/twisted-WSe2 structures.

Ferroelectricity, a spontaneous and reversible electric polarization, is found in certain classes of van der Waals (vdW) materials. The discovery of ferroelectricity in twisted vdW layers provides new opportunities to engineer spatially dependent electric and optical properties associated with the configuration of moiré superlattice domains and the network of domain walls. Here, we employ near-field infrared nano-imaging and nano-photocurrent measurements to study ferroelectricity in minimally twisted WSe2. The ferroelectric domains are visualized through the imaging of the plasmonic response in a graphene monolayer adjacent to the moiré WSe2 bilayers. Specifically, we find that the ferroelectric polarization in moiré domains is imprinted on the plasmonic response of the graphene. Complementary nano-photocurrent measurements demonstrate that the optoelectronic properties of graphene are also modulated by the proximal ferroelectric domains. Our approach represents an alternative strategy for studying moiré ferroelectricity at native length scales and opens promising prospects for (opto)electronic devices.

Infrared nano-imaging of Dirac magnetoexcitons in graphene.

Magnetic fields can have profound effects on the motion of electrons in quantum materials. Two-dimensional electron systems subject to strong magnetic fields are expected to exhibit quantized Hall conductivity, chiral edge currents and distinctive collective modes referred to as magnetoplasmons and magnetoexcitons. Generating these propagating collective modes in charge-neutral samples and imaging them at their native nanometre length scales have thus far been experimentally elusive. Here we visualize propagating magnetoexciton polaritons at their native length scales and report their magnetic-field-tunable dispersion in near-charge-neutral graphene. Imaging these collective modes and their associated nano-electro-optical responses allows us to identify polariton-modulated optical and photo-thermal electric effects at the sample edges, which are the most pronounced near charge neutrality. Our work is enabled by innovations in cryogenic near-field optical microscopy techniques that allow for the nano-imaging of the near-field responses of two-dimensional materials under magnetic fields up to 7 T. This nano-magneto-optics approach allows us to explore and manipulate magnetopolaritons in specimens with low carrier doping via harnessing high magnetic fields.

Domain-Dependent Surface Adhesion in Twisted Few-Layer Graphene: Platform for Moiré-Assisted Chemistry.

Twisted van der Waals multilayers are widely regarded as a rich platform to access novel electronic phases thanks to the multiple degrees of freedom available for controlling 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 trilayer graphene. Furthermore, we demonstrate that the manipulation of nanoparticles located at certain stacking domains can locally reconfigure the moiré superlattice in their vicinity at the micrometer scale. Our findings establish a new approach to controlling moiré-assisted chemistry and nanoengineering.

Unconventional non-local relaxation dynamics in a twisted trilayer graphene moiré superlattice.

The electronic and structural properties of atomically thin materials can be controllably tuned by assembling them with an interlayer twist. During this process, constituent layers spontaneously rearrange themselves in search of a lowest energy configuration. Such relaxation phenomena can lead to unexpected and novel material properties. Here, we study twisted double trilayer graphene (TDTG) using nano-optical and tunneling spectroscopy tools. We reveal a surprising optical and electronic contrast, as well as a stacking energy imbalance emerging between the moiré domains. We attribute this contrast to an unconventional form of lattice relaxation in which an entire graphene layer spontaneously shifts position during assembly, resulting in domains of ABABAB and BCBACA stacking. We analyze the energetics of this transition and demonstrate that it is the result of a non-local relaxation process, in which an energy gain in one domain of the moiré lattice is paid for by a relaxation that occurs in the other.

Extracting the Strain Matrix and Twist Angle from the Moiré Superlattice in van der Waals Heterostructures.

When two atomic layers are brought into contact at a relative twist angle, a large-scale pattern, called a moiré superlattice, emerges due to the (angular or lattice) mismatch between the layers. This has profound consequences in terms of the Hamiltonian of the system but was also considered in several publications as a means to extract the local strain tensor. While extracting the twist angle based on knowledge of the periodicity of the moiré is trivial in the case of a regular moiré pattern, in many examples in the literature, that is not the case. In particular, extracting the strain tensor and twist angle maps from a spatially varying moiré pattern is not straightforward. This article aims to provide a practical tool to extract the strain tensor and twist angle from an experimentally observable pattern. It further addresses the limitation of any such approach in the absence of additional experimental information beyond the moiré superlattice pattern.

Nonlinear nanoelectrodynamics of a Weyl metal.

