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Chirality pervades natural processes from the atomic to the cosmic scales, crucially impacting molecular chemistry and pharmaceutics. Traditional chirality sensing methods face challenges in sensitivity and efficiency, prompting the quest of novel chiral recognition solutions based on nanophotonics. In this work we theoretically investigate the possibility to carry out enantiomeric discrimination by measuring the spontaneous emission rate of chiral molecules on twisted two-dimensional materials. We first present a general theoretical framework based on dyadic Green's functions to calculate the chiral contribution to the decay rate in the presence of a generic chiral bilayer interface. We then combine this theory with density functional theory to obtain numerical estimates of the decay rate of helical bilayer nanographene molecules placed on top of twisted bilayer graphene., Comment: 9 pages, 2 figures, 6 appendices. Draft version. Comments are welcome!

Selective sensing of chiral molecules is a key aspect in fields spanning biology, chemistry, and pharmacology. However, conventional optical methods, such as circular dichroism (CD), encounter limitations owing to weak chiral light-matter interactions. Several strategies have been investigated to enhance CD or circularly polarised luminescence (CPL), including superchiral light, plasmonic nanoresonators and dielectric nanostructures. However, a compromise between spatial uniformity and high sensitivity, without requiring specific molecular functionalization, remains a challenge. In this work, we propose a novel approach using twisted bilayer graphene (TBG), a chiral 2D material with a strong CD peak which energy is tunable through the twist angle. By matching the CD resonance of TBG with the optical transition energy of the molecule, we achieve a decay rate enhancement mediated by resonant energy transfer that depends on the electric-magnetic interaction, that is, on the chirality of both the molecules and TBG. This leads to an enantioselective quenching of the molecule fluorescence, allowing to retrieve the molecule chirality from time-resolved photoluminescence measurements. This method demonstrates high sensitivity down to single layer of molecules, with the potential to achieve the ultimate goal of single-molecule chirality sensing, while preserving the spatial uniformity and integrability of 2D heterostructures.

Plasmon polaritons are formed by coupling light with delocalized electrons. The half-light and half-matter nature of plasmon polaritons endows them with unparalleled tunability via a range of parameters, such as dielectric environments and carrier density. Therefore, plasmon polaritons are expected to be tuned when in proximity to polar materials since the carrier density is tuned by an electrostatic potential; conversely, the plasmon polariton response might enable the sensing of polarization. Here, we use infrared nano-imaging and nano-photocurrent measurements to investigate heterostructures composed of graphene and twisted hexagonal boron nitride (t-BN), with alternating polarization in a triangular network of moir\'e stacking domains. We observe that the carrier density and the corresponding plasmonic response of graphene are modulated by polar domains in t-BN. In addition, we demonstrate that the nanometer-wide domain walls of graphene moir\'es superlattices, created by the polar domains of t-BN, provide momenta to assist the plasmonic excitations. Furthermore, our studies establish that the plasmon of graphene could function as a delicate sensor for polarization textures. The evolution of polarization textures in t-BN under uniform electric fields is tomographically examined via plasmonic imaging. Strikingly, no noticeable polarization switching is observed under applied electric fields up to 0.23 V/nm, at variance with transport reports. Our nano-images unambiguously reveal that t-BN with triangular domains acts like a ferrielectric, rather than ferroelectric claimed by many previous studies., Comment: 41 pages, 20 figures

Moir\'e materials represent strongly interacting electron systems bridging topological and correlated physics. Despite significant advances, decoding wavefunction properties underlying the quantum geometry remains challenging. Here, we utilize polarization-resolved photocurrent measurements to probe magic-angle twisted bilayer graphene, leveraging its sensitivity to the Berry connection that encompasses quantum "textures" of electron wavefunctions. Using terahertz light resonant with optical transitions of its flat bands, we observe bulk photocurrents driven by broken symmetries and reveal the interplay between electron interactions and quantum geometry. We observe inversion-breaking gapped states undetectable through quantum transport, sharp changes in the polarization axes caused by interaction-induced band renormalization, and recurring photocurrent patterns at integer fillings of the moir\'e unit cell that track the evolution of quantum geometry through the cascade of phase transitions. The large and tunable terahertz response intrinsic to flat-band systems offers direct insights into the quantum geometry of interacting electrons and paves the way for innovative terahertz quantum technologies.

