arXiv subjects

Brian J. LeRoy

Publications and source records attributed to Brian J. LeRoy.

At least 19 recordsLinked to original sources

arXiv2026

Crystallizing electrons with artificially patterned lattices

Wigner crystals are typically confined to ultralow temperatures where thermal motion is frozen out. Moiré superlattices in twisted two-dimensional materials have extended their stability to higher temperatures and densities, but rely on delicate stacking that fixes the lattice geometry and limits tunability. Here we demonstrate a lithographic approach that bypasses these constraints. Using high-resolution nanofabrication, we pattern a nanoscale triangular lattice directly into a graphene gate integrated with a monolayer MoSe2 semiconductor. This engineered potential landscape localizes electrons into generalized Wigner crystal states that persist up to 15 K and densities of 2X10^12 cm-2, representing an order of magnitude improvement over pristine monolayer MoSe2. Gate-voltage control allows real-time switching between stable and unstable crystalline states, with the latter exhibiting stochastic telegraph noise from nearly degenerate configurations. This work demonstrates the ability of this platform to transform Wigner crystals from fragile, static phases into reconfigurable quantum matter.

cond-mat.mes-hall↗

arXiv2025

Cryogenic Nano-Imaging of Excitons in a Monolayer Semiconductor

Excitons, Coulomb bound electron-hole pairs, dominate the optical response of two-dimensional semiconductors across near-infrared and visible frequencies due to their large binding energy and prominent oscillator strength. Previous measurements of excitons in 2D semiconductors have primarily relied on far-field optical spectroscopy techniques which are diffraction limited to several hundred nanometers. To precisely image nanoscale spatial disorder requires an order of magnitude increase in resolution capabilities. Here, we present a study of the exciton spectra of monolayer MoSe2 in the visible range using a cryogenic scattering-type scanning near field optical microscope (s-SNOM) operating down to 11 K. By mapping the spatial variation in the exciton resonance across an hBN encapsulated MoSe2 monolayer, we achieve sub-50 nm spatial resolution and energy resolution below 1 meV. We further investigate the material's near-field spectra and dielectric function, demonstrating the ability of cryogenic visible s-SNOM to reveal nanoscale disorder. Comparison to room temperature measurements illustrate the enhanced capabilities of cryogenic s-SNOM to reveal fine-scale material heterogeneity.

cond-mat.mes-hall↗

arXiv2023

Ultra-broadband bright light emission from a one-dimensional inorganic van der Waals material

One-dimensional (1D) van der Waals materials have emerged as an intriguing playground to explore novel electronic and optical effects. We report on inorganic one-dimensional SbPS4 nanotubes bundles obtained via mechanical exfoliation from bulk crystals. The ability to mechanically exfoliate SbPS4 nanobundles offers the possibility of applying modern 2D material fabrication techniques to create mixed-dimensional van der Waals heterostructures. We find that SbPS4 can readily be exfoliated to yield long (> 10 μm) nanobundles with thicknesses that range from of 1.3 - 200 nm. We investigated the optical response of semiconducting SbPS4 nanobundles and discovered that upon excitation with blue light, they emit bright and ultra-broadband red light with a quantum yield similar to that of hBN-encapsulated MoSe2. We discovered that the ultra-broadband red light emission is a result of a large ~1 eV exciton binding energy and a ~200 meV exciton self-trapping energy, unprecedented in previous material studies. Due to the bright and ultra-broadband light emission, we believe that this class of inorganic 1D van der Waals semiconductors has numerous potential applications including on-chip tunable nanolasers, and applications that require ultra-violet to visible light conversion such as lighting and sensing. Overall, our findings open avenues for harnessing the unique characteristics of these nanomaterials, advancing both fundamental research and practical optoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2022

Single exciton trapping in an electrostatically defined 2D semiconductor quantum dot

Interlayer excitons (IXs) in 2D semiconductors have long lifetimes and spin-valley coupled physics, with a long-standing goal of single exciton trapping for valleytronic applications. In this work, we use a nano-patterned graphene gate to create an electrostatic IX trap. We measure a unique power-dependent blue-shift of IX energy, where narrow linewidth emission exhibits discrete energy jumps. We attribute these jumps to quantized increases of the number occupancy of IXs within the trap and compare to a theoretical model to assign the lowest energy emission line to single IX recombination.

