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James H. Edgar

Publications and source records attributed to James H. Edgar.

At least 19 recordsLinked to original sources

Enabling Electrical Readout of Néel vector reversal in a van der Waals Antiferromagnet

Owing to its robustness against external perturbations and intrinsically ultrafast dynamics, the Néel vector in antiferromagnets (AFMs) can enable the development of next-generation spintronic and magnonic devices for memory and computing applications. To realize AFM-based magnetic memory devices, one of the key requirements is to demonstrate electrical readout of 180-degree reversal of Néel vector in thin film AFMs, which remains critically missing. In this work, we report experimental demonstration of a novel transport methodology to detect Néel vector reversal in atomically thin films of a van der Waals (vdW) based A-type AFM. For this, we utilize spin-dependent electronic band properties of CrSBr by coupling it to a spin-polarized layer, separated by a tunnel barrier. In this configuration, the spin-dependent tunnelling magnetoresistance (MR) becomes sensitive to the relative orientation between the magnetization of the reference electrode and the interfacial sublattice magnetization of the AFM layer, in turn enabling electrical detection of the Néel vector orientation. Importantly, the observed MR can also reveal 180-degree reversal of Néel vector in even-layers of CrSBr, wherein adjacent sublattice magnetic layers are exactly compensated and the net magnetization vanishes and thus establishes a broadly applicable strategy for electrical detection of Néel vector in vdW-based AFMs.

cond-mat.mes-hall

Observation and Control of Spontaneous Magnon Emission from Spin Ensembles in 2D Hexagonal Boron Nitride

Hybrid systems consisting of color centers and magnetic materials provide an appealing solid-state platform for advancing the burgeoning quantum technological revolution. Exploring novel coupling mechanisms between optically active spin defects and quantum degrees of freedom is directly relevant in this context. Here, we report observation and control of spontaneous magnon emission from boron-vacancy centers in 2D hexagonal boron nitride (hBN), an unconventional qubit-magnon dipole coupling channel that dominates in the near-zero temperature limit. The spontaneous magnon emission process starts to be overshadowed by thermal magnon effect as temperature increases, reflecting the crossover from an emission-dominated, effectively cold magnon reservoir to a thermally occupied spin bath where absorption and stimulated processes restore balance. By increasing the spin defect density, we further present that spontaneous magnon emission into a common spin bath could help establish quantum correlations in dense hBN spin ensembles. Our results are quantitatively captured by detailed theoretical modeling, bringing insights into understanding qubit-magnon coupling, correlated spin dynamics, and many-body physics of color centers in the quantum regime.

cond-mat.mes-hall

Signatures of quantum chaos in phonon-polariton billiards

We use scanning near-field optical microscopy to image hyperbolic phonon polaritons in hexagonal boron nitride (hBN) billiards with integrable and chaotic geometries. In Sinai billiards, we observe irregular mode patterns consistent with quantum scarring, together with an unexpected sensitivity to weak probe perturbations. These random-wave features coexist with non-chaotic one-dimensional boundary modes arising from nontrivial polariton reflection at the billiard edge. As the billiard boundary becomes increasingly complex, the Fourier transforms of the measured signals evolve toward ring-like structures consistent with Berry's random-wave conjecture. We develop a numerical framework based on the Helmholtz equation with generalized boundary conditions that encode angle-dependent reflection phase shifts. The calculated level statistics exhibit a crossover from Poisson-like behavior in integrable billiards to Wigner-Dyson-like behavior in chaotic geometries, with small deviations from the canonical form arising from nonlinear boundary conditions that require self-consistent bulk-boundary analysis. Theoretical analysis based on dissipative Green's functions qualitatively reproduces the near-field data. These results establish mesoscopic van der Waals billiards as a rich platform for studying generalized chaotic dynamics of hybrid light-matter polaritons.