The robustness of the macroscopic quantum nature of a superconductor can be characterized by the superfluid stiffness, $\rho_s$, a quantity that describes the energy required to vary the phase of the macroscopic quantum wave function. In unconventional superconductors, such as cuprates, the low-temperature behavior of $\rho_s$ drastically differs from that of conventional superconductors due to quasiparticle excitations from gapless points (nodes) in momentum space. Intensive research on the recently discovered magic-angle twisted graphene family has revealed, in addition to superconducting states, strongly correlated electronic states associated with spontaneously broken symmetries, inviting the study of $\rho_s$ to uncover the potentially unconventional nature of its superconductivity. Here we report the measurement of $\rho_s$ in magic-angle twisted trilayer graphene (TTG), revealing unconventional nodal-gap superconductivity. Utilizing radio-frequency reflectometry techniques to measure the kinetic inductive response of superconducting TTG coupled to a microwave resonator, we find a linear temperature dependence of $\rho_s$ at low temperatures and nonlinear Meissner effects in the current bias dependence, both indicating nodal structures in the superconducting order parameter. Furthermore, the doping dependence shows a linear correlation between the zero temperature $\rho_s$ and the superconducting transition temperature $T_c$, reminiscent of Uemura's relation in cuprates, suggesting phase-coherence-limited superconductivity. Our results provide strong evidence for nodal superconductivity in TTG and put strong constraints on the mechanisms of these graphene-based superconductors.

The physics of superconductivity in magic-angle twisted bilayer graphene (MATBG) is a topic of keen interest in moir\'e systems research, and it may provide insight into the pairing mechanism of other strongly correlated materials such as high-$T_{\mathrm{c}}$ superconductors. Here, we use DC-transport and microwave circuit quantum electrodynamics (cQED) to measure directly the superfluid stiffness of superconducting MATBG via its kinetic inductance. We find the superfluid stiffness to be much larger than expected from conventional single-band Fermi liquid theory; rather, it aligns well with theory involving quantum geometric effects that are dominant at the magic angle. The temperature dependence of the superfluid stiffness exhibits a power-law behavior, which contraindicates an isotropic BCS model; instead, the extracted power-law exponents indicate an anisotropic superconducting gap, whether interpreted using the conventional anisotropic BCS model or a quantum geometric theory of flat-band superconductivity. Moreover, the quadratic dependence of the stiffness on both DC and microwave current is consistent with Ginzburg-Landau theory. Taken together, these findings strongly suggest a connection between quantum geometry, superfluid stiffness, and unconventional superconductivity in MATBG. Finally, the combined DC-microwave measurement platform used here is applicable to the investigation of other atomically thin superconductors.

Applying long wavelength periodic potentials on quantum materials has recently been demonstrated to be a promising pathway for engineering novel quantum phases of matter. Here, we utilize twisted bilayer boron nitride (BN) as a moir\'e substrate for band structure engineering. Small-angle-twisted bilayer BN is endowed with periodically arranged up and down polar domains, which imprints a periodic electrostatic potential on a target two-dimensional (2D) material placed on top. As a proof of concept, we use Bernal bilayer graphene as the target material. The resulting modulation of the band structure appears as superlattice resistance peaks, tunable by varying the twist angle, and Hofstadter butterfly physics under a magnetic field. Additionally, we demonstrate the tunability of the moir\'e potential by altering the dielectric thickness underneath the twisted BN. Finally, we find that near-60{\deg}-twisted bilayer BN provides a unique platform for studying the moir\'e structural effect without the contribution from electrostatic moir\'e potentials. Tunable moir\'e polar substrates may serve as versatile platforms to engineer the electronic, optical, and mechanical properties of 2D materials and van der Waals heterostructures., Comment: 21 pages, 11 figures

In multilayer moir\'e heterostructures, the interference of multiple twist angles ubiquitously leads to tunable ultra-long-wavelength patterns known as supermoir\'e lattices. However, their impact on the system's many-body electronic phase diagram remains largely unexplored. We present local compressibility measurements revealing numerous incompressible states resulting from supermoir\'e-lattice-scale isospin symmetry breaking driven by strong interactions. By using the supermoir\'e lattice occupancy as a probe of isospin symmetry, we observe an unexpected doubling of the miniband filling near $\nu=-2$, possibly indicating a hidden phase transition or normal-state pairing proximal to the superconducting phase. Our work establishes supermoir\'e lattices as a tunable parameter for designing novel quantum phases and an effective tool for unraveling correlated phenomena in moir\'e materials.

