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John R. Schaibley

Publications and source records attributed to John R. Schaibley.

At least 19 recordsLinked to original sources

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↗

Roadmap: 2D Materials for Quantum Technologies

Two-dimensional (2D) materials have emerged as a versatile and powerful platform for quantum technologies, offering atomic-scale control, strong quantum confinement, and seamless integration into heterogeneous device architectures. Their reduced dimensionality enables unique quantum phenomena, including optically addressable spin defects, tunable single-photon emitters, low-dimensional magnetism, gate-controlled superconductivity, and correlated states in Moiré superlattices. This Roadmap provides a comprehensive overview of recent progress and future directions in exploiting 2D materials for quantum sensing, computation, communication, and simulation. We survey advances spanning spin defects and quantum sensing, quantum emitters and nonlinear photonics, computational theory and data-driven discovery of quantum defects, spintronic and magnonic devices, cavity-engineered quantum materials, superconducting and hybrid quantum circuits, quantum dots, Moiré quantum simulators, and quantum communication platforms. Across these themes, we identify common challenges in defect control, coherence preservation, interfacial engineering, and scalable integration, alongside emerging opportunities driven by machine$-$learning$-$assisted design and integrated experiment$-$theory feedback loops. By connecting microscopic quantum states to mesoscopic excitations and macroscopic device architectures, this Roadmap outlines a materials-centric framework for integrating coherent quantum functionalities and positions 2D materials as foundational building blocks for next-generation quantum technologies.

quant-ph↗

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↗

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↗

Impact of Boron doping to the tunneling magnetoresistance of Heusler alloy Co2FeAl

Heusler alloys based magnetic tunnel junctions can potentially provide high magnetoresistance, small damping and fast switching. Here junctions with Co2FeAl as a ferromagnetic electrode are fabricated by room temperature sputtering on Si/SiO2 substrates. The doping of Boron in Co2FeAl is found to have a large positive impact on the structural, magnetic and transport properties of the junctions, with a reduced interfacial roughness and substantial improved tunneling magnetoresistance. A two-level magnetoresistance is also observed in samples annealed at low temperature, which is believed to be related to the memristive effect of the tunnel barrier with impurities.

cond-mat.mtrl-sci↗

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↗

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↗

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↗

Effect of intravalley and intervalley electron-hole exchange on the nonlinear optical response of monolayer MoSe$_2$

The coherent third-order nonlinear response of monolayer transition-metal dichalcogenide (TMD) semiconductors, such as MoSe$_2$ is dominated by the nonlinear exciton response, as well as biexciton and trion resonances. The fact that these resonances may be spectrally close together makes identification of the signatures, for example in differential transmission (DT), challenging. Instead of focusing on explaining a given set of experimental data, a systematic study aimed at elucidating the roles of intravalley and intervalley electron-hole (e-h) exchange on the DT spectra is presented. Previous works have shown that the e-h exchange introduces a linear leading-order term in the exciton dispersion. Based on a generalized Lippmann-Schwinger equation, we show that the presence of this linear dispersion term can reduce the biexciton binding energy to zero, contrary to the conventional situation of quadratic dispersion where an arbitrarily weak (well-behaved) attractive interaction always supports bound state(s). The effects of spin-scattering and the spin-orbit interaction caused by e-h exchange is also clarified, and the DT lineshape at the exciton and trion resonance are studied as a function of e-h exchange strength. In particular, as the exciton lineshape is determined by the interplay of linear exciton susceptibility and the bound-state two-exciton resonance in the T-matrix, the lineshape at the trion is similarly determined by the interplay of the linear trion susceptibility and the bound-state exciton-trion resonance in the T-matrix.

cond-mat.mes-hall↗

Steady-state nonlinear optical response of excitons in monolayer MoSe$_2$

Monolayer transition metal dichalcogenide (TMD) semiconductors such as MoSe$_2$ host strongly bound excitons which are known to exhibit a strong resonant third-order nonlinear response. Although there have been numerous studies of the ultrafast nonlinear response of monolayer TMDs, a study of the steady-state nonlinear response is lacking. We report a comprehensive study of the steady-state two-color nonlinear response of excitons in hBN-encapsulated monolayer MoSe$_2$ at 7 K. We observe differential transmission (DT) signals associated with the neutral and charged exciton species, which is strongly dependent on the polarization of the pump and probe. Our results are compared to a theoretical model based on a T-matrix formulation for exciton-exciton, exciton-trion, and trion-trion correlations. The parameters are chosen such that the theory accurately reproduces the experimental DT spectrum, which is found to be dominated by two-exciton correlations without strong biexciton binding, exciton-trion attractive interactions, and strong spin mixing through incoherent relaxation.

cond-mat.mes-hall↗

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↗

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↗

Marangoni Convection-Driven Laser Fountains and Waves on Free Surfaces of Liquids

