arXiv subjects

J. H. Edgar

Publications and source records attributed to J. H. Edgar.

At least 19 recordsLinked to original sources

arXiv2025

Magnetic imaging under high pressure with a spin-based quantum sensor integrated in a van der Waals heterostructure

Pressure is a powerful thermodynamic parameter for tuning the magnetic properties of van der Waals magnets owing to their weak interlayer bonding. However, local magnetometry measurements under high pressure still remain elusive for this important class of emerging materials. Here we introduce a method enabling in situ magnetic imaging of van der Waals magnets under high pressure with sub-micron spatial resolution. Our approach relies on a quantum sensing platform based on boron-vacancy (V$_\text{B}^-$) centers in hexagonal boron nitride (hBN), which can be placed in atomic contact of any type of two-dimensional (2D) material within a van der Waals heterostructure. We first show that the V$_\text{B}^-$ center can be used as a magnetic field sensor up to pressures of a few GPa, a pressure range for which the properties of a wide variety of van der Waals magnets are efficiently altered. We then use V$_\text{B}^-$ centers in a thin hBN layer to perform magnetic imaging of a van der Waals magnet under pressure. As a proof of concept, we study the pressure-dependent magnetization in micrometer-sized flakes of $1T$-CrTe$_2$, whose evolution is explained by a shift of the Curie temperature. Besides providing a new path for studying pressure-induced phase transitions in van der Waals magnets, this work also opens up interesting perspectives for exploring the physics of 2D superconductors under pressure via local measurements of the Meissner effect.

cond-mat.mtrl-sci↗

arXiv2024

Electroluminescence and Energy Transfer Mediated by Hyperbolic Polaritons

Under high electrical current, some materials can emit electromagnetic radiation beyond incandescence. This phenomenon, referred to as electroluminescence, leads to the efficient emission of visible photons and is the basis of domestic lighting devices (e.g., light-emitting diodes). In principle, electroluminescence can lead to mid-infrared (mid-IR) emission of confined light-matter excitations called phonon-polaritons, resulting from the coupling of photons with crystal lattice vibrations (optical phonons). In particular, phonon-polaritons arising in the van der Waals crystal hexagonal boron nitride (hBN) exhibit hyperbolic dispersion, which enhances light-matter coupling. For this reason, electroluminescence of hyperbolic phonon-polaritons (HPhPs) has been proposed as an explanation for the peculiar radiative energy transfer within hBN-encapsulated graphene transistors. However, since HPhPs are confined, they are inaccessible in the far-field, so that any hint of electroluminescence is only based on indirect electronic signatures and needs to be confirmed by direct observation. Here, we demonstrate far-field mid-IR (λ = 6.5 μm) electroluminescence of HPhPs excited by strongly biased high-mobility graphene within a van der Waals heterostructure, and we quantify the associated radiative energy transfer through the material. The presence of HPhPs is revealed via far-field mid-IR spectroscopy due to their elastic scattering at discontinuities in the heterostructure. The associated radiative flux is quantified by mid-IR pyrometry of the substrate receiving the energy. This radiative energy transfer is shown to be reduced in hBN with nanoscale inhomogeneities, demonstrating the central role of the electromagnetic environment in this process.

cond-mat.mes-hall↗

arXiv2024

Isotope substitution and polytype control for point defects identification: the case of the ultraviolet color center in hexagonal boron nitride

Defects in crystals can have a transformative effect on the properties and functionalities of solid-state systems. Dopants in semiconductors are core components in electronic and optoelectronic devices. The control of single color centers is at the basis of advanced applications for quantum technologies. Unintentional defects can also be detrimental to the crystalline structure and hinder the development of novel materials. Whatever the research perspective, the identification of defects is a key but complicated, and often long-standing issue. Here, we present a general methodology to identify point defects by combining isotope substitution and polytype control, with a systematic comparison between experiments and first-principles calculations. We apply this methodology to hexagonal boron nitride (hBN) and its ubiquitous color center emitting in the ultraviolet spectral range. From isotopic purification of the host hBN matrix, a local vibrational mode of the defect is uncovered, and isotope-selective carbon doping proves that this mode belongs to a carbon-based center. Then, by varying the stacking sequence of the host hBN matrix, we unveil different optical responses to hydrostatic pressure for the non-equivalent configurations of this ultraviolet color center. We conclude that this defect is a carbon dimer in the honeycomb lattice of hBN. Our results show that tuning the stacking sequence in different polytypes of a given crystal provides unique fingerprints contributing to the identification of defects in 2D materials.

