arXiv subjects

James Hone

Publications and source records attributed to James Hone.

At least 37 records · Page 2Linked to original sources

arXiv2024

Real-Space Imaging of the Band Topology of Transition Metal Dichalcogenides

The topological properties of Bloch bands are intimately tied to the structure of their electronic wavefunctions within the unit cell of a crystal. Here, we show that scanning tunneling microscopy (STM) measurements on the prototypical transition metal dichalcogenide (TMD) semiconductor WSe$_2$ can be used to unambiguously fix the location of the Wannier center of the valence band. Using site-specific substitutional doping, we first determine the position of the atomic sites within STM images, establishing that the maximum electronic density of states at the $K$-point lies between the atoms. In contrast, the maximum density of states at the $Γ$ point is at the atomic sites. This signifies that WSe$_2$ is a topologically obstructed atomic insulator, which cannot be adiabatically transformed to the trivial atomic insulator limit.

cond-mat.mtrl-sci↗

arXiv2024

Measuring kinetic inductance and superfluid stiffness of two-dimensional superconductors using high-quality transmission-line resonators

The discovery of van der Waals superconductors in recent years has generated a lot of excitement for their potentially novel pairing mechanisms. However, their typical atomic-scale thickness and micrometer-scale lateral dimensions impose severe challenges to investigations of pairing symmetry by conventional methods. In this report we demonstrate a new technique that employs high-quality-factor superconducting resonators to measure the kinetic inductance -- up to a part per million -- and loss of a van der Waals superconductor. We analyze the equivalent circuit model to extract the kinetic inductance, superfluid stiffness, penetration depth, and ratio of imaginary and real parts of the complex conductivity. We validate the technique by measuring aluminum and finding excellent agreement in both the zero-temperature superconducting gap as well as the complex conductivity data when compared with BCS theory. We then demonstrate the utility of the technique by measuring the kinetic inductance of multi-layered niobium diselenide and discuss the limits to the accuracy of our technique when the transition temperature of the sample, NbSe$_2$ at 7.06 K, approaches our Nb probe resonator at 8.59 K. Our method will be useful for practitioners in the growing fields of superconducting physics, materials science, and quantum sensing, as a means of characterizing superconducting circuit components and studying pairing mechanisms of the novel superconducting states which arise in layered 2D materials and heterostructures.

cond-mat.supr-con↗

arXiv2024

Moiré exciton polaron engineering via twisted hBN

Twisted hexagonal boron nitride (thBN) exhibits emergent ferroelectricity due to the formation of moiré superlattices with alternating AB and BA domains. These domains possess electric dipoles, leading to a periodic electrostatic potential that can be imprinted onto other 2D materials placed in its proximity. Here we demonstrate the remote imprinting of moiré patterns from twisted hexagonal boron nitride (thBN) onto monolayer MoSe2 and investigate the resulting changes in the exciton properties. We confirm the imprinting of moiré patterns on monolayer MoSe2 via proximity using Kelvin probe force microscopy (KPFM) and hyperspectral photoluminescence (PL) mapping. By developing a technique to create large ferroelectric domain sizes ranging from 1 μm to 8.7 μm, we achieve unprecedented potential modulation of 387 +- 52 meV. We observe the formation of exciton polarons due to charge redistribution caused by the antiferroelectric moiré domains and investigate the optical property changes induced by the moiré pattern in monolayer MoSe2 by varying the moiré pattern size down to 110 nm. Our findings highlight the potential of twisted hBN as a platform for controlling the optical and electronic properties of 2D materials for optoelectronic and valleytronic applications.

