arXiv subjects

Pablo Jarillo-Herrero

Publications and source records attributed to Pablo Jarillo-Herrero.

At least 55 records · Page 3Linked to original sources

arXiv2021

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.

cond-mat.mtrl-sci↗

arXiv2021

Interfacial ferroelectricity in rhombohedral-stacked bilayer transition metal dichalcogenides

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 moiré 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.

cond-mat.mes-hall↗

arXiv2021

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 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 moiré systems with native flat Chern bands.

cond-mat.mes-hall↗

arXiv2021

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, 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.

cond-mat.mtrl-sci↗

arXiv2021

Stacking-engineered ferroelectricity in bilayer boron nitride

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 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.

cond-mat.mes-hall↗

arXiv2021

Large Pauli Limit Violation and Reentrant Superconductivity in Magic-Angle Twisted Trilayer Graphene

Moiré 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 moiré superconductivity and may pave a new route towards designing next-generation exotic quantum matter.

cond-mat.mes-hall↗

arXiv2021

Unconventional sequence of correlated Chern insulators in magic-angle twisted bilayer graphene

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 moiré band filling factors $ν= \pm 1, \, \pm 2, \, \pm 3$, 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 moiré 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.

cond-mat.mes-hall↗

arXiv2020

Tunable Phase Boundaries and Ultra-Strong Coupling Superconductivity in Mirror Symmetric Magic-Angle Trilayer Graphene

Moiré 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 moiré systems, magic-angle twisted bilayer graphene (MATBG) remains the only one where robust superconductivity has been reproducibly measured. Here we realize a new moiré 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 moiré 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 moiré superconductors with the potential to revolutionize our fundamental understanding and the applications of strong coupling superconductivity.

cond-mat.supr-con↗

arXiv2020

Highly Tunable Junctions and Nonlocal Josephson Effect in Magic Angle Graphene Tunneling Devices

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.

cond-mat.supr-con↗

arXiv2020

Entropic evidence for a Pomeranchuk effect in magic angle graphene

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.

cond-mat.mes-hall↗

arXiv2020

Flavour Hund's Coupling, Correlated Chern Gaps, and Diffusivity in Moiré Flat Bands

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 out of which ultimately correlated and topological ground states emerge. However, the microscopic mechanism of such flavour symmetry breaking and its connection to the low-temperature many-body phases remain to be understood. Here, we investigate the symmetry-broken 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 a pinning of the chemical potential $μ$ at all integer fillings of the moiré superlattice, highlighting 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 $C=3,2,1$ at filling factors $ν=1,2,3$, respectively, consistent with flavour symmetry breaking in the Hofstadter's butterfly spectrum of MATBG. Moreover, our concurrent measurements of resistivity and chemical potential allow us to obtain the temperature dependence of the charge diffusivity of MATBG in the strange metal regime, a quantity previously explored only in ultracold atom systems. Our results bring us one step closer to a unified framework for understanding interactions in the topological bands of MATBG, both in the presence and absence of a magnetic field.

cond-mat.mes-hall↗

arXiv2020

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 LLs 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 previously observed in GaAs-based heterostructures, yet 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 and offer potential for the development of novel optoelectronic devices.

cond-mat.mes-hall↗

arXiv2020

Nematicity and Competing Orders in Superconducting Magic-Angle Graphene

Strongly interacting electrons in solid-state systems often display tendency towards multiple broken symmetries in the ground state. The complex interplay between different order parameters can give rise to a rich phase diagram. Here, 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 crossing the superconducting dome, a reduction of the critical temperature is observed, similar to the behavior of certain cuprate superconductors. Furthermore, the superconducting state exhibits a anisotropic response to an directional-dependent in-plane magnetic field, revealing a nematic pairing state 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, and pave the way for using highly-tunable moiré superlattices to investigate intertwined phases in quantum materials.

cond-mat.mes-hall↗

arXiv2020

Deep-Learning-Enabled Fast Optical Identification and Characterization of Two-Dimensional Materials

Advanced microscopy and/or spectroscopy tools play indispensable role in nanoscience and nanotechnology research, as it provides rich information about the growth mechanism, chemical compositions, crystallography, and other important physical and chemical properties. However, the interpretation of imaging data heavily relies on the "intuition" of experienced researchers. As a result, many of the deep graphical features obtained through these tools are often unused because of difficulties in processing the data and finding the correlations. Such challenges can be well addressed by deep learning. In this work, we use the optical characterization of two-dimensional (2D) materials as a case study, and demonstrate a neural-network-based algorithm for the material and thickness identification of exfoliated 2D materials with high prediction accuracy and real-time processing capability. Further analysis shows that the trained network can extract deep graphical features such as contrast, color, edges, shapes, segment sizes and their distributions, based on which we develop an ensemble approach topredict the most relevant physical properties of 2D materials. Finally, a transfer learning technique is applied to adapt the pretrained network to other applications such as identifying layer numbers of a new 2D material, or materials produced by a different synthetic approach. Our artificial-intelligence-based material characterization approach is a powerful tool that would speed up the preparation, initial characterization of 2D materials and other nanomaterials and potentially accelerate new material discoveries.

