arXiv subjects

Pablo Jarillo-Herrero

Publications and source records attributed to Pablo Jarillo-Herrero.

At least 91 records · Page 5Linked to original sources

arXiv2018

Observation of exciton redshift-blueshift crossover in monolayer WS2

We report a rare atom-like interaction between excitons in monolayer WS2, measured using ultrafast absorption spectroscopy. At increasing excitation density, the exciton resonance energy exhibits a pronounced redshift followed by an anomalous blueshift. Using both material-realistic computation and phenomenological modeling, we attribute this observation to plasma effects and an attraction-repulsion crossover of the exciton-exciton interaction that mimics the Lennard-Jones potential between atoms. Our experiment demonstrates a strong analogy between excitons and atoms with respect to inter-particle interaction, which holds promise to pursue the predicted liquid and crystalline phases of excitons in two-dimensional materials.

cond-mat.mes-hall↗

arXiv2018

Electrical Control of 2D Magnetism in Bilayer CrI3

The challenge of controlling magnetism using electric fields raises fundamental questions and addresses technological needs such as low-dissipation magnetic memory. The recently reported two-dimensional (2D) magnets provide a new system for studying this problem owing to their unique magnetic properties. For instance, bilayer chromium triiodide (CrI3) behaves as a layered antiferromagnet with a magnetic field-driven metamagnetic transition. Here, we demonstrate electrostatic gate control of magnetism in CrI3 bilayers, probed by magneto-optical Kerr effect (MOKE) microscopy. At fixed magnetic fields near the metamagnetic transition, we realize voltage-controlled switching between antiferromagnetic and ferromagnetic states. At zero magnetic field, we demonstrate a time-reversal pair of layered antiferromagnetic states which exhibit spin-layer locking, leading to a remarkable linear dependence of their MOKE signals on gate voltage with opposite slopes. Our results pave the way for exploring new magnetoelectric phenomena and van der Waals spintronics based on 2D materials.

cond-mat.mes-hall↗

arXiv2018

Enhanced Superconductivity and Suppression of Charge-density Wave Order in 2H-TaS$_2$ in the Two-dimensional Limit

As superconductors are thinned down to the 2D limit, their critical temperature $T_c$ typically decreases. Here we report the opposite behavior, a substantial enhancement of $T_c$ with decreasing thickness, in 2D crystalline superconductor 2H-TaS$_2$. Remarkably, in the monolayer limit, $T_c$ increases to 3.4 K compared to 0.8 K in the bulk. Accompanying this trend in superconductivity, we observe suppression of the charge-density wave (CDW) transition with decreasing thickness. To explain these trends, we perform electronic structure calculations showing that a reduction of the CDW amplitude results in a substantial increase of the density of states at the Fermi energy, which contributes to the enhancement of $T_c$. Our results establish ultra-thin 2H-TaS$_2$ as an ideal platform to study the competition between CDW order and superconductivity.

cond-mat.mes-hall↗

arXiv2018

Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling

Magnetic insulators are a key resource for next-generation spintronic and topological devices. The family of layered metal halides promises ultrathin insulating multiferroics, spin liquids, and ferromagnets, but new characterization methods are required to unlock their potential. Here, we report tunneling through the layered magnetic insulator CrI3 as a function of temperature and applied magnetic field. We electrically detect the magnetic ground state and inter-layer coupling and observe a field-induced metamagnetic transition. The metamagnetic transition results in magnetoresistances of 95%, 300%, and 550% for bilayer, trilayer, and tetralayer CrI3 barriers, respectively. We further measure inelastic tunneling spectra for our junctions, unveiling a rich spectrum of collective magnetic excitations (magnons) in CrI3. Our results establish vertical tunneling as a versatile probe of magnetism in atomically thin insulators.

cond-mat.mes-hall↗

arXiv2017

Recent progress in the assembly of nanodevices and van der Waals heterostructures by deterministic placement of 2D materials