Chiral Weyl fermions with linear energy-momentum dispersion in the bulk accompanied by Fermi-arc states on the surfaces prompt a host of enticing optical effects. While new Weyl semimetal materials keep emerging, the available optical probes are limited. In particular, isolating bulk and surface electrodynamics in Weyl conductors remains a challenge. We devised an approach to the problem based on near-field photocurrent imaging at the nanoscale and applied this technique to a prototypical Weyl semimetal TaIrTe4 As a first step, we visualized nano-photocurrent patterns in real space and demonstrated their connection to bulk nonlinear conductivity tensors through extensive modeling augmented with density functional theory calculations. Notably, our nanoscale probe gives access to not only the in-plane but also the out-of-plane electric fields so that it is feasible to interrogate all allowed nonlinear tensors including those that remained dormant in conventional far-field optics. Surface- and bulk-related nonlinear contributions are distinguished through their "symmetry fingerprints" in the photocurrent maps. Robust photocurrents also appear at mirror-symmetry breaking edges of TaIrTe4 single crystals that we assign to nonlinear conductivity tensors forbidden in the bulk. Nano-photocurrent spectroscopy at the boundary reveals a strong resonance structure absent in the interior of the sample, providing evidence for elusive surface states.

Polaritonic Vortices with a Half-Integer Charge.

Topological spin textures are field arrangements that cannot be continuously deformed to a fully polarized state. In particular, merons are topological textures characterized by half-integer topological charge ±1/2 and vortex-like swirling patterns at large distances. Merons have been studied previously in the context of cosmology, fluid dynamics, condensed matter physics and plasmonics. Here, we visualized optical spin angular momentum of phonon polaritons that resembles nanoscale meron spin textures. Phonon polaritons, hybrids of infrared photons and phonons in hexagonal boron nitride, were excited by circularly polarized light incident on a ring-shaped antenna and imaged using infrared near-field techniques. The polariton field reveals a half-integer topological charge determined by the handedness of the incident beam. Our phonon polaritonic platform opens up new pathways to create, control, and visualize topological textures.

Enhanced tunable second harmonic generation from twistable interfaces and vertical superlattices in boron nitride homostructures.

Broken symmetries induce strong even-order nonlinear optical responses in materials and at interfaces. Unlike conventional covalently bonded nonlinear crystals, van der Waals (vdW) heterostructures feature layers that can be stacked at arbitrary angles, giving complete control over the presence or lack of inversion symmetry at a crystal interface. Here, we report highly tunable second harmonic generation (SHG) from nanomechanically rotatable stacks of bulk hexagonal boron nitride (BN) crystals and introduce the term twistoptics to describe studies of optical properties in twistable vdW systems. By suppressing residual bulk effects, we observe SHG intensity modulated by a factor of more than 50, and polarization patterns determined by moiré interface symmetry. Last, we demonstrate greatly enhanced conversion efficiency in vdW vertical superlattice structures with multiple symmetry-broken interfaces. Our study paves the way for compact twistoptics architectures aimed at efficient tunable frequency conversion and demonstrates SHG as a robust probe of buried vdW interfaces.

Dual-Gated Graphene Devices for Near-Field Nano-imaging.

Graphene-based heterostructures display a variety of phenomena that are strongly tunable by electrostatic local gates. Monolayer graphene (MLG) exhibits tunable surface plasmon polaritons, as revealed by scanning nano-infrared experiments. In bilayer graphene (BLG), an electronic gap is induced by a perpendicular displacement field. Gapped BLG is predicted to display unusual effects such as plasmon amplification and domain wall plasmons with significantly larger lifetime than MLG. Furthermore, a variety of correlated electronic phases highly sensitive to displacement fields have been observed in twisted graphene structures. However, applying perpendicular displacement fields in nano-infrared experiments has only recently become possible [Li, H.; Nano Lett. 2020, 20, 3106-3112]. In this work, we fully characterize two approaches to realizing nano-optics compatible top gates: bilayer MoS2 and MLG. We perform nano-infrared imaging on both types of structures and evaluate their strengths and weaknesses. Our work paves the way for comprehensive near-field experiments of correlated phenomena and plasmonic effects in graphene-based heterostructures.

Moiré metrology of energy landscapes in van der Waals heterostructures.

