Electrical switching of a bistable moiré superconductor.

Electrical control of superconductivity is critical for nanoscale superconducting circuits including cryogenic memory elements1-4, superconducting field-effect transistors (FETs)5-7 and gate-tunable qubits8-10. Superconducting FETs operate through continuous tuning of carrier density, but no bistable superconducting FET, which could serve as a new type of cryogenic memory element, has been reported. Recently, gate hysteresis and resultant bistability in Bernal-stacked bilayer graphene aligned to its insulating hexagonal boron nitride gate dielectrics were discovered11,12. Here we report the observation of this same hysteresis in magic-angle twisted bilayer graphene (MATBG) with aligned boron nitride layers. This bistable behaviour coexists alongside the strongly correlated electron system of MATBG without disrupting its correlated insulator or superconducting states. This all-van der Waals platform enables configurable switching between different electronic states of this rich system. To illustrate this new approach, we demonstrate reproducible bistable switching between the superconducting, metallic and correlated insulator states of MATBG using gate voltage or electric displacement field. These experiments unlock the potential to broadly incorporate this new switchable moiré superconductor into highly tunable superconducting electronics.

Robust superconductivity in magic-angle multilayer graphene family.

The discovery of correlated states and superconductivity in magic-angle twisted bilayer graphene (MATBG) established a new platform to explore interaction-driven and topological phenomena. However, despite multitudes of correlated phases observed in moiré systems, robust superconductivity appears the least common, found only in MATBG and more recently in magic-angle twisted trilayer graphene. Here we report the experimental realization of superconducting magic-angle twisted four-layer and five-layer graphene, hence establishing alternating twist magic-angle multilayer graphene as a robust family of moiré superconductors. This finding suggests that the flat bands shared by the members play a central role in the superconductivity. Our measurements in parallel magnetic fields, in particular the investigation of Pauli limit violation and spontaneous rotational symmetry breaking, reveal a clear distinction between the N = 2 and N > 2-layer structures, consistent with the difference between their orbital responses to magnetic fields. Our results expand the emergent family of moiré superconductors, providing new insight with potential implications for design of new superconducting materials platforms.

Unconventional Hysteretic Transition in a Charge Density Wave.

Hysteresis underlies a large number of phase transitions in solids, giving rise to exotic metastable states that are otherwise inaccessible. Here, we report an unconventional hysteretic transition in a quasi-2D material, EuTe_{4}. By combining transport, photoemission, diffraction, and x-ray absorption measurements, we observe that the hysteresis loop has a temperature width of more than 400 K, setting a record among crystalline solids. The transition has an origin distinct from known mechanisms, lying entirely within the incommensurate charge density wave (CDW) phase of EuTe_{4} with no change in the CDW modulation periodicity. We interpret the hysteresis as an unusual switching of the relative CDW phases in different layers, a phenomenon unique to quasi-2D compounds that is not present in either purely 2D or strongly coupled 3D systems. Our findings challenge the established theories on metastable states in density wave systems, pushing the boundary of understanding hysteretic transitions in a broken-symmetry state.

Hexagonal boron nitride as a low-loss dielectric for superconducting quantum circuits and qubits.

Dielectrics with low loss at microwave frequencies are imperative for high-coherence solid-state quantum computing platforms. Here we study the dielectric loss of hexagonal boron nitride (hBN) thin films in the microwave regime by measuring the quality factor of parallel-plate capacitors (PPCs) made of NbSe2-hBN-NbSe2 heterostructures integrated into superconducting circuits. The extracted microwave loss tangent of hBN is bounded to be at most in the mid-10-6 range in the low-temperature, single-photon regime. We integrate hBN PPCs with aluminium Josephson junctions to realize transmon qubits with coherence times reaching 25 µs, consistent with the hBN loss tangent inferred from resonator measurements. The hBN PPC reduces the qubit feature size by approximately two orders of magnitude compared with conventional all-aluminium coplanar transmons. Our results establish hBN as a promising dielectric for building high-coherence quantum circuits with substantially reduced footprint and with a high energy participation that helps to reduce unwanted qubit cross-talk.