Strong interactions between particles can lead to emergent collective excitations. These phenomena have been extensively established in electronic systems, but are also expected to occur for gases of neutral particles like spin waves, also known as magnons, in a ferromagnet. In a hydrodynamic regime where magnons are strongly interacting, they can form a slow collective density mode -- in analogy to sound waves in water -- with characteristic low-frequency signatures. While such a mode has been predicted in theory, its signatures have yet to be observed experimentally. In this work, we isolate atomically-thin sheets of ferromagnetic CrCl$_3$ where magnon interactions are strong, and develop a technique to measure its collective magnon dynamics via the quantum coherence of nearby Nitrogen-Vacancy (NV) centers in diamond. We find that the thermal magnetic fluctuations generated by CrCl$_3$ exhibit an anomalous temperature-dependence, whereby fluctuations increase upon decreasing temperature. Our analysis reveals that this anomalous trend is a consequence of the damping rate of a low-energy magnon sound mode which sharpens as magnon interactions increase with increasing temperature, providing a first glimpse of the magnon hydrodynamic regime.

We present a theoretical study of the intrinsic plasmonic properties of twisted bilayer graphene (TBG) as a function of the twist angle $\theta$ (and other microscopic parameters such as temperature and filling factor). Our calculations, which rely on the random phase approximation, take into account four crucially important effects, which are treated on equal footing: i) the layer-pseudospin degree of freedom, ii) spatial non-locality of the density-density response function, iii) crystalline local field effects, and iv) Hartree self-consistency. We show that the plasmonic spectrum of TBG displays a smooth transition from a strongly-coupled regime (at twist angles $\theta \lesssim 2^{\circ}$), where the low-energy spectrum is dominated by a weakly dispersive intra-band plasmon, to a weakly-coupled regime (for twist angles $\theta \gtrsim 2^{\circ}$) where an acoustic plasmon clearly emerges. This crossover offers the possibility of realizing tunable mid-infrared sub-wavelength cavities, whose vacuum fluctuations may be used to manipulate the ground state of strongly correlated electron systems., Comment: 11 pages, 4 figures + Supplemental Material

In strongly interacting systems with multiple energy bands, the interplay between electrons with different effective masses and the enlarged Hilbert space drives intricate correlated phenomena that do not occur in single-band systems. Recently, magic-angle twisted trilayer graphene (MATTG) has emerged as a promising tunable platform for such investigations: the system hosts both slowly dispersing, "heavy" electrons inhabiting its flat bands as well as delocalized "light" bands that disperse as free Dirac fermions. Most remarkably, superconductivity in twisted trilayer graphene and multilayer analogues with additional dispersive bands exhibits Pauli limit violation and spans a wider range of phase space compared to that in twisted bilayer graphene, where the dispersive bands are absent. This suggests that the interactions between different bands may play a fundamental role in stabilizing correlated phases in twisted graphene multilayers. Here, we elucidate the interplay between the light and heavy electrons in MATTG as a function of doping and magnetic field by performing local compressibility measurements with a scanning single-electron-transistor microscope. We establish that commonly observed resistive features near moir\'e band fillings $\nu$=-2, 1, 2 and 3 host a finite population of light Dirac electrons at the Fermi level despite a gap opening in the flat band sector. At higher magnetic field and near charge neutrality, we discover a new type of phase transition sequence that is robust over nearly 10 micrometers but exhibits complex spatial dependence. Mean-field calculations establish that these transitions arise from the competing population of the two subsystems and that the Dirac sector can be viewed as a new flavor analogous to the spin and valley degrees of freedom.