cond-mat.mtrl-sci↗

arXiv2024

Spin-dependent photodynamics of boron-vacancy centers in hexagonal boron nitride

The negatively-charged boron vacancy (V$_\text{B}^-$) center in hexagonal boron nitride (hBN) is currently garnering considerable attention for the design of two-dimensional (2D) quantum sensing units. Such developments require a precise understanding of the spin-dependent optical response of V$_\text{B}^-$ centers, which still remains poorly documented despite its key role for sensing applications. Here we investigate the spin-dependent photodynamics of V$_\text{B}^-$ centers in hBN by a series of time-resolved photoluminescence (PL) measurements. We first introduce a robust all-optical method to infer the spin-dependent lifetime of the excited states and the electron spin polarization of V$_\text{B}^-$ centers under optical pumping. Using these results, we then analyze PL time traces recorded at different optical excitation powers with a seven-level model of the V$_\text{B}^-$ center and we extract all the rates involved in the spin-dependent optical cycles, both under ambient conditions and at liquid helium temperature. These findings are finally used to study the impact of a vector magnetic field on the optical response. More precisely, we analyze PL quenching effects resulting from electron spin mixing induced by the magnetic field component perpendicular to the V$_\text{B}^-$ quantization axis. All experimental results are well reproduced by the seven-level model, illustrating its robustness to describe the spin-dependent photodymanics of V$_\text{B}^-$ centers. This work provides important insights into the properties of V$_\text{B}^-$ centers in hBN, which are valuable for future developments of 2D quantum sensing units.

cond-mat.mtrl-sci↗

arXiv2023

Isotopic control of the boron-vacancy spin defect in hexagonal boron nitride

We report on electron spin resonance (ESR) spectroscopy of boron-vacancy (V$_\text{B}^-$) centers hosted in isotopically-engineered hexagonal boron nitride (hBN) crystals. We first show that isotopic purification of hBN with $^{15}$N yields a simplified and well-resolved hyperfine structure of V$_\text{B}^-$ centers, while purification with $^{10}$B leads to narrower ESR linewidths. These results establish isotopically-purified h$^{10}$B$^{15}$N crystals as the optimal host material for future use of V$_\text{B}^-$ spin defects in quantum technologies. Capitalizing on these findings, we then demonstrate optically-induced polarization of $^{15}$N nuclei in h$^{10}$B$^{15}$N, whose mechanism relies on electron-nuclear spin mixing in the V$_\text{B}^-$ ground state. This work opens up new prospects for future developments of spin-based quantum sensors and simulators on a two-dimensional material platform.

quant-ph↗

arXiv2023

Negative refraction in hyperbolic hetero-bicrystals

We visualized negative refraction of phonon polaritons, which occurs at the interface between two natural crystals. The polaritons - hybrids of infrared photons and lattice vibrations - form collimated rays that display negative refraction when passing through a planar interface between the two hyperbolic van der Waals materials: molybdenum oxide ($MoO_3$) and isotopically pure hexagonal boron nitride ($h^{11}BN$). At a special frequency $ω_0$, these rays can circulate along closed diamond-shaped trajectories. We have shown that polariton eigenmodes display regions of both positive and negative dispersion interrupted by multiple gaps that result from polaritonic level repulsion and strong coupling.