Designer heterostructures can now be assembled layer-by-layer with unmatched precision thanks to the recently developed deterministic placement methods to transfer two-dimensional (2D) materials. This possibility constitutes the birth of a very active research field on the so-called van der Waals heterostructures. Moreover, these deterministic placement methods also open the door to fabricate complex devices, which would be otherwise very difficult to achieve by conventional bottom-up nanofabrication approaches, and to fabricate fully-encapsulated devices with exquisite electronic properties. The integration of 2D materials with existing technologies such as photonic and superconducting waveguides and fiber optics is another exciting possibility. Here, we review the state-of-the-art of the deterministic placement methods, describing and comparing the different alternative methods available in the literature and we illustrate their potential to fabricate van der Waals heterostructures, to integrate 2D materials into complex devices and to fabricate artificial bilayer structures where the layers present a user-defined rotational twisting angle.

physics.app-ph↗

arXiv2017

Observation of the Quantum Spin Hall Effect up to 100 Kelvin in a Monolayer Crystal

The field of topological insulators (TI) was sparked by the prediction of the quantum spin Hall effect (QSHE) in time reversal invariant systems, such as spin-orbit coupled monolayer graphene. Ever since, a variety of monolayer crystals have been proposed as two-dimensional (2D) TIs exhibiting the QSHE, possibly even at high temperatures. However, conclusive evidence for a monolayer QSHE is still lacking, and systems based on semiconductor heterostructures operate at temperatures close to liquid helium. Here we report the observation of the QSHE in monolayer WTe2 at temperatures up to 100 Kelvin. The monolayer exhibits the hallmark quantized transport conductance, ~ e2/h per edge, in the short edge limit. Moreover, a magnetic field suppresses the conductance, and the observed Zeeman-type gap indicates the existence of a Kramers degenerate point, demonstrating the importance of time reversal symmetry for protection from elastic backscattering. Our results establish the high-temperature QSHE and open a new realm for the discovery of topological phases based on 2D crystals.

cond-mat.mes-hall↗

arXiv2017

Ligand-field helical luminescence in a 2D ferromagnetic insulator

Bulk chromium triiodide (CrI$_3$) has long been known as a layered van der Waals ferromagnet. However, its monolayer form was only recently isolated and confirmed to be a truly two-dimensional (2D) ferromagnet, providing a new platform for investigating light-matter interactions and magneto-optical phenomena in the atomically thin limit. Here, we report spontaneous circularly polarized photoluminescence in monolayer CrI$_3$ under linearly polarized excitation, with helicity determined by the monolayer magnetization direction. In contrast, the bilayer CrI$_3$ photoluminescence exhibits vanishing circular polarization, supporting the recently uncovered anomalous antiferromagnetic interlayer coupling in CrI$_3$ bilayers. Distinct from the Wannier-Mott excitons that dominate the optical response in well-known 2D van der Waals semiconductors, our absorption and layer-dependent photoluminescence measurements reveal the importance of ligand-field and charge-transfer transitions to the optoelectronic response of atomically thin CrI$_3$. We attribute the photoluminescence to a parity-forbidden d-d transition characteristic of Cr$^{3+}$ complexes, which displays broad linewidth due to strong vibronic coupling and thickness-independent peak energy due to its localized molecular orbital nature.

cond-mat.mes-hall↗

arXiv2017

Direct optical detection of Weyl fermion chirality in a topological semimetal

A Weyl semimetal (WSM) is a novel topological phase of matter, in which Weyl fermions (WFs) arise as pseudo-magnetic monopoles in its momentum space. The chirality of the WFs, given by the sign of the monopole charge, is central to the Weyl physics, since it directly serves as the sign of the topological number and gives rise to exotic properties such as Fermi arcs and the chiral anomaly. Despite being the defining property of a WSM, the chirality of the WFs has never been experimentally measured. Here, we directly detect the chirality of the WFs by measuring the photocurrent in response to circularly polarized mid-infrared light. The resulting photocurrent is determined by both the chirality of WFs and that of the photons. Our results pave the way for realizing a wide range of theoretical proposals for studying and controlling the WFs and their associated quantum anomalies by optical and electrical means. More broadly, the two chiralities, analogous to the two valleys in 2D materials, lead to a new degree of freedom in a 3D crystal with potential novel pathways to store and carry information.