Interfacial ferroelectricity in rhombohedral-stacked bilayer transition metal dichalcogenides.

van der Waals materials have greatly expanded our design space of heterostructures by allowing individual layers to be stacked at non-equilibrium configurations, for example via control of the twist angle. Such heterostructures not only combine characteristics of the individual building blocks, but can also exhibit physical properties absent in the parent compounds through interlayer interactions1. Here we report on a new family of nanometre-thick, two-dimensional (2D) ferroelectric semiconductors, where the individual constituents are well-studied non-ferroelectric monolayer transition metal dichalcogenides (TMDs), namely WSe2, MoSe2, WS2 and MoS2. By stacking two identical monolayer TMDs in parallel, we obtain electrically switchable rhombohedral-stacking configurations, with out-of-plane polarization that is flipped by in-plane sliding motion. Fabricating nearly parallel-stacked bilayers enables the visualization of moiré ferroelectric domains as well as electric field-induced domain wall motion with piezoelectric force microscopy. Furthermore, by using a nearby graphene electronic sensor in a ferroelectric field transistor geometry, we quantify the ferroelectric built-in interlayer potential, in good agreement with first-principles calculations. The new semiconducting ferroelectric properties of these four new TMDs opens up the possibility of studying the interplay between ferroelectricity and their rich electric and optical properties2-5.

Active and Passive Tuning of Ultranarrow Resonances in Polaritonic Nanoantennas.

Optical nanoantennas are of great importance for photonic devices and spectroscopy due to their capability of squeezing light at the nanoscale and enhancing light-matter interactions. Among them, nanoantennas made of polar crystals supporting phonon polaritons (phononic nanoantennas) exhibit the highest quality factors. This is due to the low optical losses inherent in these materials, which, however, hinder the spectral tuning of the nanoantennas due to their dielectric nature. Here, active and passive tuning of ultranarrow resonances in phononic nanoantennas is realized over a wide spectral range (≈35 cm-1 , being the resonance linewidth ≈9 cm-1 ), monitored by near-field nanoscopy. To do that, the local environment of a single nanoantenna made of hexagonal boron nitride is modified by placing it on different polar substrates, such as quartz and 4H-silicon carbide, or covering it with layers of a high-refractive-index van der Waals crystal (WSe2 ). Importantly, active tuning of the nanoantenna polaritonic resonances is demonstrated by placing it on top of a gated graphene monolayer in which the Fermi energy is varied. This work presents the realization of tunable polaritonic nanoantennas with ultranarrow resonances, which can find applications in active nanooptics and (bio)sensing.

Role of Equilibrium Fluctuations in Light-Induced Order.

Engineering novel states of matter with light is at the forefront of materials research. An intensely studied direction is to realize broken-symmetry phases that are "hidden" under equilibrium conditions but can be unleashed by an ultrashort laser pulse. Despite a plethora of experimental discoveries, the nature of these orders and how they transiently appear remain unclear. To this end, we investigate a nonequilibrium charge density wave (CDW) in rare-earth tritellurides, which is suppressed in equilibrium but emerges after photoexcitation. Using a pump-pump-probe protocol implemented in ultrafast electron diffraction, we demonstrate that the light-induced CDW consists solely of order parameter fluctuations, which bear striking similarities to critical fluctuations in equilibrium despite differences in the length scale. By calculating the dynamics of CDW fluctuations in a nonperturbative model, we further show that the strength of the light-induced order is governed by the amplitude of equilibrium fluctuations. These findings highlight photoinduced fluctuations as an important ingredient for the emergence of transient orders out of equilibrium. Our results further suggest that materials with strong fluctuations in equilibrium are promising platforms to host hidden orders after laser excitation.

Fractional Chern insulators in magic-angle twisted bilayer graphene.

Fractional Chern insulators (FCIs) are lattice analogues of fractional quantum Hall states that may provide a new avenue towards manipulating non-Abelian excitations. Early theoretical studies1-7 have predicted their existence in systems with flat Chern bands and highlighted the critical role of a particular quantum geometry. However, FCI states have been observed only in Bernal-stacked bilayer graphene (BLG) aligned with hexagonal boron nitride (hBN)8, in which a very large magnetic field is responsible for the existence of the Chern bands, precluding the realization of FCIs at zero field. By contrast, magic-angle twisted BLG9-12 supports flat Chern bands at zero magnetic field13-17, and therefore offers a promising route towards stabilizing zero-field FCIs. Here we report the observation of eight FCI states at low magnetic field in magic-angle twisted BLG enabled by high-resolution local compressibility measurements. The first of these states emerge at 5 T, and their appearance is accompanied by the simultaneous disappearance of nearby topologically trivial charge density wave states. We demonstrate that, unlike the case of the BLG/hBN platform, the principal role of the weak magnetic field is merely to redistribute the Berry curvature of the native Chern bands and thereby realize a quantum geometry favourable for the emergence of FCIs. Our findings strongly suggest that FCIs may be realized at zero magnetic field and pave the way for the exploration and manipulation of anyonic excitations in flat moiré Chern bands.