cond-mat.mes-hall↗

arXiv2023

Boron and nitrogen isotope effects on hexagonal boron nitride properties

The unique physical, mechanical, chemical, optical, and electronic properties of hexagonal boron nitride (hBN) make it a promising two-dimensional material for electronic, optoelectronic, nanophotonic, and quantum devices. Here we report on the changes in hBN's properties induced by isotopic purification in both boron and nitrogen. Previous studies on isotopically pure hBN have focused on purifying the boron isotope concentration in hBN from its natural concentration (approximately 20 at$\%$ $^{10}$B, 80 at$\%$ $^{11}$B) while using naturally abundant nitrogen (99.6 at$\%$ $^{14}$N, 0.4 at$\%$ $^{15}$N), i.e. almost pure $^{14}$N. In this study, we extend the class of isotopically-purified hBN crystals to $^{15}$N. Crystals in the four configurations, namely h$^{10}$B$^{14}$N, h$^{11}$B$^{14}$N, h$^{10}$B$^{15}$N, and h$^{11}$B$^{15}$N, were grown by the metal flux method using boron and nitrogen single isotope ($>99\%$) enriched sources, with nickel plus chromium as the solvent. In-depth Raman and photoluminescence spectroscopies demonstrate the high quality of the monoisotopic hBN crystals with vibrational and optical properties of the $^{15}$N-purified crystals at the state of the art of currently available $^{14}$N-purified hBN. The growth of high-quality h$^{10}$B$^{14}$N, h$^{11}$B$^{14}$N, h$^{10}$B$^{15}$N, and h$^{11}$B$^{15}$N opens exciting perspectives for thermal conductivity control in heat management, as well as for advanced functionalities in quantum technologies.

cond-mat.mtrl-sci↗

arXiv2023

Optically-active spin defects in few-layer thick hexagonal boron nitride

Optically-active spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of two-dimensional quantum sensing units offering optimal proximity to the sample being probed. In this work, we first demonstrate that the electron spin resonance frequencies of boron vacancy centres (V$_\text{B}^-$) can be detected optically in the limit of few-atomic-layer thick hBN flakes despite the nanoscale proximity of the crystal surface that often leads to a degradation of the stability of solid-state spin defects. We then analyze the variations of the electronic spin properties of V$_\text{B}^-$ centres with the hBN thickness with a focus on (i) the zero-field splitting parameters, (ii) the optically-induced spin polarization rate and (iii) the longitudinal spin relaxation time. This work provides important insights into the properties of V$_\text{B}^-$ centres embedded in ultrathin hBN flakes, which are valuable for future developments of foil-based quantum sensing technologies.

quant-ph↗

arXiv2023

A planar defect spin sensor in a two-dimensional material susceptible to strain and electric fields

The boron-vacancy spin defect ($\text{V}_\text{B}^{-}$) in hexagonal boron nitride (hBN) has a great potential as a quantum sensor in a two-dimensional material that can directly probe various external perturbations in atomic-scale proximity to the quantum sensing layer. Here, we apply first principles calculations to determine the coupling of the $\text{V}_\text{B}^{-}$ electronic spin to strain and electric fields. Our work unravels the interplay between local piezoelectric and elastic effects contributing to the final response to the electric fields. The theoretical predictions are then used to analyse optically detected magnetic resonance (ODMR) spectra recorded on hBN crystals containing different densities of $\text{V}_\text{B}^{-}$ centres. We prove that the orthorhombic zero-field splitting parameter results from local electric fields produced by surrounding charge defects. By providing calculations of the spin-strain and spin-electric field couplings, this work paves the way towards applications of $\text{V}_\text{B}^{-}$ centres for quantitative electric field imaging and quantum sensing under pressure.

quant-ph↗

arXiv2023

Unexpected catalytic activity of nanorippled graphene

Graphite is one of the most chemically inert materials. Its elementary constituent, monolayer graphene, is generally expected to inherit most of the parent material's properties including chemical inertness. Here we show that, unlike graphite, defect-free monolayer graphene exhibits a strong activity with respect to splitting molecular hydrogen, which is comparable to that of metallic and other known catalysts for this reaction. We attribute the unexpected catalytic activity to surface corrugations (nanoscale ripples), a conclusion supported by theory. Nanoripples are likely to play a role in other chemical reactions involving graphene and, because nanorippling is inherent to atomically thin crystals, can be important for two dimensional materials in general.

cond-mat.mtrl-sci↗

arXiv2023

Dual-band coupling between nanoscale polaritons and vibrational and electronic excitations in molecules