cond-mat.mtrl-sci↗

arXiv2017

Relative efficiency of polariton emission in two-dimensional materials

We investigated emission and propagation of polaritons in a two dimensional van der Waals material hexagonal boron nitride (hBN). Our specific emphasis in this work is on hyperbolic phonon polariton emission that we investigated by means of scattering-type scanning near-field optical microscopy. Real-space nano-images detail how the polaritons are launched in several common arrangements including: light scattering by the edges of the crystal, metallic nanostructures deposited on the surface of hBN crystals, as well as random defects and impurities. Notably, the scanned tip of the near-field microscope is itself an efficient polariton launcher. Our analysis reveals that the scanning tips are superior to other types of emitters we have investigated. Furthermore, the study of polariton emission and emission efficiency may provide insights for development of polaritonic devices and for fundamental studies of collective modes in other van der Waals materials.

cond-mat.mes-hall↗

arXiv2017

Tunnelling Spectroscopy of Andreev States in Graphene

A normal conductor placed in good contact with a superconductor can inherit its remarkable electronic properties. This proximity effect microscopically originates from the formation in the conductor of entangled electron-hole states, called Andreev states. Spectroscopic studies of Andreev states have been performed in just a handful of systems. The unique geometry, electronic structure and high mobility of graphene make it a novel platform for studying Andreev physics in two dimensions. Here we use a full van der Waals heterostructure to perform tunnelling spectroscopy measurements of the proximity effect in superconductor-graphene-superconductor junctions. The measured energy spectra, which depend on the phase difference between the superconductors, reveal the presence of a continuum of Andreev bound states. Moreover, our device heterostructure geometry and materials enable us to measure the Andreev spectrum as a function of the graphene Fermi energy, showing a transition between different mesoscopic regimes. Furthermore, by experimentally introducing a novel concept, the supercurrent spectral density, we determine the supercurrent-phase relation in a tunnelling experiment, thus establishing the connection between Andreev physics at finite energy and the Josephson effect. This work opens up new avenues for probing exotic topological phases of matter in hybrid superconducting Dirac materials.

cond-mat.mes-hall↗

arXiv2017

Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit

Since the celebrated discovery of graphene, the family of two-dimensional (2D) materials has grown to encompass a broad range of electronic properties. Recent additions include spin-valley coupled semiconductors, Ising superconductors that can be tuned into a quantum metal, possible Mott insulators with tunable charge-density waves, and topological semi-metals with edge transport. Despite this progress, there is still no 2D crystal with intrinsic magnetism, which would be useful for many technologies such as sensing, information, and data storage. Theoretically, magnetic order is prohibited in the 2D isotropic Heisenberg model at finite temperatures by the Mermin-Wagner theorem. However, magnetic anisotropy removes this restriction and enables, for instance, the occurrence of 2D Ising ferromagnetism. Here, we use magneto-optical Kerr effect (MOKE) microscopy to demonstrate that monolayer chromium triiodide (CrI3) is an Ising ferromagnet with out-of-plane spin orientation. Its Curie temperature of 45 K is only slightly lower than the 61 K of the bulk crystal, consistent with a weak interlayer coupling. Moreover, our studies suggest a layer-dependent magnetic phase transition, showcasing the hallmark thickness-dependent physical properties typical of van der Waals crystals. Remarkably, bilayer CrI3 displays suppressed magnetization with a metamagnetic effect, while in trilayer the interlayer ferromagnetism observed in the bulk crystal is restored. Our work creates opportunities for studying magnetism by harnessing the unique features of atomically-thin materials, such as electrical control for realizing magnetoelectronics, and van der Waals engineering for novel interface phenomena.

cond-mat.mes-hall↗

arXiv2017

Mach-Zehnder interferometry using spin- and valley-polarized quantum Hall edge states in graphene