Chirality-induced spin selectivity (CISS) is an effect that has recently attracted a great deal of attention in chiral chemistry and that remains to be understood. In the CISS effect, electrons passing through chiral molecules acquire a large degree of spin polarization. In this work we study the case of atomically-thin chiral crystals created by van der Waals assembly. We show that this effect can be spectacularly large in systems containing just two monolayers, provided they are spin-orbit coupled. Its origin stems from the combined effects of structural chirality and spin-flipping spin-orbit coupling. We present detailed calculations for twisted homobilayer transition metal dichalcogenides, showing that the chirality-induced spin polarization can be giant, e.g. easily exceeding $50\%$ for ${\rm MoTe}_2$. Our results clearly indicate that twisted quantum materials can operate as a fully tunable platform for the study and control of the CISS effect in condensed matter physics and chiral chemistry., Comment: 6 pages, 4 figures + Supplemental Material

Two-dimensional materials (2DM) and their derived heterostructures have electrical and optical properties that are widely tunable via several approaches, most notably electrostatic gating and interfacial engineering such as twisting. While electrostatic gating is simple and has been ubiquitously employed on 2DM, being able to tailor the interfacial properties in a similar real-time manner represents the next leap in our ability to modulate the underlying physics and build exotic devices with 2DM. However, all existing approaches rely on external machinery such as scanning microscopes, which often limit their scope of applications, and there is currently no means of tuning a 2D interface that has the same accessibility and scalability as electrostatic gating. Here, we demonstrate the first on-chip platform designed for 2D materials with in situ tunable interfacial properties, utilizing a microelectromechanical system (MEMS). Each compact, cost-effective, and versatile device is a standalone micromachine that allows voltage-controlled approaching, twisting, and pressurizing of 2DM with high accuracy. As a demonstration, we engineer synthetic topological singularities, known as merons, in the nonlinear optical susceptibility of twisted hexagonal boron nitride (h-BN), via simultaneous control of twist angle and interlayer separation. The chirality of the resulting moire pattern further induces a strong circular dichroism in the second-harmonic generation. A potential application of this topological nonlinear susceptibility is to create integrated classical and quantum light sources that have widely and real-time tunable polarization. Our invention pushes the boundary of available technologies for manipulating low-dimensional quantum materials, which in turn opens up the gateway for designing future hybrid 2D-3D devices for condensed-matter physics, quantum optics, and beyond., Comment: 10 pages, 4 figures

Quantum geometry of electronic wavefunctions results in fascinating topological phenomena. A prominent example is the intrinsic anomalous Hall effect (AHE) in which a Hall voltage arises in the absence of an applied magnetic field. The AHE requires a coexistence of Berry curvature and spontaneous time-reversal symmetry breaking. These conditions can be realized in two-dimensional moir\'e systems with broken $xy$-inversion symmetry ($C_{2z}$) that host flat electronic bands. Here, we explore helical trilayer graphene (HTG), three graphene layers twisted sequentially by the same angle forming two misoriented moir\'e patterns. Although HTG is globally $C_{2z}$-symmetric, surprisingly we observe clear signatures of topological bands. At a magic angle $\theta_\mathrm{m}\approx 1.8^\circ$, we uncover a robust phase diagram of correlated and magnetic states using magnetotransport measurements. Lattice relaxation leads to large periodic domains in which $C_{2z}$ is broken on the moir\'e scale. Each domain harbors flat topological bands with valley-contrasting Chern numbers $\pm(1,-2)$. We find correlated states at integer electron fillings per moir\'e unit cell $\nu=1,2,3$ and fractional fillings $2/3,7/2$ with the AHE arising at $\nu=1,3$ and $2/3,7/2$. At $\nu=1$, a time-reversal symmetric phase appears beyond a critical electric displacement field, indicating a topological phase transition. Finally, hysteresis upon sweeping $\nu$ points to first-order phase transitions across a spatial mosaic of Chern domains separated by a network of topological gapless edge states. We establish HTG as an important platform that realizes ideal conditions for exploring strongly interacting topological phases and, due to its emergent moir\'e-scale symmetries, demonstrates a novel way to engineer topology.