Strong coupling (SC) between light and matter excitations such as excitons and molecular vibrations bear intriguing potential for controlling chemical reactivity, conductivity or photoluminescence. So far, SC has been typically achieved either between mid-infrared (mid-IR) light and molecular vibrations or between visible light and excitons. Achieving SC simultaneously in both frequency bands may open unexplored pathways for manipulating material properties. Here, we introduce a polaritonic nanoresonator (formed by h-BN layers placed on Al ribbons) hosting surface plasmon polaritons (SPPs) at visible frequencies and phonon polaritons (PhPs) at mid-IR frequencies, which simultaneously couple to excitons and atomic vibration in an adjacent molecular layer (CoPc). Employing near-field optical nanoscopy, we first demonstrate the co-localization of strongly confined near-fields at both visible and mid-IR frequencies. After covering the nanoresonator structure with a layer of CoPc molecules, we observe clear mode splittings in both frequency ranges by far-field transmission spectroscopy, unambiguously revealing simultaneous SPP-exciton and PhP-vibron coupling. Dual-band SC may be exploited for manipulating the coupling between excitons and molecular vibrations in future optoelectronics, nanophotonics, and quantum information applications.

physics.optics↗

arXiv2022

Magnetic imaging with spin defects in hexagonal boron nitride

Optically-active spin defects hosted in hexagonal boron nitride (hBN) are promising candidates for the development of a two-dimensional (2D) quantum sensing unit. Here, we demonstrate quantitative magnetic imaging with hBN flakes doped with negatively-charged boron-vacancy (V$_{\rm B}^-$) centers through neutron irradiation. As a proof-of-concept, we image the magnetic field produced by CrTe$_2$, a van der Waals ferromagnet with a Curie temperature slightly above $300$ K. Compared to other quantum sensors embedded in 3D materials, the advantages of the hBN-based magnetic sensor described in this work are its ease of use, high flexibility and, more importantly, its ability to be placed in close proximity to a target sample. Such a sensing unit will likely find numerous applications in 2D materials research by offering a simple way to probe the physics of van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2021

Decoherence of V$_{\rm B}^{-}$ spin defects in monoisotopic hexagonal boron nitride

Spin defects in hexagonal boron nitride (hBN) are promising quantum systems for the design of flexible two-dimensional quantum sensing platforms. Here we rely on hBN crystals isotopically enriched with either $^{10}$B or $^{11}$B to investigate the isotope-dependent properties of a spin defect featuring a broadband photoluminescence signal in the near infrared. By analyzing the hyperfine structure of the spin defect while changing the boron isotope, we first unambiguously confirm that it corresponds to the negatively-charged boron-vacancy center (${\rm V}_{\rm B}^-$). We then show that its spin coherence properties are slightly improved in $^{10}$B-enriched samples. This is supported by numerical simulations employing cluster correlation expansion methods, which reveal the importance of the hyperfine Fermi contact term for calculating the coherence time of point defects in hBN. Using cross-relaxation spectroscopy, we finally identify dark electron spin impurities as an additional source of decoherence. This work provides new insights into the properties of ${\rm V}_{\rm B}^-$ spin defects, which are valuable for the future development of hBN-based quantum sensing foils.

cond-mat.mtrl-sci↗

arXiv2021

Graphene's non-equilibrium fermions reveal Doppler-shifted magnetophonon resonances accompanied by Mach supersonic and Landau velocity effects

Oscillatory magnetoresistance measurements on graphene have revealed a wealth of novel physics. These phenomena are typically studied at low currents. At high currents, electrons are driven far from equilibrium with the atomic lattice vibrations so that their kinetic energy can exceed the thermal energy of the phonons. Here, we report three non-equilibrium phenomena in monolayer graphene at high currents: (i) a "Doppler-like" shift and splitting of the frequencies of the transverse acoustic (TA) phonons emitted when the electrons undergo inter-Landau level (LL) transitions; (ii) an intra-LL Mach effect with the emission of TA phonons when the electrons approach supersonic speed, and (iii) the onset of elastic inter-LL transitions at a critical carrier drift velocity, analogous to the superfluid Landau velocity. All three quantum phenomena can be unified in a single resonance equation. They offer avenues for research on out-of-equilibrium phenomena in other two-dimensional fermion systems.

cond-mat.mes-hall↗

arXiv2021

Cyclotron resonance overtones and near-field magnetoabsorption via terahertz Bernstein modes in graphene