The emerging field of twistronics, which harnesses the twist angle between two-dimensional materials, represents a promising route for the design of quantum materials, as the twist-angle-induced superlattices offer means to control topology and strong correlations. At the small twist limit, and particularly under strain, as atomic relaxation prevails, the emergent moiré superlattice encodes elusive insights into the local interlayer interaction. Here we introduce moiré metrology as a combined experiment-theory framework to probe the stacking energy landscape of bilayer structures at the 0.1 meV/atom scale, outperforming the gold-standard of quantum chemistry. Through studying the shapes of moiré domains with numerous nano-imaging techniques, and correlating with multi-scale modelling, we assess and refine first-principle models for the interlayer interaction. We document the prowess of moiré metrology for three representative twisted systems: bilayer graphene, double bilayer graphene and H-stacked MoSe2/WSe2. Moiré metrology establishes sought after experimental benchmarks for interlayer interaction, thus enabling accurate modelling of twisted multilayers.

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.

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

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

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.

Nano-photocurrent Mapping of Local Electronic Structure in Twisted Bilayer Graphene.

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

Imaging resonant dissipation from individual atomic defects in graphene.

Conversion of electric current into heat involves microscopic processes that operate on nanometer length scales and release minute amounts of power. Although central to our understanding of the electrical properties of materials, individual mediators of energy dissipation have so far eluded direct observation. Using scanning nanothermometry with submicrokelvin sensitivity, we visualized and controlled phonon emission from individual atomic-scale defects in graphene. The inferred electron-phonon "cooling power spectrum" exhibits sharp peaks when the Fermi level comes into resonance with electronic quasi-bound states at such defects. Rare in the bulk but abundant at graphene's edges, switchable atomic-scale phonon emitters provide the dominant dissipation mechanism. Our work offers insights for addressing key materials challenges in modern electronics and enables control of dissipation at the nanoscale.

Electrically Tunable Multiterminal SQUID-on-Tip.

We present a new nanoscale superconducting quantum interference device (SQUID) whose interference pattern can be shifted electrically in situ. The device consists of a nanoscale four-terminal-four-junction SQUID fabricated at the apex of a sharp pipet using a self-aligned three-step deposition of Pb. In contrast to conventional two-terminal-two-junction SQUIDs that display optimal sensitivity when flux biased to about a quarter of the flux quantum, the additional terminals and junctions allow optimal sensitivity at arbitrary applied flux, thus eliminating the magnetic field "blind spots". We demonstrate spin sensitivity of 5 to 8 µB/Hz1/2 over a continuous field range of 0 to 0.5 T with promising applications for nanoscale scanning magnetic imaging.

Three-junction SQUID-on-tip with tunable in-plane and out-of-plane magnetic field sensitivity.

Nanoscale superconducting quantum interference devices (SQUIDs) demonstrate record sensitivities to small magnetic moments but are typically sensitive only to the field component that is normal to the plane of the SQUID and out-of-plane with respect to the scanned surface. We report on a nanoscale three-junction Pb SQUID, which is fabricated on the apex of a sharp tip. Because of its three-dimensional structure, it exhibits a unique tunable sensitivity to both in-plane and out-of-plane fields. We analyze the two-dimensional interference pattern from both numerical and experimental points of view. This device is integrated into a scanning microscope, and its ability to independently measure the different components of the magnetic field with outstanding spin sensitivity better than 5 µB/Hz(1/2) is demonstrated. This highlights its potential as a local probe of nanoscale magnetic structures.

A scanning superconducting quantum interference device with single electron spin sensitivity.

Superconducting quantum interference devices (SQUIDs) can be used to detect weak magnetic fields and have traditionally been the most sensitive magnetometers available. However, because of their relatively large effective size (on the order of 1 µm), the devices have so far been unable to achieve the level of sensitivity required to detect the field generated by the spin magnetic moment (µB) of a single electron. Here we show that nanoscale SQUIDs with diameters as small as 46 nm can be fabricated on the apex of a sharp tip. The nano-SQUIDs have an extremely low flux noise of 50 nΦ0 Hz(-1/2) and a spin sensitivity of down to 0.38 µB Hz(-1/2), which is almost two orders of magnitude better than previous devices. They can also operate over a wide range of magnetic fields, providing a sensitivity of 0.6 µB Hz(-1/2) at 1 T. The unique geometry of our nano-SQUIDs makes them well suited to scanning probe microscopy, and we use the devices to image vortices in a type II superconductor, spaced 120 nm apart, and to record magnetic fields due to alternating currents down to 50 nT.