Electronic ferroelectricity represents a new paradigm where spontaneous symmetry breaking driven by electronic correlations, in contrast to traditional lattice-driven ferroelectricity, leads to the formation of electric dipoles. Despite the potential application advantages arising from its electronic nature, switchable electronic ferroelectricity remains exceedingly rare. Here, we report the discovery of an electronic ratchet effect that manifests itself as switchable electronic ferroelectricity in a layer-contrasting graphene-boron nitride moir\'e heterostructure. Our engineered layer-asymmetric moir\'e potential landscapes result in layer-polarized localized and itinerant electronic subsystems. At particular fillings of the localized subsystem, we find a ratcheting injection of itinerant carriers in a non-volatile manner, leading to a highly unusual ferroelectric response. Strikingly, the remnant polarization can be stabilized at multiple (quasi-continuous) states with behavior markedly distinct from known ferroelectrics. Our experimental observations, simulations, and theoretical analysis suggest that dipolar excitons are the driving force and elementary ferroelectric units in our system. This signifies a new type of electronic ferroelectricity where the formation of dipolar excitons with aligned moments generates a macroscopic polarization and leads to an electronically-driven ferroelectric response, which we term excitonic ferroelectricity. Such new ferroelectrics, driven by quantum objects like dipolar excitons, could pave the way to innovative quantum analog memory and synaptic devices.

We propose helical trilayer graphene (HTG), a helical structure featuring identical rotation angles $\theta\approx 1.5^\circ$ between three consecutive layers of graphene, as a unique and experimentally accessible platform for realizing exotic correlated topological states of matter. While nominally forming a supermoir\'e (or moir\'e-of-moir\'e) structure, we show that HTG locally relaxes into large regions of a periodic single-moir\'e structure in which $C_{2z}$ is broken, giving rise to flat topological bands carrying valley-Chern numbers $C=\pm(1,-2)$. These bands feature near-ideal quantum geometry and are isolated from remote bands by a large gap $E_{\mathrm{gap}}\sim 100$ meV, making HTG a promising platform for experimental realization of correlated topological states such as integer and fractional quantum anomalous Hall states in $C=1$ and $2$ bands.

We introduce a gauge-invariant model of planar, square molecules coupled to a quantized spatially-varying cavity electromagnetic vector potential A(r). Specifically, we choose a temporally chiral cavity hosting a uniform magnetic field B, as this is the simplest instance in which a transverse spatially-varying A(r) is at play. We show that when the molecules are in the Van Vleck paramagnetic regime, an equilibrium quantum phase transition to a photon condensate state occurs., Comment: 14 pages, 3 figures

Electronic states in quasiperiodic crystals generally preclude a Bloch description, rendering them simultaneously fascinating and enigmatic. Owing to their complexity and relative scarcity, quasiperiodic crystals are underexplored relative to periodic and amorphous structures. Here, we introduce a new type of highly tunable quasiperiodic crystal easily assembled from periodic components. By twisting three layers of graphene with two different twist angles, we form two moir\'e patterns with incommensurate moir\'e unit cells. In contrast to many common quasiperiodic structures that are defined on the atomic scale, the quasiperiodicity in our system is defined on moir\'e length scales of several nanometers. This novel "moir\'e quasiperiodic crystal" allows us to tune the chemical potential and thus the electronic system between a periodic-like regime at low energies and a strongly quasiperiodic regime at higher energies, the latter hosting a large density of weakly dispersing states. Interestingly, in the quasiperiodic regime we observe superconductivity near a flavor-symmetry-breaking phase transition, the latter indicative of the important role electronic interactions play in that regime. The prevalence of interacting phenomena in future systems with in situ tunability is not only useful for the study of quasiperiodic systems, but it may also provide insights into electronic ordering in related periodic moir\'e crystals. We anticipate that extending this new platform to engineer quasiperiodic crystals by varying the number of layers and twist angles, and by using different two-dimensional components, will lead to a new family of quantum materials to investigate the properties of strongly interacting quasiperiodic crystals.

Electrical control of superconductivity is critical for nanoscale superconducting circuits including cryogenic memory elements, superconducting field-effect transistors (FETs), and gate-tunable qubits. Superconducting FETs operate through continuous tuning of carrier density, but there has not yet been a bistable superconducting FET, which could serve as a new type of cryogenic memory element. Recently, unusual ferroelectricity in Bernal-stacked bilayer graphene aligned to its insulating hexagonal boron nitride (BN) gate dielectrics was discovered. Here, we report the observation of ferroelectricity in magic-angle twisted bilayer graphene (MATBG) with aligned BN layers. This ferroelectric behavior 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 moir\'{e} ferroelectric superconductor into highly tunable superconducting electronics.

