arXiv subjects

James H. Edgar

Publications and source records attributed to James H. Edgar.

At least 37 records · Page 2Linked to original sources

arXiv2025

Growth of hexagonal BN crystals by traveling-solvent floating zone

Large, high-purity single-crystals of hexagonal BN (h-BN) are essential for exploiting its many desirable and interesting properties. Here, we demonstrate via X-ray tomography, X-ray diffraction and scanning electron microscopy that h-BN crystals can be grown by traveling-solvent floating-zone (TSFZ). The diameters of grown boules range from 3 - 5 mm with lengths from 2 - 10 mm. Tomography indicates variable grain sizes within the boules, with the largest having areas of $\approx$ 1 mm $\times$ 2 mm and thickness $\approx$ 0.5 mm. Although the boules contain macroscale flux inclusions, the h-BN lattice itself is of high quality for samples grown under optimized conditions. The currently optimized growth procedure employs an Fe flux, moderate N$_2$ pressure ($P_{N2} \approx$ 6 bar), and a growth rate of 0.1 mm/h. Raman spectroscopy for an optimized sample gives an average linewidth of 7.7(2) cm$^{-1}$ for the E$_{\mathrm{2g}}$ intralayer mode at 1365.46(4) cm$^{-1}$ and 1.0(1) cm$^{-1}$ for the E$_{\mathrm{2g}}$ interlayer shear mode at 51.78(9) cm$^{-1}$. The corresponding photoluminescence spectrum shows sharp phonon-assisted free exciton peaks and minimal signal in the energy range corresponding to carbon-related defects ($E$ = 3.9 4.1 eV). Our work demonstrates the viability of growing h-BN by the TSFZ technique, thereby opening a new route towards larger, high-quality crystals and advancing the state of h-BN related research.

cond-mat.mtrl-sci↗

arXiv2025

Exciton self-trapping in twisted hexagonal boron nitride homostructures

One of the main interests of 2D materials is their ability to be assembled with many degrees of freedom for tuning and manipulating excitonic properties. There is a need to understand how the structure of the interfaces between atomic layers influences exciton properties. Here we use cathodoluminescence and time-resolved cathodoluminescence experiments to study how excitons interact with the interface between two twisted hexagonal boron nitride (hBN) crystals with various angles. An efficient capture of free excitons by the interface is demonstrated, which leads to a population of long-lived and interface-localized (2D) excitons. Temperature dependent experiments indicate that for high twist angles, these excitons localized at the interface further undergo a selftrapping. It consists in a distortion of the lattice around the exciton on which the exciton traps itself. Our results suggest that this exciton-interface interaction causes the broad 4-eV optical emission of highly twisted hBN-hBN structures. Exciton self-trapping is finally discussed as a common feature of sp2 hybridized boron nitride polytypes and nanostructures due to the ionic nature of the B-N bond and the small size of their excitons.

cond-mat.mtrl-sci↗

arXiv2025

The Importance of Pure Dephasing in the Optical Response of Excitons in High-quality van der Waals Heterostructures

Excitons in monolayer transition metal dichalcogenides (TMDs) dominate their optical response due to exceptionally large binding energies arising from their two-dimensional nature. Several theoretical models have been proposed to describe this excitonic behavior, however, it remains unclear which model most accurately captures the underlying physical properties of the response. In this work, we experimentally measure the optical response of high-quality monolayer TMD heterostructures and compare the results with the different theoretical models to address this uncertainty. We find that in high-quality heterostructures, quantum mechanical interactions in the form of pure dephasing plays a dominant role, which has been challenging to isolate experimentally in previous studies. Furthermore, accounting for an additional decay rate to the commonly used radiative and non-radiative rates is found to be important for the accurate description of the excitonic response. These findings establish a robust framework for understanding and predicting the optical properties of TMD-based heterostructures, crucial for both fundamental research and optoelectronic applications.

cond-mat.mes-hall↗

arXiv2025

Charge state tuning of spin defects in hexagonal boron nitride

Boron vacancies in hexagonal boron nitride (hBN) are among the most extensively studied optically active spin defects in van der Waals crystals, due to their promising potential to develop two-dimensional (2D) quantum sensors. In this letter, we demonstrate the tunability of the charge state of boron vacancies in ultrathin hBN layers, revealing a transition from the optically active singly negatively charged state to the optically inactive doubly negatively charged state when sandwiched between graphene electrodes. Notably, there is a photoluminescence quenching of a few percent upon the application of a bias voltage between the electrodes. Our findings emphasize the critical importance of considering the charge state of optically active defects in 2D materials, while also showing that the negatively charged boron vacancy remains robust against external perpendicular electric fields. This stability makes it a promising candidate for integration into various van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2025