cond-mat.mtrl-sci↗

arXiv2024

Dynamical Control of Excitons in Atomically Thin Semiconductors

Excitons in transition metal dichalcogenides (TMDs) have emerged as a promising platform for novel applications ranging from optoelectronic devices to quantum optics and solid state quantum simulators. While much progress has been made towards characterizing and controlling excitons in TMDs, manipulating their properties during the course of their lifetime - a key requirement for many optoelectronic device and information processing modalities - remains an outstanding challenge. Here we combine long-lived interlayer excitons in angle-aligned MoSe$_2$/WSe$_2$ heterostructures with fast electrical control to realize dynamical control schemes, in which exciton properties are not predetermined at the time of excitation but can be dynamically manipulated during their lifetime. Leveraging the out-of-plane exciton dipole moment, we use electric fields to demonstrate dynamical control over the exciton emission wavelength. Moreover, employing a patterned gate geometry, we demonstrate rapid local sample doping and toggling of the radiative decay rate through exciton-charge interactions during the exciton lifetime. Spatially mapping the exciton response reveals charge redistribution, offering a novel probe of electronic transport in twisted TMD heterostructures. Our results establish the feasibility of dynamical exciton control schemes, unlocking new directions for exciton-based information processing and optoelectronic devices, and the realization of excitonic phenomena in TMDs.

cond-mat.mes-hall↗

arXiv2024

Electronic interactions in Dirac fluids visualized by nano-terahertz spacetime interference of electron-photon quasiparticles

Ultraclean graphene at charge neutrality hosts a quantum critical Dirac fluid of interacting electrons and holes. Interactions profoundly affect the charge dynamics of graphene, which is encoded in the properties of its electron-photon collective modes: surface plasmon polaritons (SPPs). Here we show that polaritonic interference patterns are particularly well suited to unveil the interactions in Dirac fluids by tracking polaritonic interference in time at temporal scales commensurate with the electronic scattering. Spacetime SPP interference patterns recorded in tera-hertz (THz) frequency range provided unobstructed readouts of the group velocity and lifetime of polariton that can be directly mapped onto the electronic spectral weight and the relaxation rate. Our data uncovered prominent departures of the electron dynamics from the predictions of the conventional Fermi-liquid theory. The deviations are particularly strong when the densities of electrons and holes are approximately equal. The proposed spacetime imaging methodology can be broadly applied to probe the electrodynamics of quantum materials.

cond-mat.str-el↗

arXiv2024

Superconductivity in twisted bilayer WSe$_2$

The discovery of superconductivity in twisted bilayer and twisted trilayer graphene has generated tremendous interest. The key feature of these systems is an interplay between interlayer coupling and a moiré superlattice that gives rise to low-energy flat bands with strong correlations. Flat bands can also be induced by moiré patterns in lattice-mismatched and or twisted heterostructures of other two-dimensional materials such as transition metal dichalcogenides (TMDs). Although a wide range of correlated phenomenon have indeed been observed in the moiré TMDs, robust demonstration of superconductivity has remained absent. Here we report superconductivity in 5 degree twisted bilayer WSe$_2$ (tWSe$_2$) with a maximum critical temperature of 426 mK. The superconducting state appears in a limited region of displacement field and density that is adjacent to a metallic state with Fermi surface reconstruction believed to arise from antiferromagnetic order. A sharp boundary is observed between the superconducting and magnetic phases at low temperature, reminiscent of spin-fluctuation mediated superconductivity. Our results establish that moiré flat-band superconductivity extends beyond graphene structures. Material properties that are absent in graphene but intrinsic among the TMDs such as a native band gap, large spin-orbit coupling, spin-valley locking, and magnetism offer the possibility to access a broader superconducting parameter space than graphene-only structures.

cond-mat.mes-hall↗

arXiv2024

Pick-and-place transfer of arbitrary-metal electrodes for van der Waals device fabrication

Van der Waals electrode integration is a promising strategy to create near-perfect interfaces between metals and two-dimensional materials, with advantages such as eliminating Fermi-level pinning and reducing contact resistance. However, the lack of a simple, generalizable pick-and-place transfer technology has greatly hampered the wide use of this technique. We demonstrate the pick-and-place transfer of pre-fabricated electrodes from reusable polished hydrogenated diamond substrates without the use of any surface treatments or sacrificial layers. The technique enables transfer of large-scale arbitrary metal electrodes, as demonstrated by successful transfer of eight different elemental metals with work functions ranging from 4.22 to 5.65 eV. The mechanical transfer of metal electrodes from diamond onto van der Waals materials creates atomically smooth interfaces with no interstitial impurities or disorder, as observed with cross-sectional high-resolution transmission electron microscopy and energy-dispersive X-ray spectroscopy. As a demonstration of its device application, we use the diamond-transfer technique to create metal contacts to monolayer transition metal dichalcogenide semiconductors with high-work-function Pd, low-work-function Ti, and semi metal Bi to create n- and p-type field-effect transistors with low Schottky barrier heights. We also extend this technology to other applications such as ambipolar transistor and optoelectronics, paving the way for new device architectures and high-performance devices.