Confined to a two-dimensional plane, electrons in a strong magnetic field travel along the edge in one-dimensional quantum Hall channels that are protected against backscattering. These channels can be used as solid-state analogues of monochromatic beams of light, providing a unique platform for studying electron interference. Electron interferometry is regarded as one of the most promising routes for studying fractional and non-Abelian statistics and quantum entanglement via two-particle interference. However, creating an edge-channel interferometer in which electron-electron interactions play an important role requires a clean system and long phase coherence lengths. Here we realize electronic Mach-Zehnder interferometers with record visibilities of up to 98% using spin- and valley-polarized edge channels that co-propagate along a PN junction in graphene. We find that inter-channel scattering between same-spin edge channels along the physical graphene edge can be used to form beamsplitters, while the absence of inter-channel scattering along gate-defined interfaces can be used to form isolated interferometer arms. Surprisingly, our interferometer is robust to dephasing effects at energies an order of magnitude larger than observed in pioneering experiments on GaAs/AlGaAs quantum wells. Our results shed light on the nature of edge-channel equilibration and open up new possibilities for studying exotic electron statistics and quantum phenomena.

cond-mat.mes-hall↗

arXiv2017

Magnetoresistance and Quantum Oscillations of an Electrostatically Tuned Semimetal-to-Metal Transition in Ultra-Thin WTe2

We report on electronic transport measurements of electrostatically gated nano-devices of the semimetal WTe\textsubscript{2}. High mobility metallic behavior is achieved in the 2D limit by encapsulating thin flakes in an inert atmosphere. At low temperatures, we find that a large magnetoresistance can be turned on and off by electrostatically doping the system between a semimetallic state and an electron-only metallic state, respectively. We confirm the nature of the two regimes by analyzing the magnetoresistance and Hall effect with a two-carrier model, as well as by analysis of Shubnikov-de Haas oscillations, both of which indicate depletion of hole carriers via the electrostatic gate. This confirms that semiclassical transport of two oppositely charged carriers accurately describes the exceptional magnetoresistance observed in this material. Finally, we also find that the magnetoresistance power law is sub-quadratic and density-independent, suggesting new physics specifically in the semimetallic regime.

cond-mat.mes-hall↗

arXiv2016

Tunable and high purity room-temperature single photon emission from atomic defects in hexagonal boron nitride

Two-dimensional van der Waals materials have emerged as promising platforms for solid-state quantum information processing devices with unusual potential for heterogeneous assembly. Recently, bright and photostable single photon emitters were reported from atomic defects in layered hexagonal boron nitride (hBN), but controlling inhomogeneous spectral distribution and reducing multi-photon emission presented open challenges. Here, we demonstrate that strain control allows spectral tunability of hBN single photon emitters over 6 meV, and material processing sharply improves the single-photon purity. We report high single photon count rates exceeding 10^7 counts/sec at saturation, which is the highest single photon detection rate for room-temperature single photon emitters, to our knowledge. Furthermore, these emitters are stable to material transfer to other substrates. High-purity and photostable single photon emission at room temperature, together with spectral tunability and transferability, opens the door to scalable integration of high-quality quantum emitters in photonic quantum technologies.

cond-mat.mes-hall↗

arXiv2016

Self-aligned local electrolyte gating of 2D materials with nanoscale resolution

In the effort to make 2D materials-based devices smaller, faster, and more efficient, it is important to control charge carrier at lengths approaching the nanometer scale. Traditional gating techniques based on capacitive coupling through a gate dielectric cannot generate strong and uniform electric fields at this scale due to divergence of the fields in dielectrics. This field divergence limits the gating strength, boundary sharpness, and pitch size of periodic structures, and restricts possible geometries of local gates (due to wire packaging), precluding certain device concepts, such as plasmonics and transformation optics based on metamaterials. Here we present a new gating concept based on a dielectric-free self-aligned electrolyte technique that allows spatially modulating charges with nanometer resolution. We employ a combination of a solid-polymer electrolyte gate and an ion-impenetrable e-beam-defined resist mask to locally create excess charges on top of the gated surface. Electrostatic simulations indicate high carrier density variations of $Δn =10^{14}\text{cm}^{-2}$ across a length of 10 nm at the mask boundaries on the surface of a 2D conductor, resulting in a sharp depletion region and a strong in-plane electric field of $6\times10^8 \text{Vm}^{-1}$ across the so-created junction. We apply this technique to the 2D material graphene to demonstrate the creation of tunable p-n junctions for optoelectronic applications. We also demonstrate the spatial versatility and self-aligned properties of this technique by introducing a novel graphene thermopile photodetector.