Pauli-limit violation and re-entrant superconductivity in moiré graphene.

Moiré quantum matter has emerged as a materials platform in which correlated and topological phases can be explored with unprecedented control. Among them, magic-angle systems constructed from two or three layers of graphene have shown robust superconducting phases with unconventional characteristics1-5. However, direct evidence of unconventional pairing remains to be experimentally demonstrated. Here we show that magic-angle twisted trilayer graphene exhibits superconductivity up to in-plane magnetic fields in excess of 10 T, which represents a large (2-3 times) violation of the Pauli limit for conventional spin-singlet superconductors6,7. This is an unexpected observation for a system that is not predicted to have strong spin-orbit coupling. The Pauli-limit violation is observed over the entire superconducting phase, which indicates that it is not related to a possible pseudogap phase with large superconducting amplitude pairing. Notably, we observe re-entrant superconductivity at large magnetic fields, which is present over a narrower range of carrier densities and displacement fields. These findings suggest that the superconductivity in magic-angle twisted trilayer graphene is likely to be driven by a mechanism that results in non-spin-singlet Cooper pairs, and that the external magnetic field can cause transitions between phases with potentially different order parameters. Our results demonstrate the richness of moiré superconductivity and could lead to the design of next-generation exotic quantum matter.

Stacking-engineered ferroelectricity in bilayer boron nitride.

2D ferroelectrics with robust polarization down to atomic thicknesses provide building blocks for functional heterostructures. Experimental realization remains challenging because of the requirement of a layered polar crystal. Here, we demonstrate a rational design approach to engineering 2D ferroelectrics from a non-ferroelectric parent compound via employing van der Waals assembly. Parallel-stacked bilayer boron nitride exhibits out-of-plane electric polarization that reverses depending on the stacking order. The polarization switching is probed via the resistance of an adjacently stacked graphene sheet. Twisting the boron nitride sheets by a small angle changes the dynamics of switching thanks to the formation of moiré ferroelectricity with staggered polarization. The ferroelectricity persists to room temperature while keeping the high mobility of graphene, paving the way for potential ultrathin nonvolatile memory applications.

Highly tunable junctions and non-local Josephson effect in magic-angle graphene tunnelling devices.

Magic-angle twisted bilayer graphene (MATBG) has recently emerged as a highly tunable two-dimensional material platform exhibiting a wide range of phases, such as metal, insulator and superconductor states. Local electrostatic control over these phases may enable the creation of versatile quantum devices that were previously not achievable in other single-material platforms. Here we engineer Josephson junctions and tunnelling transistors in MATBG, solely defined by electrostatic gates. Our multi-gated device geometry offers independent control of the weak link, barriers and tunnelling electrodes. These purely two-dimensional MATBG Josephson junctions exhibit non-local electrodynamics in a magnetic field, in agreement with the Pearl theory for ultrathin superconductors. Utilizing the intrinsic bandgaps of MATBG, we also demonstrate monolithic edge tunnelling spectroscopy within the same MATBG devices and measure the energy spectrum of MATBG in the superconducting phase. Furthermore, by inducing a double-barrier geometry, the devices can be operated as a single-electron transistor, exhibiting Coulomb blockade. With versatile functionality encompassed within a single material, these MATBG tunnelling devices may find applications in graphene-based tunable superconducting qubits, on-chip superconducting circuits and electromagnetic sensing.

Nematicity and competing orders in superconducting magic-angle graphene.

Strongly interacting electrons in solid-state systems often display multiple broken symmetries in the ground state. The interplay between different order parameters can give rise to a rich phase diagram. We report on the identification of intertwined phases with broken rotational symmetry in magic-angle twisted bilayer graphene (TBG). Using transverse resistance measurements, we find a strongly anisotropic phase located in a "wedge" above the underdoped region of the superconducting dome. Upon its crossing with the superconducting dome, a reduction of the critical temperature is observed. Furthermore, the superconducting state exhibits an anisotropic response to a direction-dependent in-plane magnetic field, revealing nematic ordering across the entire superconducting dome. These results indicate that nematic fluctuations might play an important role in the low-temperature phases of magic-angle TBG.

Flavour Hund's coupling, Chern gaps and charge diffusivity in moiré graphene.