Probing Stress and Magnetism at High Pressures with Two-Dimensional Quantum Sensors

Pressure serves as a fundamental tuning parameter capable of drastically modifying all properties of matter. The advent of diamond anvil cells (DACs) has enabled a compact and tabletop platform for generating extreme pressure conditions in laboratory settings. However, the limited spatial dimensions and ultrahigh pressures within these environments present significant challenges for conventional spectroscopy techniques. In this work, we integrate optical spin defects within a thin layer of two-dimensional (2D) materials directly into the high-pressure chamber, enabling an in situ quantum sensing platform for mapping local stress and magnetic environments up to 4~GPa. Compared to nitrogen-vacancy (NV) centers embedded in diamond anvils, our 2D sensors exhibit around three times stronger response to local stress and provide nanoscale proximity to the target sample in heterogeneous devices. We showcase the versatility of our approach by imaging both stress gradients within the high-pressure chamber and a pressure-driven magnetic phase transition in a room-temperature self-intercalated van der Waals ferromagnet, Cr$_{1+δ}$Te$_2$. Our work demonstrates an integrated quantum sensing device for high-pressure experiments, offering potential applications in probing pressure-induced phenomena such as superconductivity, magnetism, and mechanical deformation.

cond-mat.mes-hall↗

arXiv2024

Hall signal-dominated microwave transmission through graphene-loaded waveguides

Microwave transmission line spectroscopy is used to observe the integer quantum Hall effect in two samples of monolayer graphene with different geometries that are resistively-coupled to a coplanar waveguide. We find plateaus in transmitted power that do not vary significantly with microwave frequency but are significantly different for two samples due to their shape. With each drop in transmitted power corresponding to an additional quantum Hall edge mode that short the transmission line to ground, these well-known quanta of conductance allow us to calibrate the sensitivity of the devices. One sample with short contact regions matched the sensitivity expected when considering only the quantum Hall conductance of $νe^2/h$; another sample with long contact regions demonstrated a nearly three-fold enhancement in sensitivity. We model this result with a purely resistive circuit that introduces an additional resistance to explain the increased sensitivity.

cond-mat.mes-hall↗

arXiv2024

On the origin of anomalous hysteresis in graphite/boron nitride transistors

Field-effect devices constructed by stacking flakes of van der Waals (vdW) materials, with hexagonal boron nitride (hBN) playing the role of gate dielectric, often exhibit virtually no hysteresis in their characteristics. This permits exquisitely detailed studies of diverse gate-voltage-tuned phenomena in vdW devices. Recently, however, a dramatic form of gate hysteresis, sometimes called the "gate doesn't work" (GDW) or "electron ratchet" effect, has been seen in certain individual vdW devices that seem otherwise unexceptional. When it occurs, this hysteresis phenomenon is striking and robust, yet it is difficult to reliably reproduce between devices and, largely as a result, its origin remains disputed. Most devices where it has been seen have a bilayer graphene channel and nominal rotational alignment between the graphene and hBN, which has engendered explanations based on properties of bilayer graphene combined with moiré effects. Here, we report our studies of the phenomenon observed in devices that have multilayer graphene channels. We find that the effect can occur in devices with graphite channels that have many more than two graphene layers, in which case it is unambiguously associated with just one surface of the graphite. It can also survive to room temperature, occur in the absence of intentional rotational alignment with hBN, persist when a monolayer of WSe2 is inserted between the graphene and hBN, and exhibit continuous relaxation on timescales of hours or longer. These observations impose strong constraints on the origin of this puzzling phenomenon, which has exciting potential applications if it can be mastered.

cond-mat.mes-hall↗

arXiv2024

Electrical Spectroscopy of Polaritonic Nanoresonators

One of the most captivating properties of polaritons is their capacity to confine light at the nanoscale. This confinement is even more extreme in two-dimensional (2D) materials. 2D polaritons have been investigated by optical measurements using an external photodetector. However, their effective spectrally resolved electrical detection via far-field excitation remains unexplored. This fact hinders their potential exploitation in crucial applications such as sensing molecules and gases, hyperspectral imaging and optical spectrometry, banking on their potential for integration with silicon technologies. Herein, we present the first electrical spectroscopy of polaritonic nanoresonators based on a high-quality 2D-material heterostructure, which serves at the same time as the photodetector and the polaritonic platform. We employ metallic nanorods to create hybrid nanoresonators within the hybrid plasmon-phonon polaritonic medium in the mid and long-wave infrared ranges. Subsequently, we electrically detect these resonators by near-field coupling to a graphene pn-junction. The nanoresonators simultaneously present a record of lateral confinement and high-quality factors of up to 200, exhibiting prominent peaks in the photocurrent spectrum, particularly at the underexplored lower reststrahlen band of hBN. We exploit the geometrical and gate tunability of these nanoresonators to investigate their impact on the photocurrent spectrum and the polaritonic's waveguided modes. This work opens a venue for studying this highly tunable and complex hybrid system, as well as for using it in compact platforms for sensing and photodetection applications.

