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James Hone

Publications and source records attributed to James Hone.

At least 55 records · Page 3Linked to original sources

Ultra Localized Optoelectronic Properties of Nanobubbles in 2D Semiconductors

The optical properties of transition metal dichalcogenides have previously been modified at the nanoscale by using mechanical and electrical nanostructuring. However, a clear experimental picture relating the local electronic structure with emission properties in such structures has so far been lacking. Here, we use a combination of scanning tunneling microscopy (STM) and near-field photoluminescence (nano-PL) to probe the electronic and optical properties of single nano-bubbles in bilayer heterostructures of WSe2 on MoSe2. We show from tunneling spectroscopy that there are electronic states deeply localized in the gap at the edge of such bubbles, which are independent of the presence of chemical defects in the layers. We also show a significant change in the local bandgap on the bubble, with a continuous evolution to the edge of the bubble over a length scale of ~20 nm. Nano-PL measurements observe a continuous redshift of the interlayer exciton on entering the bubble, in agreement with the band to band transitions measured by STM. We use self-consistent Schrödinger-Poisson (SP) simulations to capture the essence of the experimental results and find that strong doping in the bubble region is a key ingredient to achieving the observed localized states, together with mechanical strain.

cond-mat.mes-hall↗

Quadrupolar excitons in a tunnel-coupled van der Waals heterotrilayer

Strongly bound excitons and many-body interactions between them determine light-matter interactions in van der Waals (vdW) heterostructures of 2D semiconductors. Unlike fundamental particles, quasiparticles in condensed matter, such as excitons, can be tailored to alter their interactions and realize emergent quantum phases. Here, using a WS$_2$/WSe$_2$/WS$_2$ heterotrilayer, we create a quantum superposition of oppositely oriented dipolar excitons - a quadrupolar exciton - wherein an electron is layer-hybridized in WS$_2$ layers while the hole localizes in WSe$_2$. In contrast to dipolar excitons, symmetric quadrupolar excitons only redshift in an out-of-plane electric field, consistent with ab initio calculations, regaining dipolar characteristics at higher fields. Electric field tunes the hybridization and allows for lifetime control through modification of the excitonic wavefunction. Lack of density-dependent blue shift of heterotrilayer excitons compared to dipolar excitons is consistent with quadrupolar interactions. Our results present vdW heterotrilayers as a field-tunable platform to engineer light-matter interactions and explore quantum phase transitions between spontaneously ordered many-exciton phases.

cond-mat.mes-hall↗

Electron spin resonance and collective excitations in magic-angle twisted bilayer graphene

In a strongly correlated system, collective excitations contain key information regarding the electronic order of the underlying ground state. An abundance of collective modes in the spin and valley isospin channels of magic-angle graphene moiré bands has been alluded to by a series of recent experiments. However, direct observation of collective excitations has remained elusive due to the lack of a spin probe. In this work, we use a resistively-detected electron spin resonance technique to look for low-energy collective excitations in magic-angle twisted bilayer graphene. We report direct observation of collective modes in the form of microwave-induced resonance near half filling of the moiré flatbands. The frequency-magnetic field dependence of these resonance modes sheds light onto the nature of intervalley spin coupling, allowing us to extract parameters such as intervalley exchange interaction and spin stiffness. Two independent observations testify that the generation and detection of the microwave resonance relies on the strong correlation within the flat moiré energy band. First, the onset of robust resonance response coincides with the spontaneous flavor polarization at half moiré filling, and remains absent in the density range where the underlying Fermi surface is isospin unpolarized. Second, we performed the same resonance measurement on graphene monolayer and bilayer samples, including twisted bilayer with a large twist angle, where flatband physics is absent. We observe no indication of resonance response in these samples across a large range of carrier density, microwave frequency and power. A natural explanation is that the resonance response near the magic angle originates from "Dirac revivals" and the resulting isospin order.

cond-mat.mes-hall↗

P-type Ohmic contact to monolayer WSe2 field-effect transistors using high electron affinity amorphous MoO3

1 School of Physics and Astronomy, Monash University, Clayton, Victoria 3800, Australia 2 Australian Research Council Centre of Excellence in Future Low-Energy Electronics Technologies (FLEET), Monash University, Clayton, Victoria 3800, Australia 3 Department of Mechanical Engineering, Columbia University, New York, New York 10027, United States 4 Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, United States 5 School of Physics, the University of Melbourne, Melbourne, VIC 3010, Australia 6 Research Center for Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan 7 International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan 8 School of Physics, University of New South Wales, 2052 Sydney, Australia 9 Center of Condensed Matter Sciences and Center of Atomic Initiative for New Material, National Taiwan University, Taipei 106, Taiwan 10 Monash Centre for Atomically Thin Materials, Monash University, Clayton, 3800, VIC, Australia