Interaction-driven spontaneous symmetry breaking lies at the heart of many quantum phases of matter. In moiré systems, broken spin/valley 'flavour' symmetry in flat bands underlies the parent state from which correlated and topological ground states ultimately emerge1-10. However, the microscopic mechanism of such flavour symmetry breaking and its connection to the low-temperature phases are not yet understood. Here we investigate the broken-symmetry many-body ground state of magic-angle twisted bilayer graphene (MATBG) and its nontrivial topology using simultaneous thermodynamic and transport measurements. We directly observe flavour symmetry breaking as pinning of the chemical potential at all integer fillings of the moiré superlattice, demonstrating the importance of flavour Hund's coupling in the many-body ground state. The topological nature of the underlying flat bands is manifested upon breaking time-reversal symmetry, where we measure energy gaps corresponding to Chern insulator states with Chern numbers 3, 2, 1 at filling factors 1, 2, 3, respectively, consistent with flavour symmetry breaking in the Hofstadter butterfly spectrum of MATBG. Moreover, concurrent measurements of resistivity and chemical potential provide the temperature-dependent charge diffusivity of MATBG in the strange-metal regime11-a quantity previously explored only in ultracold atoms12. Our results bring us one step closer to a unified framework for understanding interactions in the topological bands of MATBG, with and without a magnetic field.

Entropic evidence for a Pomeranchuk effect in magic-angle graphene.

In the 1950s, Pomeranchuk1 predicted that, counterintuitively, liquid 3He may solidify on heating. This effect arises owing to high excess nuclear spin entropy in the solid phase, where the atoms are spatially localized. Here we find that an analogous effect occurs in magic-angle twisted bilayer graphene2-6. Using both local and global electronic entropy measurements, we show that near a filling of one electron per moiré unit cell, there is a marked increase in the electronic entropy to about 1kB per unit cell (kB is the Boltzmann constant). This large excess entropy is quenched by an in-plane magnetic field, pointing to its magnetic origin. A sharp drop in the compressibility as a function of the electron density, associated with a reset of the Fermi level back to the vicinity of the Dirac point, marks a clear boundary between two phases. We map this jump as a function of electron density, temperature and magnetic field. This reveals a phase diagram that is consistent with a Pomeranchuk-like temperature- and field-driven transition from a low-entropy electronic liquid to a high-entropy correlated state with nearly free magnetic moments. The correlated state features an unusual combination of seemingly contradictory properties, some associated with itinerant electrons-such as the absence of a thermodynamic gap, metallicity and a Dirac-like compressibility-and others associated with localized moments, such as a large entropy and its disappearance under a magnetic field. Moreover, the energy scales characterizing these two sets of properties are very different: whereas the compressibility jump has an onset at a temperature of about 30 kelvin, the bandwidth of magnetic excitations is about 3 kelvin or smaller. The hybrid nature of the present correlated state and the large separation of energy scales have implications for the thermodynamic and transport properties of the correlated states in twisted bilayer graphene.

Tunable strongly coupled superconductivity in magic-angle twisted trilayer graphene.

Moiré superlattices1,2 have recently emerged as a platform upon which correlated physics and superconductivity can be studied with unprecedented tunability3-6. Although correlated effects have been observed in several other moiré systems7-17, magic-angle twisted bilayer graphene remains the only one in which robust superconductivity has been reproducibly measured4-6. Here we realize a moiré superconductor in magic-angle twisted trilayer graphene (MATTG)18, which has better tunability of its electronic structure and superconducting properties than magic-angle twisted bilayer graphene. Measurements of the Hall effect and quantum oscillations as a function of density and electric field enable us to determine the tunable phase boundaries of the system in the normal metallic state. Zero-magnetic-field resistivity measurements reveal that the existence of superconductivity is intimately connected to the broken-symmetry phase that emerges from two carriers per moiré unit cell. We find that the superconducting phase is suppressed and bounded at the Van Hove singularities that partially surround the broken-symmetry phase, which is difficult to reconcile with weak-coupling Bardeen-Cooper-Schrieffer theory. Moreover, the extensive in situ tunability of our system allows us to reach the ultrastrong-coupling regime, characterized by a Ginzburg-Landau coherence length that reaches the average inter-particle distance, and very large TBKT/TF values, in excess of 0.1 (where TBKT and TF are the Berezinskii-Kosterlitz-Thouless transition and Fermi temperatures, respectively). These observations suggest that MATTG can be electrically tuned close to the crossover to a two-dimensional Bose-Einstein condensate. Our results establish a family of tunable moiré superconductors that have the potential to revolutionize our fundamental understanding of and the applications for strongly coupled superconductivity.