cond-mat.mes-hall↗

arXiv2022

Interlayer Exciton Diode and Transistor

Controlling the flow of charge neutral interlayer exciton (IX) quasiparticles can potentially lead to low loss excitonic circuits. Here, we report unidirectional transport of IXs along nanoscale electrostatically defined channels in an MoSe$_2$-WSe$_2$ heterostructure. These results are enabled by a lithographically defined triangular etch in a graphene gate to create a potential energy ''slide''. By performing spatially and temporally resolved photoluminescence measurements, we measure smoothly varying IX energy along the structure and high-speed exciton flow with a drift velocity up to 2 * 10$^6$ cm/s, an order of magnitude larger than previous experiments. Furthermore, exciton flow can be controlled by saturating exciton population in the channel using a second laser pulse, demonstrating an optically gated excitonic transistor. Our work paves the way towards low loss excitonic circuits, the study of bosonic transport in one-dimensional channels, and custom potential energy landscapes for excitons in van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2022

Direct STM Measurements of R- and H-type Twisted MoSe2/WSe2 Heterostructures

When semiconducting transition metal dichalcogenides heterostructures are stacked the twist angle and lattice mismatch leads to a periodic moiré potential. As the angle between the layers changes, so do the electronic properties. As the angle approaches 0- or 60-degrees interesting characteristics and properties such as modulations in the band edges, flat bands, and confinement are predicted to occur. Here we report scanning tunneling microscopy and spectroscopy measurements on the band gaps and band modulations in MoSe2/WSe2 heterostructures with near 0 degree rotation (R-type) and near 60 degree rotation (H-type). We find a modulation of the band gap for both stacking configurations with a larger modulation for R-type than for H-type as predicted by theory. Furthermore, local density of states images show that electrons are localized differently at the valence band and conduction band edges.

cond-mat.mtrl-sci↗

arXiv2022

Localized Interlayer Excitons in MoSe2-WSe2 Heterostructures without a Moiré Potential

Trapped interlayer excitons (IXs) in MoSe2-WSe2 heterobilayers have generated interest for use as single quantum emitter arrays and as an opportunity to study moiré physics in transition metal dichalcogenide (TMD) heterostructures. IXs are spatially indirectly excitons comprised of an electron in the MoSe2 layer bound to a hole in the WSe2 layer. Previous reports of spectrally narrow (<1 meV) photoluminescence (PL) emission lines at low temperature have been attributed to IXs localized by the moiré potential between the TMD layers. Here, we show that spectrally narrow IX PL lines are present even when the moiré potential is suppressed by inserting a bilayer hexagonal boron nitride (hBN) spacer between the TMD layers. We directly compare the doping, electric field, magnetic field, and temperature dependence of IXs in a directly contacted MoSe2-WSe2 region to those in a region separated by bilayer hBN. Our results show that the localization potential resulting in the narrow PL lines is independent of the moiré potential, and instead likely due to extrinsic effects such as nanobubbles or defects. We show that while the doping, electric field, and temperature dependence of the narrow IX lines is similar for both regions, their excitonic g-factors have opposite signs, indicating that the IXs in the directly contacted region are trapped by both moiré and extrinsic localization potentials.

cond-mat.other↗

arXiv2021

Nanoscale trapping of interlayer excitons in a 2D semiconductor heterostructure

For quantum technologies based on single excitons and spins, the deterministic placement and control of a single exciton is a long-standing goal. MoSe2-WSe2 heterostructures host spatially indirect interlayer excitons (IXs) which exhibit highly tunable energies and unique spin-valley physics, making them promising candidates for quantum information processing. Previous IX trapping approaches involving moiré superlattices and nanopillars do not meet the quantum technology requirements of deterministic placement and energy tunability. Here, we use a nanopatterned graphene gate to create a sharply varying electric field in close proximity to a MoSe2-WSe2 heterostructure. The dipole interaction between the IX and the electric field creates an ~20 nm trap. The trapped IXs show the predicted electric field dependent energy, saturation at low excitation power, and increased lifetime, all signatures of strong spatial confinement. The demonstrated architecture is a crucial step towards deterministic trapping of single IXs, which has broad applications to scalable quantum technologies.

cond-mat.mes-hall↗

arXiv2021

Temperature dependent moiré trapping of interlayer excitons in MoSe2-WSe2 heterostructures