physics.app-ph↗

arXiv2024

Hybrid moiré excitons and trions in twisted MoTe$_2$-MoSe$_2$ heterobilayers

We report experimental and theoretical studies of MoTe$_2$-MoSe$_2$ heterobilayers with rigid moiré superlattices controlled by the twist angle. Using an effective continuum model that combines resonant interlayer electron tunneling with stacking-dependent moiré potentials, we identify the nature of moiré excitons and the dependence of their energies, oscillator strengths and Landé $g$-factors on the twist angle. Within the same framework, we interpret distinct signatures of bound complexes among electrons and moiré excitons in nearly collinear heterostacks. Our work provides fundamental understanding of hybrid moiré excitons and trions in MoTe$_2$-MoSe$_2$ heterobilayers, and establishes the material system as a prime candidate for optical studies of correlated phenomena in moiré lattices.

cond-mat.mes-hall↗

arXiv2023

Charge-transfer Contact to a High-Mobility Monolayer Semiconductor

Two-dimensional (2D) semiconductors, such as the transition metal dichalcogenides, have demonstrated tremendous promise for the development of highly tunable quantum devices. Realizing this potential requires low-resistance electrical contacts that perform well at low temperatures and low densities where quantum properties are relevant. Here we present a new device architecture for 2D semiconductors that utilizes a charge-transfer layer to achieve large hole doping in the contact region, and implement this technique to measure magneto-transport properties of high-purity monolayer WSe$_2$. We measure a record-high hole mobility of 80,000 cm$^2$/Vs and access channel carrier densities as low as $1.6\times10^{11}$ cm$^{-2}$, an order of magnitude lower than previously achievable. Our ability to realize transparent contact to high-mobility devices at low density enables transport measurement of correlation-driven quantum phases including observation of a low temperature metal-insulator transition in a density and temperature regime where Wigner crystal formation is expected, and observation of the fractional quantum Hall effect under large magnetic fields. The charge transfer contact scheme paves the way for discovery and manipulation of new quantum phenomena in 2D semiconductors and their heterostructures.

cond-mat.mes-hall↗

arXiv2023

Transport Study of Charge Carrier Scattering in Monolayer WSe$_2$

Employing flux-grown single crystal WSe$_2$, we report charge carrier scattering behaviors measured in $h$-BN encapsulated monolayer field effect transistors. We perform quantum transport measurements across various hole densities and temperatures and observe a non-monotonic change of transport mobility $μ$ as a function of hole density in the degenerately doped sample. This unusual behavior can be explained by energy dependent scattering amplitude of strong defects calculated using the T-matrix approximation. Utilizing long mean-free path ($>$500 nm), we demonstrate the high quality of our electronic devices by showing quantized conductance steps from an electrostatically-defined quantum point contact. Our results show the potential for creating ultra-high quality quantum optoelectronic devices based on atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2023