cond-mat.mes-hall↗

Unzipping hBN with ultrashort mid-infrared pulses

Manipulating the nanostructure of materials is critical for numerous applications in electronics, magnetics, and photonics. However, conventional methods such as lithography and laser-writing require cleanroom facilities or leave residue. Here, we describe a new approach to create atomically sharp line defects in hexagonal boron nitride (hBN) at room temperature by direct optical phonon excitation in the mid-infrared (mid-IR). We term this phenomenon "unzipping" to describe the rapid formation and growth of a <30-nm-wide crack from a point within the laser-driven region. The formation of these features is attributed to large atomic displacements and high local bond strain from driving the crystal at a natural resonance. This process is distinguished by (i) occurring only under resonant phonon excitation, (ii) producing highly sub-wavelength features, and (iii) sensitivity to crystal orientation and pump laser polarization. Its cleanliness, directionality, and sharpness enable applications in in-situ flake cleaving and phonon-wave-coupling via free space optical excitation.

cond-mat.mtrl-sci↗

Miniaturizing transmon qubits using van der Waals materials

Quantum computers can potentially achieve an exponential speedup versus classical computers on certain computational tasks, as recently demonstrated in systems of superconducting qubits. However, these qubits have large footprints due to their large capacitor electrodes needed to suppress losses by avoiding dielectric materials. This tactic hinders scaling by increasing parasitic coupling among circuit components, degrading individual qubit addressability, and limiting the spatial density of qubits. Here, we take advantage of the unique properties of the van der Waals (vdW) materials to reduce the qubit area by a factor of $>1000$ while preserving the required capacitance without increasing substantial loss. Our qubits combine conventional aluminum-based Josephson junctions with parallel-plate capacitors composed of crystalline layers of superconducting niobium diselenide (NbSe$_2$) and insulating hexagonal-boron nitride (hBN). We measure a vdW transmon $T_1$ relaxation time of 1.06 $μ$s, which demonstrates a path to achieve high-qubit-density quantum processors with long coherence times, and illustrates the broad utility of layered heterostructures in low-loss, high-coherence quantum devices.

quant-ph↗

Tunable and giant valley-selective Hall effect in gapped bilayer graphene

Berry curvature is analogous to magnetic field but in momentum space and is commonly present in materials with non-trivial quantum geometry. It endows Bloch electrons with transverse anomalous velocities to produce Hall-like currents even in the absence of a magnetic field. We report the direct observation of in situ tunable valley-selective Hall effect (VSHE), where inversion symmetry, and thus the geometric phase of electrons, is controllable by an out-of-plane electric field. We use high-quality bilayer graphene with an intrinsic and tunable bandgap, illuminated by circularly polarized mid-infrared light and confirm that the observed Hall voltage arises from an optically-induced valley population. Compared with molybdenum disulfide, we find orders of magnitude larger VSHE, attributed to the inverse scaling of the Berry curvature with bandgap. By monitoring the valley-selective Hall conductivity, we study Berry curvature's evolution with bandgap. This in situ manipulation of VSHE paves the way for topological and quantum geometric opto-electronic devices, such as more robust switches and detectors.

cond-mat.mes-hall↗

Frustrated magnetic interactions in a Wigner-Mott insulator

Two-dimensional semiconductor moiré materials have emerged as a highly controllable platform to simulate and explore quantum condensed matter. Compared to real solids, electrons in semiconductor moiré materials are less strongly attracted to the moiré lattice sites, making the nonlocal contributions to the magnetic interactions as important as the Anderson super-exchange. It provides a unique platform to study the effects of competing magnetic interactions. Here, we report the observation of strongly frustrated magnetic interactions in a Wigner-Mott insulating state at 2/3 filling of the moiré lattice in angle-aligned WSe2/WS2 heterobilayers. Magneto-optical measurements show that the net exchange interaction is antiferromagnetic for filling factors below 1 with a strong suppression at 2/3 filling. The suppression is lifted upon screening of the long-range Coulomb interactions and melting of the Wigner-Mott insulator by a nearby metallic gate. The results can be qualitatively captured by a honeycomb-lattice spin model with an antiferromagnetic nearest-neighbor coupling and a ferromagnetic second-neighbor coupling. Our study establishes semiconductor moiré materials as a model system for the lattice-spin physics and frustrated magnetism.