MoSe2-WSe2 heterostructures host strongly bound interlayer excitons (IXs) which exhibit bright photoluminescence (PL) when the twist-angle is near 0° or 60°. Over the past several years, there have been numerous reports on the optical response of these heterostructures but no unifying model to understand the dynamics of IXs and their temperature dependence. Here, we perform a comprehensive study of the temperature, excitation power, and time-dependent PL of IXs. We observe a significant decrease in PL intensity above a transition temperature that we attribute to a transition from localized to delocalized IXs. Astoundingly, we find a simple inverse relationship between the IX PL energy and the transition temperature, which exhibits opposite power dependent behaviors for near 0° and 60° samples. We conclude that this temperature dependence is a result of IX-IX exchange interactions, whose effect is suppressed by the moiré potential trapping IXs at low temperature.

physics.optics↗

arXiv2020

Probing the wavefunctions of correlated states in magic angle graphene

Using scanning probe microscopy and spectroscopy, we explore the spatial symmetry of the electronic wavefunctions of twisted bilayer graphene at the "magic angle" of 1.1 degrees. This small twist angle leads to a long wavelength moiré unit cell on the order of 13 nm and the appearance of two flat bands. As the twist angle is decreased, correlation effects increase until they are maximized at the magic angle. At this angle, the wavefunctions at the charge neutrality point show only C2 symmetry due to the emergence of a charge ordered state. As the system is doped, the symmetry of the wavefunctions change at each commensurate filling of the moiré unit cell pointing to the correlated nature of the spin and valley degeneracy broken states.

cond-mat.mes-hall↗

arXiv2020

Flat bands in twisted bilayer transition metal dichalcogenides

The crystal structure of a material creates a periodic potential that electrons move through giving rise to the electronic band structure of the material. When two-dimensional materials are stacked, the twist angle between the layers becomes an additional degree freedom for the resulting heterostructure. As this angle changes, the electronic band structure is modified leading to the possibility of flat bands with localized states and enhanced electronic correlations. In transition metal dichalcogenides, flat bands have been theoretically predicted to occur for long moiré wavelengths over a range of twist angles around 0 and 60 degrees giving much wider versatility than magic angle twisted bilayer graphene. Here we show the existence of a flat band in the electronic structure of 3° and 57.5° twisted bilayer WSe2 samples using scanning tunneling spectroscopy. Direct spatial mapping of wavefunctions at the flat band energy have shown that the flat bands are localized differently for 3° and 57.5°, in excellent agreement with first-principle density functional theory calculations.

cond-mat.str-el↗

arXiv2020

Local characterization and engineering of proximitized correlated states in graphene-NbSe$_2$ vertical heterostructures

Using a van der Waals vertical heterostructure consisting of monolayer graphene, monolayer hBN and NbSe$_2$, we have performed local characterization of induced correlated states in different configurations. At a temperature of 4.6 K, we have shown that both superconductivity and charge density waves can be induced in graphene from NbSe2 by proximity effects. By applying a vertical magnetic field, we imaged the Abrikosov vortex lattice and extracted the coherence length for the proximitized superconducting graphene. We further show that the induced correlated states can be completely blocked by adding a monolayer hBN between the graphene and the NbSe$_2$, which demonstrates the importance of the tunnel barrier and surface conditions between the normal metal and superconductor for the proximity effect.

cond-mat.mes-hall↗

arXiv2019

2D Semiconductor Nonlinear Plasmonic Modulators

A plasmonic modulator is a device that controls the amplitude or phase of propagating plasmons. In a pure plasmonic modulator, the presence or absence of a pump plasmonic wave controls the amplitude of a probe plasmonic wave through a channel. This control has to be mediated by an interaction between disparate plasmonic waves, typically requiring the integration of a nonlinear material. In this work, we demonstrate the first 2D semiconductor nonlinear plasmonic modulator based on a WSe2 monolayer integrated on top of a lithographically defined metallic waveguide. We utilize the strong coupling between the surface plasmon polaritons, SPPs, and excitons in the WSe2 to give a 73 percent change in transmission through the device. We demonstrate control of the propagating SPPs using both optical and SPP pumps, realizing the first demonstration of a 2D semiconductor nonlinear plasmonic modulator, with a modulation depth of 4.1 percent, and an ultralow switching energy estimated to be 40 aJ.