Technologies operating on the basis of quantum mechanical laws and resources such as phase coherence and entanglement are expected to revolutionize our future. Quantum technologies are often divided into four main pillars: computing, simulation, communication, and sensing & metrology. Moreover, a great deal of interest is currently also nucleating around energy-related quantum technologies. In this Perspective, we focus on advanced superconducting materials, van der Waals materials, and moir\'e quantum matter, summarizing recent exciting developments and highlighting a wealth of potential applications, ranging from high-energy experimental and theoretical physics to quantum materials science and energy storage., Comment: 19 pages, 4 figures, 215 references, Perspective article on solid-state quantum technologies

The discovery of correlated states and superconductivity in magic-angle twisted bilayer graphene (MATBG) has established moir\'e quantum matter as a new platform to explore interaction-driven and topological quantum phenomena. Multitudes of phases have been realized in moir\'e systems, but surprisingly, robust superconductivity has been one of the least common of all, initially found in MATBG and only more recently also in magic-angle twisted trilayer graphene (MATTG). While MATBG and MATTG share some similar characteristics, they also exhibit substantial differences, such as in their response to external electric and magnetic fields. This raises the question of whether they are simply two separate unique systems, or whether they form part of a broader family of superconducting materials. Here, we report the experimental realization of magic-angle twisted 4-layer and 5-layer graphene (MAT4G and MAT5G, respectively), which turn out to be superconductors, hence establishing alternating-twist magic-angle multilayer graphene as a robust family of moir\'e superconductors. The members of this family have flat bands in their electronic structure as a common feature, suggesting their central role in the observed robust superconductivity. On the other hand, there are also important variations across the family, such as different symmetries for members with even and odd number of layers. However, our measurements in parallel magnetic fields, in particular the investigation of Pauli limit violation and spontaneous rotational symmetry breaking, reveal that the most pronounced distinction is between the N=2 and N>2-layer structures. Our results expand the emergent family of moir\'e superconductors, providing new insight with potential implications for the design of novel superconducting materials platforms., Comment: 15 pages, 4 figures

Emergent phenomena arising from the collective behavior of electrons is generally expected when Coulomb interactions dominate over the kinetic energy, as in delocalized quasiparticles in highly degenerate flat bands. Bernal-stacked bilayer graphene intrinsically supports a pair of flat bands predicted to host a variety of spontaneous broken-symmetry states arising from van Hove singularities and a four-fold spin-valley (isospin) degeneracy. Here, we show that ultra-clean samples of bilayer graphene display a cascade of symmetry-broken states with spontaneous and spin and valley ordering at zero magnetic field. Using capacitive sensing in a dual-gated geometry, we tune the carrier density and electric displacement field independently to explore the phase space of transitions and probe the character of the isospin order. Itinerant ferromagnetic states emerge near the conduction and valence band edges with complete spin and valley polarization and a high degree of displacement field tunability. At larger hole densities, two-fold degenerate quantum oscillations manifest in an additional broken symmetry state that is enhanced by the application of an in-plane magnetic field. Both types of symmetry-broken states display enhanced layer polarization at low temperatures, suggesting a coupling to the layer pseudospin degree of freedom in the electronic wavefunctions. Notably, the zero-field spontaneous symmetry breaking reported here emerges in the absence of a moir\'e superlattice and is intrinsic to natural graphene bilayers. Thus, we demonstrate that the tunable bands of bilayer graphene represent a related, but distinct approach to produce flat band collective behavior, complementary to engineered moir\'e structures.

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.

Dielectrics with low loss at microwave frequencies are imperative for high-coherence solid-state quantum computing platforms. 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 NbSe$_{2}$-hBN-NbSe$_{2}$ 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 aluminum Josephson junctions to realize transmon qubits with coherence times reaching 25 $\mu$s, 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 to conventional all-aluminum 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.