Evidence for Exciton Crystals in a 2D Semiconductor Heterotrilayer

Two-dimensional (2D) transition metal dichalcogenides (TMDC) and their moiré interfaces have been demonstrated for correlated electron states, including Mott insulators and electron/hole crystals commensurate with moiré superlattices. Here we present spectroscopic evidences for ordered bosons - interlayer exciton crystals in a WSe2/MoSe2/WSe2 trilayer, where the enhanced Coulomb interactions over those in heterobilayers have been predicted to result in exciton ordering. While the dipolar interlayer excitons in the heterobilayer may be ordered by the periodic moiré traps, their mutual repulsion results in de-trapping at exciton density n_ex larger than 10^11 cm^-2 to form mobile exciton gases and further to electron-hole plasmas, both accompanied by broadening in photoluminescence (PL) peaks and large increases in mobility. In contrast, ordered interlayer excitons in the trilayer are characterized by negligible mobility and by sharper PL peaks persisting to n_ex approximately 10^12 cm^-2. We present evidences for the predicted quadrupolar exciton crystal and its transitions to dipolar excitons either with increasing n_ex or by an applied electric field. These ordered interlayer excitons may serve as models for the exploration of quantum phase transitions and quantum coherent phenomena.

cond-mat.mes-hall↗

arXiv2023

Phonon-Enhanced Nonlinearities in Hexagonal Boron Nitride

We investigate optical nonlinearities that are induced and enhanced due to the strong phonon resonance in hexagonal boron nitride. We predict and observe large sub-picosecond duration signals due to four-wave mixing (FWM) during resonant excitation. The resulting FWM signal allows for time-resolved observation of the crystal motion. In addition, we observe enhancements of third-harmonic generation with resonant pumping at the hBN transverse optical phonon. Phonon-induced nonlinear enhancements are also predicted to yield large increases in high-harmonic efficiencies.

physics.optics↗

arXiv2023

Spin-selective magneto-conductivity in WSe$_2$

Material systems that exhibit tunable spin-selective conductivity are key components of spintronic technologies. Here we demonstrate a novel type of spin-selective transport, based on the unusual Landau level (LL) sequence observed in bilayer WSe$_2$ under large applied magnetic fields. We find that the conductivity depends strongly on the relative iso-spin ordering between conducting electrons in a partially filled LL and the localized electrons of lower energy filled LLs, with conductivity observed to be almost completely suppressed when the spin-ratio and field-tuned Coulomb energy exceed a critical threshold. Switching between "on/off" states is achievable through either modulation of the external magnetic or electric fields, with many-body interaction driving a collective switching mechanism. In contrast to magnetoresistive heterostructures, this system achieves electrically tunable spin filtering within a single material, driven by interaction between free and localized spins residing in energy-separated spin/valley polarized bands. Similar spin-selective conductivity may be realizable in multi-flat band systems at zero magnetic field.

cond-mat.mes-hall↗

arXiv2023

Domain-dependent surface adhesion in twisted few-layer graphene: Platform for moiré-assisted chemistry

Twisted van der Waals multilayers are widely regarded as a rich platform to access novel electronic phases, thanks to the multiple degrees of freedom such as layer thickness and twist angle that allow control of their electronic and chemical properties. Here, we propose that the stacking domains that form naturally due to the relative twist between successive layers act as an additional "knob" for controlling the behavior of these systems, and report the emergence and engineering of stacking domain-dependent surface chemistry in twisted few-layer graphene. Using mid-infrared near-field optical microscopy and atomic force microscopy, we observe a selective adhesion of metallic nanoparticles and liquid water at the domains with rhombohedral stacking configurations of minimally twisted double bi- and tri-layer graphene. Furthermore, we demonstrate that the manipulation of nanoparticles located at certain stacking domains can locally reconfigure the moiré superlattice in their vicinity at the μm-scale. In addition, we report first-principles simulations of the energetics of adhesion of metal atoms and water molecules on the stacking domains in an attempt to elucidate the origin of the observed selective adhesion. Our findings establish a new approach to controlling moiré-assisted chemistry and nanoengineering.

cond-mat.mtrl-sci↗

arXiv2023

Two-step flux synthesis of ultrapure transition metal dichalcogenides

Here, we describe synthesis of TMD crystals using a two-step flux growth method that eliminates a major potential source of contamination. Detailed characterization of TMDs grown by this two-step method reveals charged and isovalent defects with densities an order of magnitude lower than in TMDs grown by a single-step flux technique. Initial temperature-dependent electrical transport measurements of monolayer WSe2 yield room-temperature hole mobility above 840 cm2/Vs and low-temperature disorder-limited mobility above 44,000 cm2/Vs. Electrical transport measurements of graphene-WSe2 heterostructures fabricated from the two-step flux grown WSe2 also show superior performance: higher graphene mobility, lower charged impurity density, and well-resolved integer quantum Hall states.