cond-mat.mes-hall↗

arXiv2016

Direct measurement of proximity-induced magnetism at the interface between a topological insulator and a ferromagnet

When a topological insulator (TI) is in contact with a ferromagnet, both time reversal and inversion symmetries are broken at the interface. An energy gap is formed at the TI surface, and its electrons gain a net magnetic moment through short-range exchange interactions. Magnetic TIs can host various exotic quantum phenomena, such as massive Dirac fermions, Majorana fermions, the quantum anomalous Hall effect and chiral edge currents along the domain boundaries. However, selective measurement of induced magnetism at the buried interface has remained a challenge. Using magnetic second harmonic generation, we directly probe both the in-plane and out-of-plane magnetizations induced at the interface between the ferromagnetic insulator (FMI) EuS and the three-dimensional TI Bi2Se3. Our findings not only allow characterizing magnetism at the TI-FMI interface but also lay the groundwork for imaging magnetic domains and domain boundaries at the magnetic TI surfaces.

cond-mat.mes-hall↗

arXiv2016

Landau level splittings, phase transitions, and non-uniform charge distribution in trilayer graphene

We report on magneto-transport studies of dual-gated, Bernal-stacked trilayer graphene (TLG) encapsulated in boron nitride crystals. We observe a quantum Hall effect staircase which indicates a complete lifting of the twelve-fold degeneracy of the zeroth Landau level. As a function of perpendicular electric field, our data exhibits a sequence of phase transitions between all integer quantum Hall states in the filling factor interval $-8<ν<0$. We develop a theoretical model and argue that, in contrast to monolayer and bilayer graphene, the observed Landau level splittings and quantum Hall phase transitions can be understood within a single-particle picture, but imply the presence of a charge density imbalance between the inner and outer layers of TLG, even at charge neutrality and zero transverse electric field. Our results indicate the importance of a previously unaccounted band structure parameter which, together with a more accurate estimate of the other tight-binding parameters, results in a significantly improved determination of the electronic and Landau level structure of TLG.

cond-mat.mes-hall↗

arXiv2016

Tuning ultrafast electron thermalization pathways in a van der Waals heterostructure

Ultrafast electron thermalization - the process leading to Auger recombination, carrier multiplication via impact ionization and hot carrier luminescence - occurs when optically excited electrons in a material undergo rapid electron-electron scattering to redistribute excess energy and reach electronic thermal equilibrium. Due to extremely short time and length scales, the measurement and manipulation of electron thermalization in nanoscale devices remains challenging even with the most advanced ultrafast laser techniques. Here, we overcome this challenge by leveraging the atomic thinness of two-dimensional van der Waals (vdW) materials in order to introduce a highly tunable electron transfer pathway that directly competes with electron thermalization. We realize this scheme in a graphene-boron nitride-graphene (G-BN-G) vdW heterostructure, through which optically excited carriers are transported from one graphene layer to the other. By applying an interlayer bias voltage or varying the excitation photon energy, interlayer carrier transport can be controlled to occur faster or slower than the intralayer scattering events, thus effectively tuning the electron thermalization pathways in graphene. Our findings, which demonstrate a novel means to probe and directly modulate electron energy transport in nanoscale materials, represent an important step toward designing and implementing novel optoelectronic and energy-harvesting devices with tailored microscopic properties.

cond-mat.mes-hall↗