Van der Waals (vdW) 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 emergent physical properties absent in the parent compounds through interlayer interactions. Here we report on a new family of emergent, nanometer-thick, semiconductor 2D ferroelectrics, 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 moir\'e ferroelectric domains as well as electric-field-induced domain wall motion with piezoelectric force microscopy (PFM). 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 novel semiconducting ferroelectric properties of these four new TMDs opens up the possibility of studying the interplay between ferroelectricity and their rich electric and optical properties., Comment: 16 pages, 4 figures

Fractional Chern insulators (FCIs) are lattice analogues of fractional quantum Hall states that may provide a new avenue toward manipulating non-abelian excitations. Early theoretical studies have predicted their existence in systems with energetically flat Chern bands and highlighted the critical role of a particular quantum band geometry. Thus far, however, FCI states have only been observed in Bernal-stacked bilayer graphene aligned with hexagonal boron nitride (BLG/hBN), in which a very large magnetic field is responsible for the existence of the Chern bands, precluding the realization of FCIs at zero field and limiting its potential for applications. By contrast, magic angle twisted bilayer graphene (MATBG) supports flat Chern bands at zero magnetic field, and therefore offers a promising route toward stabilizing zero-field FCIs. Here we report the observation of eight FCI states at low magnetic field in MATBG 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. Unlike the BLG/hBN platform, we demonstrate that the principal role of the weak magnetic field here is merely to redistribute the Berry curvature of the native Chern bands and thereby realize a quantum band geometry favorable 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 moir\'e systems with native flat Chern bands.

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, EuTe4. By combining transport, photoemission, diffraction, and x-ray absorption measurements, we observed 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 EuTe4 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.

Moir\'e quantum matter has emerged as a novel materials platform where 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 characteristics. However, direct evidence for unconventional pairing remains to be experimentally demonstrated. Here, we show that magic-angle twisted trilayer graphene (MATTG) exhibits superconductivity up to in-plane magnetic fields in excess of 10 T, which represents a large ($2\sim3$ times) violation of the Pauli limit for conventional spin-singlet superconductors. This observation is surprising for a system which is not expected to have strong spin-orbit coupling. Furthermore, the Pauli limit violation is observed over the entire superconducting phase, indicating that it is not related to a possible pseudogap phase with large superconducting amplitude pairing. More strikingly, we observe reentrant superconductivity at large magnetic fields, which is present in a narrower range of carrier density and displacement field. These findings suggest that the superconductivity in MATTG is likely driven by a mechanism resulting in non-spin-singlet Cooper pairs, where the external magnetic field can cause transitions between phases with potentially different order parameters. Our results showcase the richness of moir\'e superconductivity and may pave a new route towards designing next-generation exotic quantum matter., Comment: 19 pages, 9 figures

Starphenes are attractive compounds due to their characteristic physicochemical properties that are inherited from acenes, making them interesting compounds for organic electronics and optics. However, the instability and low solubility of larger starphene homologs make their synthesis extremely challenging. Herein, we present a new strategy leading to pristine [16]starphene in preparative scale. Our approach is based on a synthesis of a carbonyl-protected starphene precursor that is thermally converted in a solid-state form to the neat [16]starphene, which is then characterised with a variety of analytical methods, such as 13C CP-MAS NMR, TGA, MS MALDI, UV-Vis and FTIR spectroscopy. Furthermore, high-resolution STM experiments unambiguously confirm its expected structure and reveal a moderate electronic delocalisation between the pentacene arms. Nucleus-independent chemical shifts NICS(1) are also calculated to survey its aromatic character., Comment: Angewandte Chemie International Edition, Wiley-VCH Verlag, 2021