physics.app-ph↗

arXiv2018

Topologically Protected Helical States in Minimally Twisted Bilayer Graphene

In minimally twisted bilayer graphene, a moir{é} pattern consisting of AB and BA stacking regions separated by domain walls forms. These domain walls are predicted to support counterpropogating topologically protected helical (TPH) edge states when the AB and BA regions are gapped. We fabricate designer moir{é} crystals with wavelengths longer than 50 nm and demonstrate the emergence of TPH states on the domain wall network by scanning tunneling spectroscopy measurements. We observe a double-line profile of the TPH states on the domain walls, only occurring when the AB and BA regions are gapped. Our results demonstrate a practical and flexible method for TPH state network construction.

cond-mat.mes-hall↗

arXiv2017

Evolution of the electronic band structure of twisted bilayer graphene upon doping

The electronic band structure of twisted bilayer graphene develops van Hove singularities whose energy depends on the twist angle between the two layers. Using Raman spectroscopy, we monitor the evolution of the electronic band structure upon doping using the G peak area which is enhanced when the laser photon energy is resonant with the energy separation of the van Hove singularities. Upon charge doping, the Raman G peak area initially increases for twist angles larger than a critical angle and decreases for smaller angles. To explain this behavior with twist angle, the energy of separation of the van Hove singularities must decrease with increasing charge density demonstrating the ability to modify the electronic and optical properties of twisted bilayer graphene with doping.

cond-mat.mtrl-sci↗

arXiv2017

Ultrafast relaxation of hot phonons in Graphene-hBN Heterostructures

Fast carrier cooling is important for high power graphene based devices. Strongly Coupled Optical Phonons (SCOPs) play a major role in the relaxation of photoexcited carriers in graphene. Heterostructures of graphene and hexagonal boron nitride (hBN) have shown exceptional mobility and high saturation current, which makes them ideal for applications, but the effect of the hBN substrate on carrier cooling mechanisms is not understood. We track the cooling of hot photo-excited carriers in graphene-hBN heterostructures using ultrafast pump-probe spectroscopy. We find that the carriers cool down four times faster in the case of graphene on hBN than on a silicon oxide substrate thus overcoming the hot phonon (HP) bottleneck that plagues cooling in graphene devices.

cond-mat.mes-hall↗

arXiv2017

Tunable Moiré Bands and Strong Correlations in Small-Twist-Angle Bilayer Graphene

According to electronic structure theory, bilayer graphene is expected to have anomalous electronic properties when it has long-period moiré patterns produced by small misalignments between its individual layer honeycomb lattices. We have realized bilayer graphene moiré crystals with accurately controlled twist angles smaller than 1 degree and studied their properties using scanning probe microscopy and electron transport. We observe conductivity minima at charge neutrality, satellite gaps that appear at anomalous carrier densities for twist angles smaller than 1 degree, and tunneling densities-of-states that are strongly dependent on carrier density. These features are robust up to large transverse electric fields. In perpendicular magnetic fields, we observe the emergence of a Hofstadter butterfly in the energy spectrum, with four-fold degenerate Landau levels, and broken symmetry quantum Hall states at filling factors 1, 2, 3. These observations demonstrate that at small twist angles, the electronic properties of bilayer graphene moiré crystals are strongly altered by electron-electron interactions.

cond-mat.mes-hall↗

arXiv2017

Pressure-induced commensurate stacking of graphene on boron nitride

Combining atomically-thin van der Waals materials into heterostructures provides a powerful path towards the creation of designer electronic devices. The interaction strength between neighboring layers, most easily controlled through their interlayer separation, can have significant influence on the electronic properties of these composite materials. Here, we demonstrate unprecedented control over interlayer interactions by locally modifying the interlayer separation between graphene and boron nitride, which we achieve by applying pressure with a scanning tunneling microscopy tip. For the special case of aligned or nearly-aligned graphene on boron nitride, the graphene lattice can stretch and compress locally to compensate for the slight lattice mismatch between the two materials. We find that modifying the interlayer separation directly tunes the lattice strain and induces commensurate stacking underneath the tip. Our results motivate future studies tailoring the electronic properties of van der Waals heterostructures by controlling the interlayer separation of the entire device using hydrostatic pressure.

cond-mat.mes-hall↗