cond-mat.mtrl-sci↗

arXiv2023

Unconventional Nonlocal Relaxation Dynamics in a Twisted Graphene Moire Superlattice

The electronic and structural properties of atomically thin materials can be controllably tuned by assembling them with an interlayer twist. During this process, constituent layers spontaneously rearrange themselves in search of a lowest energy configuration. Such relaxation phenomena can lead to unexpected and novel material properties. Here, we study twisted double trilayer graphene (TDTG) using nano-optical and tunneling spectroscopy tools. We reveal a surprising optical and electronic contrast, as well as a stacking energy imbalance emerging between the moiré domains. We attribute this contrast to an unconventional form of lattice relaxation in which an entire graphene layer spontaneously shifts position during fabrication. We analyze the energetics of this transition and demonstrate that it is the result of a non-local relaxation process, in which an energy gain in one domain of the moire lattice is paid for by a relaxation that occurs in the other.

cond-mat.mes-hall↗

arXiv2022

2D material platform for overcoming the amplitude-phase tradeoff in ring modulators

Compact, high-speed electro-optic phase modulators play a vital role in various large-scale applications including phased arrays, quantum and neural networks, and optical communication links. Conventional phase modulators suffer from a fundamental tradeoff between device length and optical loss that limits their scaling capabilities. High-finesse ring resonators have been traditionally used as compact intensity modulators, but their use for phase modulation have been limited due to the high insertion loss associated with the phase change. Here, we show that high-finesse resonators can achieve a strong phase change with low insertion loss by simultaneous modulation of the real and imaginary parts of the refractive index, to the same extent i.e. $\frac{Δn}{Δk} \sim 1$. To implement this strategy, we utilize a hybrid platform that combines a low-loss SiN ring resonator with electro-absorptive graphene (Gr) and electro-refractive WSe$_2$. We achieve a phase modulation efficiency ($V_{\fracπ{2}} \cdot L_{\fracπ{2}}$) of 0.045 V $\cdot$ cm with an insertion loss (IL$_{\fracπ{2}}$) of 4.7 dB for a phase change of $\fracπ{2}$ radians, in a 25 $μ$m long Gr-Al$_2$O$_3$-WSe$_2$ capacitor embedded on a SiN ring of 50 $μ$m radius. We find that our Gr-Al$_2$O$_3$-WSe$_2$ capacitor can support an electro-optic bandwidth of 14.9 $\pm$ 0.1 GHz. We further show that the $V_{\fracπ{2}} \cdot L_{\fracπ{2}}$ of our SiN-2D platform is at least an order of magnitude lower than that of electro-optic phase modulators based on silicon, III-V on silicon, graphene on silicon and lithium niobate. This SiN-2D hybrid platform provides the impetus to design compact and high-speed reconfigurable circuits with graphene and transition metal dichalcogenide (TMD) monolayers that can enable large-scale photonic systems.

physics.optics↗

arXiv2022

Programming moiré patterns in 2D materials by bending

Moiré superlattices in twisted two-dimensional materials have generated tremendous excitement as a platform for achieving quantum properties on demand. However, the moiré pattern is highly sensitive to the interlayer atomic registry, and current assembly techniques suffer from imprecise control of the average twist angle, spatial inhomogeneity in the local twist angle, and distortions due to random strain. Here, we demonstrate a new way to manipulate the moiré patterns in hetero- and homo-bilayers through in-plane bending of monolayer ribbons, using the tip of an atomic force microscope. This technique achieves continuous variation of twist angles with improved twist-angle homogeneity and reduced random strain, resulting in moiré patterns with highly tunable wavelength and ultra-low disorder. Our results pave the way for detailed studies of ultra-low disorder moiré systems and the realization of precise strain-engineered devices.

cond-mat.mes-hall↗