The interplay between strong electron-electron interactions and band topology can lead to novel electronic states that spontaneously break symmetries. The discovery of flat bands in magic-angle twisted bilayer graphene (MATBG) with nontrivial topology has provided a unique platform in which to search for new symmetry-broken phases. Recent scanning tunneling microscopy and transport experiments have revealed a sequence of topological insulating phases in MATBG with Chern numbers $C=\pm 3, \, \pm 2, \, \pm 1$ near moir\'e band filling factors $\nu = \pm 1, \, \pm 2, \, \pm 3$, corresponding to a simple pattern of flavor-symmetry-breaking Chern insulators. Here, we report high-resolution local compressibility measurements of MATBG with a scanning single electron transistor that reveal a new sequence of incompressible states with unexpected Chern numbers observed down to zero magnetic field. We find that the Chern numbers for eight of the observed incompressible states are incompatible with the simple picture in which the $C= \pm 1$ bands are sequentially filled. We show that the emergence of these unusual incompressible phases can be understood as a consequence of broken translation symmetry that doubles the moir\'e unit cell and splits each $C=\pm 1$ band into a $C=\pm 1$ band and a $C=0$ band. Our findings significantly expand the known phase diagram of MATBG, and shed light onto the origin of the close competition between different correlated phases in the system.

Moir\'e superlattices have recently emerged as a novel platform where correlated physics and superconductivity can be studied with unprecedented tunability. Although correlated effects have been observed in several other moir\'e systems, magic-angle twisted bilayer graphene (MATBG) remains the only one where robust superconductivity has been reproducibly measured. Here we realize a new moir\'e superconductor, mirror symmetric magic-angle twisted trilayer graphene (MATTG) with dramatically richer tunability in electronic structure and superconducting properties. Hall effect and quantum oscillations measurements as a function of density and electric field allow us to determine the system's tunable phase boundaries in the normal state. Zero magnetic field resistivity measurements then reveal that the existence of superconductivity is intimately connected to the broken symmetry phase emerging from two carriers per moir\'e unit cell. Strikingly, we find that the superconducting phase gets suppressed and bounded at the van Hove singularities (vHs) partially surrounding the broken-symmetry phase, which is difficult to reconcile with weak-coupling BCS theory. Moreover, the extensive in situ tunability of our system allows us to achieve the ultra-strong coupling regime, characterized by a Ginzburg-Landau coherence length reaching the average inter-particle distance and very large $T_\mathrm{BKT}/T_{F}$ ratios in excess of 0.1, where $T_\mathrm{BKT}$ and $T_F$ are the Berezinskii-Kosterlitz-Thouless transition and Fermi temperatures, respectively. These observations suggest that MATTG can be electrically tuned close to the two-dimensional BCS-BEC crossover. Our results establish a new generation of tunable moir\'e superconductors with the potential to revolutionize our fundamental understanding and the applications of strong coupling superconductivity., Comment: 29 pages, 13 figures

Magic-angle twisted bilayer graphene (MATBG) has recently emerged as a highly tunable two-dimensional (2D) 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 exploit the electrical tunability of MATBG to engineer Josephson junctions and tunneling transistors all within one material, defined solely by electrostatic gates. Our multi-gated device geometry offers complete control over the Josephson junction, with the ability to independently tune the weak link, barriers, and tunneling electrodes. We show that these purely 2D MATBG Josephson junctions exhibit nonlocal 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 tunneling 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. These MATBG tunneling devices, with versatile functionality encompassed within a single material, may find applications in graphene-based tunable superconducting qubits, on-chip superconducting circuits, and electromagnetic sensing in next-generation quantum nanoelectronics.

2D ferroelectrics with robust polarization down to atomic thicknesses provide novel building blocks for functional heterostructures. Experimental reports, however, remain scarce 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 is shown to exhibit 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. Furthermore, twisting the boron nitride sheets by a small-angle changes the dynamics of switching due to the formation of moir\'e 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., Comment: Initial draft. The published paper contains piezoelectric force microscopy data

In the 1950's, Pomeranchuk predicted that, counterintuitively, liquid 3He may solidify upon heating, due to a high excess spin entropy in the solid phase. Here, using both local and global electronic entropy and compressibility measurements, we show that an analogous effect occurs in magic angle twisted bilayer graphene. Near a filling of one electron per moir'e unit cell, we observe a dramatic increase in the electronic entropy to about 1kB per unit cell. 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 with magnetic field. Moreover, the energy scales characterizing these two sets of properties are very different: whereas the compressibility jump onsets at T~30K, the bandwidth of magnetic excitations is ~3K or smaller. The hybrid nature of the new correlated state and the large separation of energy scales have key implications for the physics of correlated states in twisted bilayer graphene.