physics.optics↗

arXiv2024

Determining van der Waals materials' optical and polaritonic properties using cryogenic FTIR micro-spectroscopy

Van-der-Waals materials have been shown to support numerous exotic polaritonic phenomena originating from their layered structures and associated vibrational and electronic properties. This includes emergent polaritonic phenomena, including hyperbolicity and exciton-polariton formation. However, many van-der-Waals materials' unique properties are most prominent at cryogenic temperatures. This presents a particular challenge for polaritonics research, as reliable optical constant data is required for understanding light-matter coupling. For infrared polaritonics (3-100um), the small size of exfoliated flakes makes conventional ellipsometry impossible. This paper presents a cryogenic Fourier transform infrared microscope design constructed entirely from off-the-shelf components and fitting procedures for determining optical constants. We use this microscope to present the first temperature-dependent characterization of the optical properties of hexagonal boron nitride grown with isotopically pure boron. We show that Fabry Perot-type resonances close to the transverse optical phonon show the key temperature-dependent tuning of several parameters. Our full analysis of the infrared dielectric function shows small but significant tuning of the optical constants, which is highly consistent with Raman data from the literature. We then use this dielectric data to perform and analyze the polariton propagation properties, which agree extremely well with published cryogenic scattering-type nearfield microscopy results. In addition to the insights gained into hyperbolic polaritons in hBN, our paper represents a transferable framework for characterizing exfoliated infrared polaritonic materials and other infrared devices. This could accelerate discoveries in other material systems, especially those that are spatially inhomogeneous or cannot be prepared as large single crystals.

physics.optics↗

arXiv2024

Coherently amplified ultrafast imaging using a free-electron interferometer

Accessing the low-energy non-equilibrium dynamics of materials and their polaritons with simultaneous high spatial and temporal resolution has been a bold frontier of electron microscopy in recent years. One of the main challenges lies in the ability to retrieve extremely weak signals while simultaneously disentangling amplitude and phase information. Here, we present Free-Electron Ramsey Imaging (FERI), a microscopy approach based on light-induced electron modulation that enables coherent amplification of optical near-fields in electron imaging. We provide simultaneous time-, space-, and phase-resolved measurements of a micro-drum made from a hexagonal boron nitride membrane visualizing the sub-cycle dynamics of 2D polariton wavepackets therein. The phase-resolved measurements reveals vortex-anti-vortex singularities on the polariton wavefronts, together with an intriguing phenomenon of a traveling wave mimicking the amplitude profile of a standing wave. Our experiments show a 20-fold coherent amplification of the near-field signal compared to conventional electron near-field imaging, resolving peak field intensities in the order of ~W/cm2, corresponding to field amplitudes of a few kV/m. As a result, our work paves the way for spatio-temporal electron microscopy of biological specimens and quantum materials, exciting yet delicate samples that are currently difficult to investigate.

physics.optics↗

arXiv2024

Intrinsic high-fidelity spin polarization of charged vacancies in hexagonal boron nitride

The negatively charged boron vacancy ($\mathrm{V}_{\mathrm{B}}^-$) in hexagonal boron nitride (hBN) has garnered significant attention among defects in two-dimensional materials. This owes, in part, to its deterministic generation, well-characterized atomic structure, and optical polarizability at room temperature. We investigate the latter through extensive measurements probing both the ground and excited state polarization dynamics. We develop a semiclassical model based on these measurements that predicts a near-unity degree of spin polarization, surpassing other solid-state spin defects under ambient conditions. Building upon our model, we include the presence of nuclear spin degrees of freedom adjacent to the $\mathrm{V}_{\mathrm{B}}^-$ and perform a comprehensive set of Lindbladian numerics to investigate the hyperfine-induced polarization of the nuclear spins. Our simulations predict a number of important features that emerge as a function of magnetic field which are borne out by experiment.