Two-dimensional electron systems subjected to a perpendicular magnetic field absorb electromagnetic radiation via the cyclotron resonance (CR). Here we report a qualitative breach of this well-known behaviour in graphene. Our study of the terahertz photoresponse reveals a resonant burst at the main overtone of the CR, drastically exceeding the signal detected at the position of the ordinary CR. In accordance with the developed theory, the photoresponse dependencies on the magnetic field, doping level, and sample geometry suggest that the origin of this anomaly lies in the near-field magnetoabsorption facilitated by the Bernstein modes, ultra-slow magnetoplasmonic excitations reshaped by nonlocal electron dynamics. Close to the CR harmonics, these modes are characterized by a flat dispersion and a diverging plasmonic density of states that strongly amplifies the radiation absorption. Besides fundamental interest, our experimental results and developed theory show that the radiation absorption via nonlocal collective modes can facilitate a strong photoresponse, a behaviour potentially useful for infrared and terahertz technology.

cond-mat.mes-hall↗

arXiv2021

Planar nano-optics in anisotropic media: anomalous refraction and diffraction-free lensing of highly confined polaritons

As one of the most fundamental optical phenomena, refraction between isotropic media is characterized by light bending towards the normal to the boundary when passing from a low- to a high-refractive-index medium. However, in anisotropic media, refraction is a much more exotic phenomenon. The most general case of refraction between two anisotropic media remains unexplored, particularly in natural media and at the nanoscale. Here, we visualize and comprehensively study refraction of electromagnetic waves between two strongly anisotropic (hyperbolic) media, and, importantly, we do it with the use of polaritons confined to the nanoscale in a low-loss natural medium, alpha-MoO3. Our images show refraction of polaritons under the general case in which both the direction of propagation and the wavevector are not collinear. As they traverse planar nanoprisms tailored in alpha-MoO3, refracted polaritons exhibit non-intuitive directions of propagation, enabling us to unveil an exotic optical effect: bending-free refraction. Furthermore, we succeed in developing the first in-plane refractive hyperlens, which yields foci as small as lamdap/6, being lamdap the polariton wavelength (lamda0/50 with respect to the wavelength of light in free space). Our results set the grounds for planar nano-optics in strongly anisotropic media, with potential for unprecedented control of the flow of energy at the nanoscale.

physics.optics↗

arXiv2021

Fizeau Drag in Graphene Plasmonics

Dragging of light by moving dielectrics was predicted by Fresnel and verified by Fizeau's celebrated experiments with flowing water. This momentous discovery is among the experimental cornerstones of Einstein's special relativity and is well understood in the context of relativistic kinematics. In contrast, experiments on dragging photons by an electron flow in solids are riddled with inconsistencies and so far eluded agreement with the theory. Here we report on the electron flow dragging surface plasmon polaritons (SPPs): hybrid quasiparticles of infrared photons and electrons in graphene. The drag is visualized directly through infrared nano-imaging of propagating plasmonic waves in the presence of a high-density current. The polaritons in graphene shorten their wavelength when launched against the drifting carriers. Unlike the Fizeau effect for light, the SPP drag by electrical currents defies the simple kinematics interpretation and is linked to the nonlinear electrodynamics of the Dirac electrons in graphene. The observed plasmonic Fizeau drag enables breaking of time-reversal symmetry and reciprocity at infrared frequencies without resorting to magnetic fields or chiral optical pumping.

cond-mat.mes-hall↗

arXiv2019

Excellent electronic transport in heterostructures of graphene and monoisotopic boron-nitride grown at atmospheric pressure

Hexagonal boron nitride (BN), one of the very few layered insulators, plays a crucial role in 2D materials research. In particular, BN grown with a high pressure technique has proven to be an excellent substrate material for graphene and related 2D materials, but at the same time very hard to replace. Here we report on a method of growth at atmospheric pressure as a true alternative for producing BN for high quality graphene/BN heterostructures. The process is not only more scalable, but also allows to grow isotopically purified BN crystals. We employ Raman spectroscopy, cathodoluminescence, and electronic transport measurements to show the high-quality of such monoisotopic BN and its potential for graphene-based heterostructures. The excellent electronic performance of our heterostructures is demonstrated by well developed fractional quantum Hall states, ballistic transport over distances around $10\,\mathrm{μm}$ at low temperatures and electron-phonon scattering limited transport at room temperature.

cond-mat.mes-hall↗