cond-mat.mes-hall

Fröhlich-type Polarons in Isotopically Enriched Hexagonal Boron Nitride

Exciton-phonon interactions play a central role in defining the optical response of hexagonal boron nitride (hBN), yet their quantitative determination has remained incomplete. Here, we reveal the Fröhlich-type exciton-phonon coupling in boron-10-enriched hBN using low-temperature cathodoluminescence. We resolve the indirect exciton 5.95$\pm$0.02 eV together with its longitudinal optical (LO) phonon replica detuned by 184$\pm$56 meV, enabling the extraction of a Fröhlich coupling constant $α$=0.159 and a larger exciton binding energy of 161 meV, larger than previously reported values for natural-abundance hBN, which is attributed to isotope enrichment. The inferred polaron radius exceeds the lattice constant, indicating large-polaron behavior. We deduced an exciton scattering time ~of 97 fs, corresponding to a homogeneous linewidth of ~6.76 meV. We further obtain a polaron binding energy of ~48 meV and an effective mass of 1.045 $m_0$. These results provide a direct quantitative characterization of exciton-phonon coupling in isotopically engineered hBN and establish a foundation for tailoring its phonon-polaritonic and quantum-optical properties.

cond-mat.mes-hall

Quantum sensing with a spin ensemble in a two-dimensional material

Quantum sensing with solid-state spin defects has transformed nanoscale metrology, offering sub-wavelength spatial resolution with exceptional sensitivity to multiple signal types. Maximizing these advantages requires minimizing both the sensor-target separation and the detectable signal threshold. However, leading platforms such as nitrogen-vacancy (NV) centers in diamond suffer from performance degradation near surfaces or in nanoscale volumes, motivating the search for optically addressable spin sensors in atomically thin, two-dimensional (2D) van der Waals materials. Here, we present a comprehensive experimental framework to probe a 2D spin ensemble, including its Hamiltonian, coherent sensing dynamics, and noise environment. Using a central spin system in a hexagonal boron nitride (hBN) crystal, we fully map the hyperfine interactions with proximal nuclear spins, demonstrate switchable magnetic and electric noise sensing, and introduce a method to accurately reconstruct the environmental noise spectrum while explicitly accounting for quantum control imperfections. We achieve a record coherence time of $80~μ\mathrm{s}$ under dynamical decoupling, enabling sub-microtesla AC magnetic sensitivity at a $10~\mathrm{nm}$ target distance. Leveraging the broad opportunities for defect engineering in atomically thin hosts, these results lay the foundation for next-generation quantum sensors with ultrahigh sensitivity, tunable noise selectivity, and versatile functionalities.

quant-ph

Probing Azimuthal Anatomy of Hyperbolic Whispering Gallery Modes in hBN

Scattering-type scanning near-field optical microscopy (s-SNOM) is a powerful tool for investigating polaritonic modes. However, an inherent limitation of this technique is that excitation and detection occur at the same location. This constraint makes it challenging to resolve excitations with complex spatial structures, which can exhibit delicate dependence on the in-coupling conditions. Here, we present a strategy to overcome this limitation by introducing an auxiliary cavity, which serves as a stationary near-field excitation source. This configuration allows the s-SNOM tip to act solely as a detector, and decouples excitation from detection. We apply this approach to whispering gallery modes (WGMs) of hyperbolic phonon-polaritons in hexagonal boron nitride resonators. Through spatially resolved near-field maps we directly observe subwavelength polaritonic WGMs with large and discrete azimuthal momentum ($k_ϕ/ k_0$ up to 15). This allows us to map the frequency and angular behavior of the modes. Notably, we observe dynamic tuning of the effective refractive index by the WGMs to preserve consistent azimuthal momentum \(k_ϕ\) under varying excitation conditions. Numerical simulations support the experimental observations and confirm the observation of hyperbolic WGMs. This approach enables direct visualization of previously hidden mode structures in hyperbolic cavities and opens new pathways for momentum-controlled polaritonic device engineering.

cond-mat.mes-hall

Probing Boron Vacancy Defects in hBN via Single Spin Relaxometry

Spin defects in solids offer promising platforms for quantum sensing and memory due to their long coherence times and optical addressability. Here, we integrate a single nitrogen-vacancy (NV) center in diamond with scanning probe microscopy to discover, read out, and spatially map arbitrary spin-based quantum sensors at the nanoscale. Using the boron vacancy ($\mathrm{V}_\mathrm{B}^-$) center in hexagonal boron nitride$\unicode{x2013}$an emerging two-dimensional spin system$\unicode{x2013}$as a model, we detect its electron spin resonance indirectly via changes in the spin relaxation time ($T_1$) of a nearby NV center, eliminating the need for optical excitation or fluorescence detection of the $\mathrm{V}_\mathrm{B}^-$. Cross-relaxation between NV and $\mathrm{V}_\mathrm{B}^-$ ensembles significantly reduces NV $T_1$, enabling quantitative nanoscale mapping of defect densities beyond the optical diffraction limit and clear resolution of hyperfine splitting in isotopically enriched h$^{10}$B$^{15}$N. Our method demonstrates interactions between 3D and 2D spin sensors, establishing NV centers as versatile probes for characterizing otherwise inaccessible spin defects.