quant-ph↗

arXiv2024

Unconventional Unidirectional Magnetoresistance in vdW Heterostructures

Electrical readout of magnetic states is a key to realize novel spintronics devices for efficient computing and data storage. Unidirectional magnetoresistance (UMR) in bilayer systems, consisting of a spin source material and a magnetic layer, refers to a change in the longitudinal resistance upon the reversal of magnetization, which typically originates from the interaction of spin-current and magnetization at the interface. Because of UMR s linear dependence on applied charge current and magnetization, it can be used to electrically read the magnetization state. However, in conventional spin source materials, the spin polarization of an electric field induced spin current is restricted to be in the film plane and hence the ensuing UMR can only respond to the in plane component of the magnetization. On the other hand, magnets with perpendicular magnetic anisotropy (PMA) are highly desired for magnetic memory and spin-logic devices, while the electrical read out of PMA magnets through UMR is critically missing. Here, we report the discovery of an unconventional UMR in bilayer heterostructures of a topological semimetal (WTe2) and a PMA ferromagnetic insulator (Cr2Ge2Te6, CGT), which allows to electrically read the up and down magnetic states of the CGT layer by measuring the longitudinal resistance. Our theoretical calculations based on a tight binding model show that the unconventional UMR originates from the interplay of crystal symmetry breaking in WTe2 and magnetic exchange interaction across the WTe2 and CGT interface. Combining with the ability of WTe2 to obtain magnetic field free switching of the PMA magnets, our discoveries open an exciting pathway to achieve two terminal magnetic memory devices that operate solely on the spin orbit torque and UMR, which is critical for developing next-generation non volatile and low power consumption data storage technologies.

cond-mat.mes-hall↗

arXiv2024

Isotope engineering for spin defects in van der Waals materials

Spin defects in van der Waals materials offer a promising platform for advancing quantum technologies. Here, we propose and demonstrate a powerful technique based on isotope engineering of host materials to significantly enhance the coherence properties of embedded spin defects. Focusing on the recently-discovered negatively charged boron vacancy center ($\mathrm{V}_{\mathrm{B}}^-$) in hexagonal boron nitride (hBN), we grow isotopically purified $\mathrm{h}{}^{10}\mathrm{B}{}^{15}\mathrm{N}$ crystals. Compared to $\mathrm{V}_{\mathrm{B}}^-$ in hBN with the natural distribution of isotopes, we observe substantially narrower and less crowded $\mathrm{V}_{\mathrm{B}}^-$ spin transitions as well as extended coherence time $T_2$ and relaxation time $T_1$. For quantum sensing, $\mathrm{V}_{\mathrm{B}}^-$ centers in our $\mathrm{h}{}^{10}\mathrm{B}{}^{15}\mathrm{N}$ samples exhibit a factor of $4$ ($2$) enhancement in DC (AC) magnetic field sensitivity. For additional quantum resources, the individual addressability of the $\mathrm{V}_{\mathrm{B}}^-$ hyperfine levels enables the dynamical polarization and coherent control of the three nearest-neighbor ${}^{15}\mathrm{N}$ nuclear spins. Our results demonstrate the power of isotope engineering for enhancing the properties of quantum spin defects in hBN, and can be readily extended to improving spin qubits in a broad family of van der Waals materials.

quant-ph↗

arXiv2023

High quality nanocavities through multimodal confinement of hyperbolic polaritons in hexagonal boron nitride

A conventional optical cavity supports modes which are confined because they are unable to leak out of the cavity. Bound state in continuum (BIC) cavities are an unconventional alternative, where light can leak out, but is confined by multimodal destructive interference. BICs are a general wave phenomenon, of particular interest to optics, but BICs and multimodal interference have never been demonstrated at the nanoscale. Here, we demonstrate the first nanophotonic cavities based on BIC-like multimodal interference. This novel confinement mechanism for deep sub-wavelength light shows orders of magnitude improvement in several confinement metrics. Specifically, we obtain cavity volumes below 100x100x3nm^3 with quality factors about 100, with extreme cases having 23x23x3nm^3 volumes or quality factors above 400. Key to our approach, is the use of pristine crystalline hyperbolic dispersion media (HyM) which can support large momentum excitations with relatively low losses. Making a HyM cavity is complicated by the additional modes that appear in a HyM. Ordinarily, these serve as additional channels for leakage, reducing cavity performance. But, in our experiments, we find a BIC-like cavity confinement enhancement effect, which is intimately related to the ray-like nature of HyM excitations. In fact, the quality factors of our cavities exceed the maximum that is possible in the absence of higher order modes. The alliance of HyM with BICs in our work yields a radically novel way to confine light and is expected to have far reaching consequences wherever strong optical confinement is utilized, from ultra-strong light-matter interactions, to mid-IR nonlinear optics and a range of sensing applications.

physics.optics↗

arXiv2023

Hyperbolic phonon-polariton electroluminescence in graphene-hBN van der Waals heterostructures