It is well accepted that an outward Marangoni convection from a low surface tension region will make the surface depressed. Here, we report that this established perception is only valid for thin liquid films. Using surface laser heating, we show that in deep liquids a laser beam actually pulls up the fluid above the free surface generating fountains with different shapes. Whereas with decreasing liquid depth a transition from fountain to indentation with fountain in-indentation is observed. Further, high-speed imaging reveals a transient surface process before steady elevation is formed, and this dynamic deformation is subsequently utilized to resonantly excite giant surface waves by a modulated laser beam. Computational fluid dynamics models reveal the underlying flow patterns and quantify the depth-dependent and time-resolved surface deformations. Our discoveries and techniques have upended the century-old perception and opened up a new regime of interdisciplinary research and applications of Marangoni-induced interface phenomena and optocapillary fluidic surfaces-the control of fluids with light.

physics.flu-dyn↗

Monolayer Semiconductor Auger Detector

Auger recombination in semiconductors is a many-body phenomenon in which recombination of electrons and holes is accompanied by excitation of other charge carriers. Being nonradiative, it is detrimental to light emission. The excess energy of the excited carriers is normally rapidly converted to heat, making Auger processes difficult to probe directly. Here, we employ a technique in which the Auger-excited carriers are detected by their ability to tunnel out of the semiconductor through a thin barrier, generating a current. We employ vertical van der Waals (vdW) heterostructures with monolayer WSe2 as the semiconductor and the wide band gap hexagonal boron nitride (hBN) as the tunnel barrier to preferentially transmit high-energy Auger-excited carriers to a graphite electrode. The unambiguous signatures of Auger processes are a rise in the photocurrent when excitons are created by resonant excitation, and negative differential photoconductance resulting from the shifts of the exciton resonances with voltage. We detect holes Auger-excited by both neutral and charged excitons, and find that the Auger scattering is surprisingly strong under weak excitation. The selective extraction of Auger carriers at low, controlled carrier densities that is enabled by vdW heterostructures illustrates an important addition to the techniques available for probing relaxation processes in 2D materials.

cond-mat.mes-hall↗

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↗

Phonon-assisted oscillatory exciton dynamics in monolayer MoSe2

In monolayer semiconductor transition metal dichalcogenides, the exciton-phonon interaction is expected to strongly affect the photocarrier dynamics. Here, we report on an unusual oscillatory enhancement of the neutral exciton photoluminescence with the excitation laser frequency in monolayer MoSe2. The frequency of oscillation matches that of the M-point longitudinal acoustic phonon, LA(M). Oscillatory behavior is also observed in the steady-state emission linewidth and in timeresolved photoluminescence excitation data, which reveals variation with excitation energy in the exciton lifetime. These results clearly expose the key role played by phonons in the exciton formation and relaxation dynamics of two-dimensional van der Waals semiconductors.

cond-mat.mtrl-sci↗

Directional Interlayer Spin-Valley Transfer in Two-Dimensional Heterostructures

Van der Waals heterostructures formed by two different monolayer semiconductors have emerged as a promising platform for new optoelectronic and spin/valleytronic applications. In addition to its atomically thin nature, a two-dimensional semiconductor heterostructure is distinct from its three-dimensional counterparts due to the unique coupled spin-valley physics of its constituent monolayers. Here, we report the direct observation that an optically generated spin-valley polarization in one monolayer can be transferred between layers of a two-dimensional MoSe2-WSe2 heterostructure. Using nondegenerate optical circular dichroism spectroscopy, we show that charge transfer between two monolayers conserves spin-valley polarization and is only weakly dependent on the twist angle between layers. Our work points to a new spin-valley pumping scheme in nanoscale devices, provides a fundamental understanding of spin-valley transfer across the two-dimensional interface, and shows the potential use of two-dimensional semiconductors as a spin-valley generator in 2D spin/valleytronic devices for storing and processing information.

cond-mat.mes-hall↗

Expansion of a Valley-Polarized Exciton Cloud in a 2D Heterostructure

Heterostructures comprising different monolayer semiconductors provide a new system for fundamental science and device technologies, such as in the emerging field of valleytronics. Here, we realize valley-specific interlayer excitons in monolayer WSe2-MoSe2 vertical heterostructures. We create interlayer exciton spin-valley polarization by circularly polarized optical pumping and determine a valley lifetime of 40 nanoseconds. This long-lived polarization enables the visualization of the expansion of a valley-polarized exciton cloud over several microns. The spatial pattern of the polarization evolves into a ring with increasing exciton density, a manifestation of valley exciton exchange interactions. Our work lays a foundation for quantum optoelectronics and valleytronics based on interlayer excitons in van der Waals heterostructures.

cond-mat.mes-hall↗