cond-mat.mtrl-sci

Landau Zener Interaction Enhanced Quantum Sensing in Spin Defects of Hexagonal Boron Nitride

Negatively charged boron vacancies (V$_{\text{B}}^{-}$) in hexagonal boron nitride (hBN) comprise a promising quantum sensing platform, optically addressable at room temperature and transferrable onto samples. However, broad hyperfine-split spin transitions of the ensemble pose challenges for quantum sensing with conventional resonant excitation due to limited spectral coverage. While isotopically enriched hBN using $^{10}$B and $^{15}$N isotopes (h$^{10}$B$^{15}$N) exhibits sharper spectral features, significant inhomogeneous broadening persists. We demonstrate that, implemented via frequency modulation on an FPGA, a frequency-ramped microwave pulse achieves around 4-fold greater $|0\rangle\rightarrow|-1\rangle$ spin-state population transfer and thus contrast than resonant microwave excitation and thus 16-fold shorter measurement time for spin relaxation based quantum sensing. Quantum dynamics simulations reveal that an effective two-state Landau-Zener model captures the complex relationship between population inversion and pulse length with relaxations incorporated. Our approach is robust and valuable for quantum relaxometry with spin defects in hBN in noisy environments.

quant-ph

Non-radiative energy transfer between boron vacancies in hexagonal boron nitride and other 2D materials

Boron vacancies ($V_B^-$) in hexagonal boron nitride (hBN) have emerged as a promising platform for two-dimensional quantum sensors capable of operating at atomic-scale proximity. However, the mechanisms responsible for photoluminescence quenching in thin hBN sensing layers when placed in contact with absorptive materials remain largely unexplored. In this Letter, we investigate non-radiative F\"orster resonance energy transfer (FRET) between $V_B^-$ centers and either monolayer graphene or 2D semiconductors. Strikingly, we find that the FRET rate is negligible for hBN sensing layers thicker than 3 nm, highlighting the potential of $V_B^-$ centers for integration into ultra-thin quantum sensors within van der Waals heterostructures. Furthermore, we experimentally extract the intrinsic radiative decay rate of $V_B^-$ defects.

cond-mat.mtrl-sci

Water induced bandgap engineering in nanoribbons of hexagonal boron nitride

Different from hexagonal boron nitride (hBN) sheets, the bandgap of hBN nanoribbons (BNNRs) can be changed by spatial/electrostatic confinement. It has been predicted that a transverse electric field can narrow the bandgap and even cause an insulator-metal transition in BNNRs. However, experimentally introducing an overhigh electric field across the BNNR remains challenging. Here, we theoretically and experimentally demonstrate that water adsorption greatly reduces bandgap of zigzag oriented BNNRs (zBNNRs). Ab initio calculations show that water adsorbed beside the BNNR induces a transverse equivalent electric field of over 2 V/nm thereby reducing its bandgap. Field effect transistors were successfully fabricated from zBNNRs with different widths. The conductance of zBNNRs with adsorbates of water could be tuned over 3 orders in magnitude via electrical field modulation at room temperature. Furthermore, photocurrent response measurements were taken to determine the optical bandgap in zBNNR. Wider zBNNRs exhibit a bandgap down to 1.17 eV. This study yields fundamental insights in new routes toward realizing electronic/optoelectronic devices and circuits based on hexagonal boron nitride.

cond-mat.mtrl-sci

Isofrequency spin-wave imaging using color center magnetometry for magnon spintronics

