arXiv subjects

Pablo Jarillo-Herrero

Publications and source records attributed to Pablo Jarillo-Herrero.

At least 37 records · Page 2Linked to original sources

arXiv2024

Superfluid stiffness of twisted multilayer graphene superconductors

The robustness of the macroscopic quantum nature of a superconductor can be characterized by the superfluid stiffness, $ρ_s$, 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 $ρ_s$ 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 $ρ_s$ to uncover the potentially unconventional nature of its superconductivity. Here we report the measurement of $ρ_s$ 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 $ρ_s$ 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 $ρ_s$ 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.

cond-mat.supr-con↗

arXiv2024

On-chip multi-degree-of-freedom control of two-dimensional quantum and nonlinear materials

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.

cond-mat.mes-hall↗

arXiv2024

Theory of intrinsic acoustic plasmons in twisted bilayer graphene

We present a theoretical study of the intrinsic plasmonic properties of twisted bilayer graphene (TBG) as a function of the twist angle $θ$ (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 $θ\lesssim 2^{\circ}$), where the low-energy spectrum is dominated by a weakly dispersive intra-band plasmon, to a weakly-coupled regime (for twist angles $θ\gtrsim 2^{\circ}$) 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.

cond-mat.mes-hall↗

arXiv2024

Band structure engineering using a moiré polar substrate

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 moiré 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 moiré potential by altering the dielectric thickness underneath the twisted BN. Finally, we find that near-60°-twisted bilayer BN provides a unique platform for studying the moiré structural effect without the contribution from electrostatic moiré potentials. Tunable moiré polar substrates may serve as versatile platforms to engineer the electronic, optical, and mechanical properties of 2D materials and van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2024

Strong interactions and isospin symmetry breaking in a supermoiré lattice

In multilayer moiré heterostructures, the interference of multiple twist angles ubiquitously leads to tunable ultra-long-wavelength patterns known as supermoiré 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 supermoiré-lattice-scale isospin symmetry breaking driven by strong interactions. By using the supermoiré lattice occupancy as a probe of isospin symmetry, we observe an unexpected doubling of the miniband filling near $ν=-2$, possibly indicating a hidden phase transition or normal-state pairing proximal to the superconducting phase. Our work establishes supermoiré lattices as a tunable parameter for designing novel quantum phases and an effective tool for unraveling correlated phenomena in moiré materials.

cond-mat.mes-hall↗

arXiv2024

Photon condensation, Van Vleck paramagnetism, and chiral cavities

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.

cond-mat.mes-hall↗

arXiv2024

Giant chirality-induced spin polarization in twisted transition metal dichalcogenides

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.

cond-mat.mes-hall↗

arXiv2024

Tunable interplay between light and heavy electrons in twisted trilayer graphene

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 moiré band fillings $ν$=-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.

cond-mat.mes-hall↗

arXiv2023

Helical trilayer graphene: a moiré platform for strongly-interacting topological bands

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 moiré 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 moiré patterns. Although HTG is globally $C_{2z}$-symmetric, surprisingly we observe clear signatures of topological bands. At a magic angle $θ_\mathrm{m}\approx 1.8^\circ$, 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 moiré scale. Each domain harbors flat topological bands with valley-contrasting Chern numbers $\pm(1,-2)$. We find correlated states at integer electron fillings per moiré unit cell $ν=1,2,3$ and fractional fillings $2/3,7/2$ with the AHE arising at $ν=1,3$ and $2/3,7/2$. At $ν=1$, a time-reversal symmetric phase appears beyond a critical electric displacement field, indicating a topological phase transition. Finally, hysteresis upon sweeping $ν$ 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 moiré-scale symmetries, demonstrates a novel way to engineer topology.

cond-mat.mes-hall↗

arXiv2023

Electronic ratchet effect in a moiré system: signatures of excitonic ferroelectricity

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 moiré heterostructure. Our engineered layer-asymmetric moiré 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.

cond-mat.mes-hall↗

arXiv2023

Magic-angle helical trilayer graphene

We propose helical trilayer graphene (HTG), a helical structure featuring identical rotation angles $θ\approx 1.5^\circ$ 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 supermoiré (or moiré-of-moiré) structure, we show that HTG locally relaxes into large regions of a periodic single-moiré 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.

cond-mat.str-el↗

arXiv2023

Superconductivity and strong interactions in a tunable moiré quasiperiodic crystal

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 moiré patterns with incommensurate moiré unit cells. In contrast to many common quasiperiodic structures that are defined on the atomic scale, the quasiperiodicity in our system is defined on moiré length scales of several nanometers. This novel "moiré 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 moiré 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.

cond-mat.mes-hall↗

arXiv2022

Intrinsic 1T' phase induced in atomically thin 2H-MoTe$_2$ by a single terahertz pulse

Polymorphic transitions in layered transition metal dichalcogenides provide an excellent platform for discovering exotic phenomena associated with metastable states, ranging from topological phase transitions to enhanced superconductivity. In particular, the transition from 2H to 1T'-MoTe$_2$, which was thought to be induced by high-energy photon irradiation among many other means, has been intensely studied for its technological relevance in nanoscale transistors. Despite the remarkable electrical performance arising from this 2H-to-1T' transition, it remains controversial whether a crystalline 1T' phase is produced because optical signatures of this putative transition are found to be associated with the formation of elemental Te clusters instead. Here, we demonstrate the creation of an intrinsic 1T' lattice after irradiating a mono- or few-layer 2H-MoTe$_2$ with a single field-enhanced terahertz pulse, whose low photon energy limits possible structural damage by optical pulses. To visualize the temporal evolution of this irreversible transition, we further develop a single-shot terahertz pump-second harmonic probe technique, and we find that the transition out of the 2H phase occurs within 10 ns after photoexcitation. Our results not only resolve the long-standing debate over the light-induced polymorphic transition in MoTe$_2$, they also highlight the unique capability of strong-field terahertz pulses in manipulating the structure of quantum materials.

cond-mat.mes-hall↗

arXiv2022

Electrical switching of a moiré ferroelectric superconductor

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 moiré ferroelectric superconductor into highly tunable superconducting electronics.

cond-mat.supr-con↗

arXiv2022

Materials and devices for fundamental quantum science and quantum technologies

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 moiré 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.

quant-ph↗

arXiv2022

Hexagonal Boron Nitride (hBN) 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. 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 $μ$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.

cond-mat.mes-hall↗

arXiv2021

Magic-Angle Multilayer Graphene: A Robust Family of Moiré Superconductors

The discovery of correlated states and superconductivity in magic-angle twisted bilayer graphene (MATBG) has established moiré quantum matter as a new platform to explore interaction-driven and topological quantum phenomena. Multitudes of phases have been realized in moiré 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 moiré 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 moiré superconductors, providing new insight with potential implications for the design of novel superconducting materials platforms.

cond-mat.supr-con↗

arXiv2021

Cascade of isospin phase transitions in Bernal bilayer graphene at zero magnetic field

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 moiré 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 moiré structures.

cond-mat.mes-hall↗