cond-mat.mtrl-sci↗

Dissipation-enabled hydrodynamic conductivity in a tunable bandgap semiconductor

Electronic transport in the regime where carrier-carrier collisions are the dominant scattering mechanism has taken on new relevance with the advent of ultraclean two-dimensional materials. Here we present a combined theoretical and experimental study of ambipolar hydrodynamic transport in bilayer graphene demonstrating that the conductivity is given by the sum of two Drude-like terms that describe relative motion between electrons and holes, and the collective motion of the electron-hole plasma. As predicted, the measured conductivity of gapless, charge-neutral bilayer graphene is sample- and temperature-independent over a wide range. Away from neutrality, the electron-hole conductivity collapses to a single curve, and a set of just four fitting parameters provides quantitative agreement between theory and experiment at all densities, temperatures, and gaps measured. This work validates recent theories for dissipation-enabled hydrodynamic conductivity and creates a link between semiconductor physics and the emerging field of viscous electronics.

cond-mat.mes-hall↗

A new flavor of correlation and superconductivity in small twist-angle trilayer graphene

When layers of graphene are rotationally misaligned by the magic angle, the moiré superlattice features extremely flat bands. Due to the enhanced density of states, the Coulomb interaction induces a variety of instabilities. The most prominent occur at integer filling and are therefore commonly attributed to spontaneous polarization of the moiré unit cell's `flavor' degrees of freedom -- spin, valley, and the flat-band degeneracy. As the dominant member of the hierarchy, these correlated states are thought to crucially determine further instabilities at lower energy scales, such as superconductivity and weaker incompressible states at fractional filling. In this work, we examine the behavior of twisted trilayer graphene in a window of twist angle around $1.3^{\circ}$, well below the expected magic angle of $1.55^{\circ}$. In this small twist angle regime, we find surprisingly narrow bands, which are populated with both an abundance of correlation-driven states at fractional filling as well as robust superconductivity. The absence of linear-in-$T$ resistivity without significant reduction of the superconducting transition temperature, provides insights into the origin of both phenomena. Most remarkably, the hierarchy between integer and fractional filling is absent, indicating that flavor polarization does not play a governing role. The prominence of fractional filling in the small twist angle regime also points towards a longer-range effective Coulomb interaction. Combined, our results shed new light on outstanding questions in the field, while establishing the small twist angle regime as a new paradigm for exploring novel flavors of moiré physics.

cond-mat.mes-hall↗

Zero-field superconducting diode effect in small-twist-angle trilayer graphene

The critical current of a superconductor can be different for opposite directions of current flow when both time-reversal and inversion symmetry are broken. %When time-reversal and inversion symmetry are simultaneously broken, the critical current of a 2D superconductor is expected to depend on the directions of current flow. Such nonreciprocal behavior in superconducting transport, which creates a superconducting diode, has recently been demonstrated experimentally by breaking these symmetries with an applied magnetic field \cite{Ando2020diodes} or by construction of a magnetic tunnel junction \cite{Diez2021magnetic}. Here we report an intrinsic superconducting diode effect which is present at zero external magnetic field in mirror symmetric twisted trilayer graphene (tTLG). Such nonreciprocal behavior, with sign that can be reversed through training with an out-of-plane magnetic field, provides direct evidence of the microscopic coexistence between superconductivity and time-reversal symmetry breaking. In addition to the magnetic-field trainability, we show that the zero-field diode effect can be controlled by varying carrier density or twist angle. In accordance with these experimental controls, a natural interpretation for the origin of the intrinsic diode effect is an imbalance in valley occupation of the underlying Fermi surface, which likely leads to finite-momentum Cooper pairing and nematicity in the superconducting phase.

cond-mat.mes-hall↗

Dark-exciton driven energy funneling into dielectric inhomogeneities in two-dimensional semiconductors

The optoelectronic and transport properties of two-dimensional transition metal dichalcogenide semiconductors (2D TMDs) are highly susceptible to external perturbation, enabling precise tailoring of material function through post-synthetic modifications. Here we show that nanoscale inhomogeneities known as nanobubbles can be used for both strain and, less invasively, dielectric tuning of exciton transport in bilayer tungsten disulfide (WSe2). We use ultrasensitive spatiotemporally resolved optical scattering microscopy to directly image exciton transport, revealing that dielectric nanobubbles are surprisingly efficient at funneling and trapping excitons at room temperature, even though the energies of the bright excitons are negligibly affected. Our observations suggest that exciton funneling in dielectric inhomogeneities is driven by momentum-indirect (dark) excitons whose energies are more sensitive to dielectric perturbations than bright excitons. These results reveal a new pathway to control exciton transport in 2D semiconductors with exceptional spatial and energetic precision using dielectric engineering of dark state energetic landscapes.