Phonon-polaritons are electromagnetic waves resulting from the coherent coupling of photons with optical phonons in polar dielectrics. Due to their exceptional ability to confine electric fields to deep subwavelength scales with low loss, they are uniquely poised to enable a suite of applications beyond the reach of conventional photonics, such as sub-diffraction imaging and near-field energy transfer. The conventional approach to exciting phonon-polaritons through optical methods, however, necessitates costly mid-infrared and terahertz coherent light sources along with near-field scanning probes, and generally leads to low excitation efficiency due to the substantial momentum mismatch between phonon-polaritons and free-space photons. Here, we demonstrate that under proper conditions, phonon-polaritons can be excited all-electrically by flowing charge carriers. Specifically, in hexagonal boron nitride (hBN)/graphene heterostructures, by electrically driving charge carriers in ultra-high-mobility graphene out of equilibrium, we observe bright electroluminescence of hBN's hyperbolic phonon-polaritons (HPhPs) at mid-IR frequencies. The HPhP electroluminescence shows a temperature and carrier density dependence distinct from black-body or super-Planckian thermal emission. Moreover, the carrier density dependence of HPhP electroluminescence spectra reveals that HPhP electroluminescence can arise from both inter-band transition and intra-band Cherenkov radiation of charge carriers in graphene. The HPhP electroluminescence offers fundamentally new avenues for realizing electrically-pumped, tunable mid-IR and THz phonon-polariton lasers, and efficient cooling of electronic devices.

cond-mat.mes-hall↗

arXiv2023

Deep Subwavelength Topological Edge State in a Hyperbolic Medium

Topological nanophotonics presents the potential for cutting-edge photonic systems, with a core aim revolving around the emergence of topological edge states. These states are primed to propagate robustly while embracing deep subwavelength confinement that defies diffraction limits. Such attributes make them particularly appealing for nanoscale applications, where achieving these elusive states has remained challenging. We unveil the first experimental proof of deep subwavelength topological edge states by implementing periodic modulation of hyperbolic phonon polaritons within a Van der Waals heterostructure. This finding represents a significant milestone in the field of nanophotonics, and it can be directly extended to and hybridized with other Van der Waals materials in various applications. The extensive scope for material substitution facilitates broadened operational frequency ranges, streamlined integration of diverse polaritonic materials, and compatibility with electronic and excitonic systems.

physics.optics↗

arXiv2023

Bound states in the continuum and long-range coupling of polaritons in hexagonal boron nitride nanoresonators

Bound states in the continuum (BICs) garnered significant for their potential to create new types of nanophotonic devices. Most prior demonstrations were based on arrays of dielectric resonators, which cannot be miniaturized beyond the diffraction limit, reducing the applicability of BICs for advanced functions. Here, we demonstrate BICs and quasi-BICs based on high-quality factor phonon-polariton resonances in isotopically pure h11BN and how these states can be supported by periodic arrays of nanoresonators with sizes much smaller than the wavelength. We theoretically illustrate how BICs emerge from the band structure of the arrays and verify both numerically and experimentally the presence of these states and enhanced quality factor. Furthermore, we identify and characterize simultaneously quasi-BICs and bright states. Our method can be generalized to create a large number of optical states and to tune their coupling with the environment, paving the way to miniaturized nanophotonic devices with more advanced functions.

physics.optics↗

arXiv2023

Chemically detaching hBN crystals grown at atmospheric pressure and high temperature for high-performance graphene devices

In this work, we report on the growth of hexagonal boron nitride (hBN) crystals from an iron flux at atmospheric pressure and high temperature and demonstrate that (i) the entire sheet of hBN crystals can be detached from the metal in a single step using hydrochloric acid and that (ii) these hBN crystals allow the fabrication of high carrier mobility graphene devices. By combining spatially-resolved confocal Raman spectroscopy and electrical transport measurements, we confirm the excellent quality of these crystals for high-performance hBN-graphene-based van der Waals heterostructures. The full width at half maximum of the graphene Raman 2D peak is as low as 16 cm$^{-1}$, and the room temperature charge carrier mobilitiy is around 80000 cm$^2$/(Vs) at a carrier density 1$\times$10$^{12}$cm$^{-12}$. This is fully comparable with devices of similar dimensions fabricated using crystalline hBN synthesized by the high pressure and high temperature method. Finally, we show that for exfoliated high-quality hBN flakes with a thickness between 20 nm and 40 nm the line width of the hBN Raman peak, in contrast to the graphene 2D line width, is not useful for benchmarking hBN in high mobility graphene devices.

cond-mat.mes-hall↗