A versatile sample fabrication method for ultrafast electron diffraction.

Integral to the exploration of nonequilibrium phenomena in solid-state systems is the study of lattice motion after photoexcitation by a femtosecond laser pulse. For the past two decades, ultrafast electron diffraction (UED) has played a critical role in this regard. Despite remarkable progress in instrumental development, this technique is still bottlenecked by a demanding sample preparation process, where ultrathin single crystals of large lateral size are typically required. In this work, we describe an efficient, versatile method that yields high-quality, laterally extended (≥ 100 µm), and thin (≤ 50 nm) single crystals on amorphous films of Si3N4 windows. It applies to most exfoliable materials, including those reactive in ambient conditions, and promises clean, flat surfaces. Besides the natural extension to fabricating van der Waals heterostructures, our method can also be applied to future-generation UED that enables additional control of sample parameters, such as electrostatic gating and excitation by a locally enhanced terahertz field. Our work significantly expands the type of samples for UED studies and also finds application in other time-resolved techniques such as attosecond extreme-ultraviolet absorption spectroscopy. This method hence provides further opportunities to explore photoinduced transitions and to discover novel states of matter out of equilibrium.

Unconventional ferroelectricity in moiré heterostructures.

The constituent particles of matter can arrange themselves in various ways, giving rise to emergent phenomena that can be surprisingly rich and often cannot be understood by studying only the individual constituents. Discovering and understanding the emergence of such phenomena in quantum materials-especially those in which multiple degrees of freedom or energy scales are delicately balanced-is of fundamental interest to condensed-matter research1,2. Here we report on the surprising observation of emergent ferroelectricity in graphene-based moiré heterostructures. Ferroelectric materials show electrically switchable electric dipoles, which are usually formed by spatial separation between the average centres of positive and negative charge within the unit cell. On this basis, it is difficult to imagine graphene-a material composed of only carbon atoms-exhibiting ferroelectricity3. However, in this work we realize switchable ferroelectricity in Bernal-stacked bilayer graphene sandwiched between two hexagonal boron nitride layers. By introducing a moiré superlattice potential (via aligning bilayer graphene with the top and/or bottom boron nitride crystals), we observe prominent and robust hysteretic behaviour of the graphene resistance with an externally applied out-of-plane displacement field. Our systematic transport measurements reveal a rich and striking response as a function of displacement field and electron filling, and beyond the framework of conventional ferroelectrics. We further directly probe the ferroelectric polarization through a non-local monolayer graphene sensor. Our results suggest an unconventional, odd-parity electronic ordering in the bilayer graphene/boron nitride moiré system. This emergent moiré ferroelectricity may enable ultrafast, programmable and atomically thin carbon-based memory devices.

Emergent phenomena and proximity effects in two-dimensional magnets and heterostructures.

Ultrathin van der Waals materials and their heterostructures offer a simple, yet powerful platform for discovering emergent phenomena and implementing device structures in the two-dimensional limit. The past few years has pushed this frontier to include magnetism. These advances have brought forth a new assortment of layered materials that intrinsically possess a wide variety of magnetic properties and are instrumental in integrating exchange and spin-orbit interactions into van der Waals heterostructures. This Review Article summarizes recent progress in exploring the intrinsic magnetism of atomically thin van der Waals materials, manipulation of their magnetism by tuning the interlayer coupling, and device structures for spin- and valleytronic applications.

Author Correction: Configurable phonon polaritons in twisted α-MoO3.

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

Observation of Terahertz-Induced Magnetooscillations in Graphene.

When high-frequency radiation is incident upon graphene subjected to a perpendicular magnetic field, graphene absorbs incident photons by allowing transitions between nearest Landau levels that follow strict selection rules dictated by angular momentum conservation. Here, we show a qualitative deviation from this behavior in high-quality graphene devices exposed to terahertz (THz) radiation. We demonstrate the emergence of a pronounced THz-driven photoresponse, which exhibits low-field magnetooscillations governed by the ratio of the frequency of the incoming radiation and the quasiclassical cyclotron frequency. We analyze the modifications of generated photovoltage with the radiation frequency and carrier density and demonstrate that the observed photoresponse shares a common origin with microwave-induced resistance oscillations discovered in GaAs-based heterostructures; however, in graphene it appears at much higher frequencies and persists above liquid nitrogen temperatures. Our observations expand the family of radiation-driven phenomena in graphene, paving the way for future studies of nonequilibrium electron transport.