cond-mat.mes-hall↗

Making high-quality quantum microwave devices with van der Waals superconductors

Ultra low-loss microwave materials are crucial for enhancing quantum coherence and scalability of superconducting qubits. Van der Waals (vdW) heterostructure is an attractive platform for quantum devices due to the single-crystal structure of the constituent two-dimensional (2D) layered materials and the lack of dangling bonds at their atomically sharp interfaces. However, new fabrication and characterization techniques are required to determine whether these structures can achieve low loss in the microwave regime. Here we report the fabrication of superconducting microwave resonators using NbSe$_2$ that achieve a quality factor $Q > 10^5$. This value sets an upper bound that corresponds to a resistance of $\leq 192 μΩ$ when considering the additional loss introduced by integrating NbSe$_2$ into a standard transmon circuit. This work demonstrates the compatibility of 2D layered materials with high-quality microwave quantum devices.

cond-mat.supr-con↗

Disorder of Excitons and Trions in Monolayer MoSe2

The optical spectra of transition metal dichalcogenide (TMDC) monolayers are dominated by excitons and trions. Here we establish the dependences of these optical transitions on disorder from hyperspectral imaging of h-BN encapsulated monolayer MoSe2. While both exciton and trion energies vary spatially, these two quantities are almost perfectly correlated, with spatial variation in the trion binding energy of only ~0.18 meV. In contrast, variation in the energy splitting between the two lowest energy exciton states is one order of magnitude larger at ~1.7 meV. Statistical analysis and theoretical modeling reveal that disorder results from dielectric and bandgap fluctuations, not electrostatic fluctuations. Our results shed light on disorder in high quality TMDC monolayers, its impact on optical transitions, and the many-body nature of excitons and trions.

cond-mat.mes-hall↗

Andreev Reflections in NbN/graphene Junctions under Large Magnetic Fields

Hybrid superconductor/graphene (SC/g) junctions are excellent candidates for investigating correlations between Cooper pairs and quantum Hall (QH) edge modes. Experimental studies are challenging as Andreev reflections are extremely sensitive to junction disorder and high magnetic fields are required to form QH edge states. We fabricated low-resistance SC/g interfaces, composed of graphene edge contacted with NbN with a barrier strength of $Z\approx 0.4$, that remain superconducting under magnetic fields larger than $18$ T. We establish the role of graphene's Dirac band structure on zero-field Andreev reflections and demonstrate dynamic tunability of the Andreev reflection spectrum by moving the boundary between specular and retro Andreev reflections with parallel magnetic fields. Through the application of perpendicular magnetic fields, we observe an oscillatory suppression of the 2-probe conductance in the $ν= 4$ Landau level attributed to the reduced efficiency of Andreev processes at the NbN/g interface, consistent with theoretical predictions.

cond-mat.mes-hall↗

Bilayer WSe$_2$ as a natural platform for interlayer exciton condensates in the strong coupling limit

Exciton condensates (EC) are macroscopic coherent states arising from condensation of electron-hole pairs. Bilayer heterostructures, consisting of two-dimensional electron and hole layers separated by a tunnel barrier, provide a versatile platform to realize and study EC. The tunnel barrier suppresses recombination yielding long-lived excitons. However, this separation also reduces interlayer Coulomb interactions, limiting the exciton binding strength. Here, we report the observation of EC in naturally occurring 2H-stacked bilayer WSe$_2$. In this system, the intrinsic spin-valley structure suppresses interlayer tunneling even when the separation is reduced to the atomic limit, providing access to a previously unattainable regime of strong interlayer coupling. Using capacitance spectroscopy, we investigate magneto-EC, formed when partially filled Landau levels (LL) couple between the layers. We find that the strong-coupling EC show dramatically different behaviour compared with previous reports, including an unanticipated variation of the EC robustness with the orbital number, and find evidence for a transition between two types of low-energy charged excitations. Our results provide a demonstration of tuning EC properties by varying the constituent single-particle wavefunctions.

cond-mat.mes-hall↗

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↗

Spin-orbit driven ferromagnetism at half moiré filling in magic-angle twisted bilayer graphene

Strong electron correlation and spin-orbit coupling (SOC) provide two non-trivial threads to condensed matter physics. When these two strands of physics come together, a plethora of quantum phenomena with novel topological order have been predicted to emerge in the correlated SOC regime. In this work, we examine the combined influence of electron correlation and SOC on a 2-dimensional (2D) electronic system at the atomic interface between magic-angle twisted bilayer graphene (tBLG) and a tungsten diselenide (\WSe) crystal. In such a structure, strong electron correlation within the moiré flatband stabilizes correlated insulating states at both quarter and half-filling, whereas SOC transforms these Mott-like insulators into ferromagnets, evidenced by robust anomalous Hall effect with hysteretic switching behavior. The coupling between spin and valley degrees of freedom is unambiguously demonstrated as the magnetic order is shown to be tunable with an in-plane magnetic field, or a perpendicular electric field. In addition, we examine the influence of SOC on the isospin order and stability of superconductivity. Our findings establish an efficient experimental knob to engineer topological properties of moiré bands in twisted bilayer graphene and related systems.

cond-mat.mes-hall↗