Magnon spintronics aims to harness spin waves in magnetic films for information technologies. Color center magnetometry is a promising tool for imaging spin waves, using electronic spins associated with atomic defects in solid-state materials as sensors. However, two main limitations persist: the magnetic fields required for spin-wave control detune the sensor-spin detection frequency, and this frequency is further restricted by the color center nature. Here, we overcome these limitations by decoupling the sensor spins from the spin-wave control fields -selecting color centers with intrinsic anisotropy axes orthogonal to the film magnetization- and by using color centers in diamond and hexagonal boron nitride to operate at complementary frequencies. We demonstrate isofrequency imaging of field-controlled spin waves in a magnetic half-plane and show how intrinsic magnetic anisotropies trigger bistable spin textures that govern spin-wave transport at device edges. Our results establish color center magnetometry as a versatile tool for advancing spin-wave technologies.

cond-mat.mes-hall

Cavity-altered superconductivity

Is it feasible to alter the ground state properties of a material by engineering its electromagnetic environment? Inspired by theoretical predictions, experimental realizations of such cavity-controlled properties without optical excitation are beginning to emerge. Here, we devised and implemented a novel platform to realize cavity-altered materials. Single crystals of hyperbolic van der Waals (vdW) compounds provide a resonant electromagnetic environment with enhanced density of photonic states and prominent mode confinement. We interfaced hexagonal boron nitride (hBN) with the molecular superconductor $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br ($κ$-ET). The frequencies of infrared (IR) hyperbolic modes of hBN match the IR-active carbon-carbon stretching molecular resonance of ($κ$-ET) implicated in superconductivity. Nano-optical data supported by first-principles molecular Langevin dynamics simulations confirm the presence of resonant coupling between the hBN hyperbolic cavity modes and the carbon-carbon stretching mode in ($κ$-ET). Meissner effect measurements via magnetic force microscopy demonstrate a strong suppression of superfluid density near the hBN/($κ$-ET) interface. Non-resonant control heterostructures, including RuCl$_3$/($κ$-ET) and hBN/$\text{Bi}_2\text{Sr}_2\text{CaCu}_2\text{O}_{8+x}$, do not display the superfluid suppression. These observations suggest that hBN/($κ$-ET) realizes a cavity-altered superconducting ground state. Our work highlights the potential of dark cavities devoid of external photons for engineering electronic ground state properties of complex quantum materials.

cond-mat.supr-con

Coherent control of nitrogen nuclear spins via the V$_B^-$-center in hexagonal boron nitride

Charged boron vacancies (V$_\text{B}^-$) in hexagonal boron nitride (hBN) have emerged as a promising platform for quantum nanoscale sensing and imaging. While these primarily involve electron spins, nuclear spins provide an additional resource for quantum operations. This work presents a comprehensive experimental and theoretical study of the properties and coherent control of the nearest-neighbor $^{15}$N nuclear spins of V$_\text{B}^-$-ensembles in isotope-enriched h$^{10}$B$^{15}$N. Multi-nuclear spin states are selectively addressed, enabled by state-specific nuclear spin transitions arising from spin-state mixing. We perform Rabi driving between selected state pairs, define elementary quantum gates, and measure longer than 10~$μ$s nuclear Rabi coherence times. We observe a two orders of magnitude nuclear g-factor enhancement that underpins fast nuclear spin gates. Accompanying numerical simulations provide a deep insight into the underlying mechanisms. These results establish the foundations for leveraging nuclear spins in V$_\text{B}^-$ center-based quantum applications, particularly for extending coherence times and enhancing the sensitivity of 2D quantum sensing foils.

cond-mat.mtrl-sci

Probing the Linewidth of the 12.4-keV Solid-State $^{45}$Sc Isomeric Resonance

The $^{45}$Sc nuclear transition from the ground to the isomeric state at 12.389~keV, with a lifetime of 0.46~s, exhibits an extraordinarily narrow natural width of 1.4~feV and a quality factor $\simeq 10^{19}$ -- surpassing those of the most precise atomic clocks -- making $^{45}$Sc a compelling platform for advanced metrology and nuclear clocks. Here we investigate how closely the spectral width and quality factor of the solid-state $^{45}$Sc resonance can approach these natural limits. Using the European X-ray Free-Electron Laser, we confirm the isomer's lifetime via time-delayed incoherent $K_{α,β}$ fluorescence and observe previously unreported elastic fluorescence, yielding a partial internal conversion coefficient of 390(60). The absence of a clear nuclear forward scattering signal beyond a 2-ms delay implies environmental broadening of at least $500~Γ_{0}$ under experimental conditions, placing bounds on solid-state decoherence mechanisms. These findings set new experimental benchmarks for solid-state nuclear clock development.