cond-mat.mtrl-sci↗

arXiv2019

Cascade of Phase Transitions and Dirac Revivals in Magic Angle Graphene

Twisted bilayer graphene near the magic angle exhibits remarkably rich electron correlation physics, displaying insulating, magnetic, and superconducting phases. Here, using measurements of the local electronic compressibility, we reveal that these phases originate from a high-energy state with an unusual sequence of band populations. As carriers are added to the system, rather than filling all the four spin and valley flavors equally, we find that the population occurs through a sequence of sharp phase transitions, which appear as strong asymmetric jumps of the electronic compressibility near integer fillings of the moire lattice. At each transition, a single spin/valley flavor takes all the carriers from its partially filled peers, "resetting" them back to the vicinity of the charge neutrality point. As a result, the Dirac-like character observed near the charge neutrality reappears after each integer filling. Measurement of the in-plane magnetic field dependence of the chemical potential near filling factor one reveals a large spontaneous magnetization, further substantiating this picture of a cascade of symmetry breakings. The sequence of phase transitions and Dirac revivals is observed at temperatures well above the onset of the superconducting and correlated insulating states. This indicates that the state we reveal here, with its strongly broken electronic flavor symmetry and revived Dirac-like electronic character, is a key player in the physics of magic angle graphene, forming the parent state out of which the more fragile superconducting and correlated insulating ground states emerge.

cond-mat.mes-hall↗

arXiv2019

Optical detection and manipulation of spontaneous gyrotropic electronic order in a transition-metal dichalcogenide semimetal

The observation of chirality is ubiquitous in nature. Contrary to intuition, the population of opposite chiralities is surprisingly asymmetric at fundamental levels. Examples range from parity violation in the subatomic weak force to the homochirality in essential biomolecules. The ability to achieve chirality-selective synthesis (chiral induction) is of great importance in stereochemistry, molecular biology and pharmacology. In condensed matter physics, a crystalline electronic system is geometrically chiral when it lacks any mirror plane, space inversion center or roto-inversion axis. Typically, the geometrical chirality is predefined by a material's chiral lattice structure, which is fixed upon the formation of the crystal. By contrast, a particularly unconventional scenario is the gyrotropic order, where chirality spontaneously emerges across a phase transition as the electron system breaks the relevant symmetries of an originally achiral lattice. Such a gyrotropic order, proposed as the quantum analogue of the cholesteric liquid crystals, has attracted significant interest. However, to date, a clear observation and manipulation of the gyrotropic order remain challenging. We report the realization of optical chiral induction and the observation of a gyrotropically ordered phase in the transition-metal dichalcogenide semimetal $1T$-TiSe$_2$. We show that shining mid-infrared circularly polarized light near the critical temperature leads to the preferential formation of one chiral domain. As a result, we are able to observe an out-of-plane circular photogalvanic current, whose direction depends on the optical induction. Our study provides compelling evidence for the spontaneous emergence of chirality in the correlated semimetal TiSe$_2$. Such chiral induction provides a new way of optical control over novel orders in quantum materials.

cond-mat.mes-hall↗

arXiv2019

Collective excitations in twisted bilayer graphene close to the magic angle

The electronic properties of twisted bilayer graphene (TBG) can be dramatically different from those of a single graphene layer, in particular when the two layers are rotated relative to each other by a small angle. TBG has recently attracted a great deal of interest, sparked by the discovery of correlated insulating and superconducting states, for twist angle $θ$ close to a so-called 'magic angle' $\approx 1.1°$. In this work, we unveil, via near-field optical microscopy, a collective plasmon mode in charge-neutral TBG near the magic angle, which is dramatically different from the ordinary single-layer graphene intraband plasmon. In selected regions of our samples, we find a gapped collective mode with linear dispersion, akin to the bulk magnetoplasmons of a two-dimensional (2D) electron gas. We interpret these as interband plasmons and associate those with the optical transitions between quasi-localized states originating from the moiré superlattice. Surprisingly, we find a higher plasmon group velocity than expected, which implies an enhanced strength of the corresponding optical transition. This points to a weaker interlayer coupling in the AA regions. These intriguing optical properties offer new insights, complementary to other techniques, on the carrier dynamics in this novel quantum electron system.

cond-mat.str-el↗

arXiv2019

Mapping the twist angle and unconventional Landau levels in magic angle graphene

The emergence of flat electronic bands and of the recently discovered strongly correlated and superconducting phases in twisted bilayer graphene crucially depends on the interlayer twist angle upon approaching the magic angle $θ_M \approx 1.1°$. Although advanced fabrication methods allow alignment of graphene layers with global twist angle control of about 0.1$°$, little information is currently available on the distribution of the local twist angles in actual magic angle twisted bilayer graphene (MATBG) transport devices. Here we map the local $θ$ variations in hBN encapsulated devices with relative precision better than 0.002$°$ and spatial resolution of a few moir$é$ periods. Utilizing a scanning nanoSQUID-on-tip, we attain tomographic imaging of the Landau levels in the quantum Hall state in MATBG, which provides a highly sensitive probe of the charge disorder and of the local band structure determined by the local $θ$. We find that even state-of-the-art devices, exhibiting high-quality global MATBG features including superconductivity, display significant variations in the local $θ$ with a span close to 0.1$°$. Devices may even have substantial areas where no local MATBG behavior is detected, yet still display global MATBG characteristics in transport, highlighting the importance of percolation physics. The derived $θ$ maps reveal substantial gradients and a network of jumps. We show that the twist angle gradients generate large unscreened electric fields that drastically change the quantum Hall state by forming edge states in the bulk of the sample, and may also significantly affect the phase diagram of correlated and superconducting states. The findings call for exploration of band structure engineering utilizing twist-angle gradients and gate-tunable built-in planar electric fields for novel correlated phenomena and applications.

cond-mat.mes-hall↗