quant-ph

Topologically Protected Polaritonic Bound State in the Continuum

Bound states in the continuum (BICs) have emerged as powerful tools to realize ultra-high-Q resonances in nanophotonics. While previous implementations have primarily relied on dielectric metasurfaces, their optical confinement remains fundamentally limited by diffraction. In this work, we theoretically and numerically demonstrate and experimentally validate the existence of topologically protected phonon-polaritonic BICs in periodic arrays of cylindrical nanoresonators composed of isotopically enriched hexagonal boron nitride (h11BN), which support two restrahlen bands (lower (type-I) and upper (type II)), with the present work focusing on the lower Reststrahlen band (RB-1). Owing to the uniaxial anisotropy of hBN and the rotational symmetry of the structure, these systems support topologically symmetry-protected BICs at the {\Gamma}-point, where radiative losses are suppressed. The total quality factor is ultimately bounded by the intrinsic phonon damping of h11BN, enabling high-Q polaritonic modes with minimal radiation leakage. When cylindrical symmetry is broken via angular tilting of incident light away from normal incidence, these BICs transition into quasi-BICs (q-BICs), with strong field confinement and tunable radiation leakage. Their topological features enable robust control over mode lifetimes and confinement, paving the way towards scalable polaritonic platforms for mid-infrared optoelectronics, sensing and quantum nanophotonics.

physics.optics

The Transmission Line Model for 2D Materials and van der Waals Heterostructures

Van der Waals heterostructures (VdWHs) composed of 2D materials have attracted significant attention in recent years due to their intriguing optical properties, such as strong light-matter interactions and large intrinsic anisotropy. In particular, VdWHs support a variety of polaritons-hybrid quasiparticles arising from the coupling between electromagnetic waves and material excitations-enabling the confinement of electromagnetic radiation to atomic scales. The ability to predict and simulate the optical response of 2D materials heterostructures is thus of high importance, being commonly performed until now via methods such as the TMM, or Fresnel equations. While straight forward, these often yield long and complicated expressions, limiting intuitive and simple access to the underlying physical mechanisms that govern the optical response. In this work, we demonstrate the adaptation of the transmission line model for VdWHs, based on expressing its constituents by distributed electrical circuit elements described by their admittance. Since the admittance carries fundamental physical meaning of the material response to electromagnetic fields, the approach results in a system of propagating voltage and current waves, offering a compact and physically intuitive formulation that simplifies algebraic calculations, clarifies the conditions for existence of physical solutions, and provides valuable insight into the fundamental physical response. To demonstrate this, we derive the transmission line analogs of bulk to monolayer 2D materials and show it can be used to compute the reflection/transmission coefficients, polaritonic dispersion relations, and electromagnetic field distributions in a variety of VdWHs, and compare them to experimental measurements yielding very good agreement. This method provides a valuable tool for exploring and understanding the optical response of layered 2D systems.

physics.optics

Magnetization Dependent In-plane Anomalous Hall Effect in a Low-dimensional System

Anomalous Hall Effect (AHE) response in magnetic systems is typically proportional to an out-of-plane magnetization component because of the restriction imposed by system symmetries, which demands that the magnetization, applied electric field, and induced Hall current are mutually orthogonal to each other. Here, we report experimental realization of an unconventional form of AHE in a low-dimensional heterostructure, wherein the Hall response is not only proportional to the out-of-plane magnetization component but also to the in-plane magnetization component. By interfacing a low-symmetry topological semimetal (TaIrTe4) with the ferromagnetic insulator (Cr2Ge2Te6), we create a low-dimensional magnetic system, where only one mirror symmetry is preserved. We show that as long as the magnetization has a finite component in the mirror plane, this last mirror symmetry is broken, allowing the emergence of an AHE signal proportional to in-plane magnetization. Our experiments, conducted on multiple devices, reveal a gate-voltage-dependent AHE response, suggesting that the underlying mechanisms responsible for the Hall effect in our system can be tuned via electrostatic gating. A minimal microscopic model constrained by the symmetry of the heterostructure shows that both interfacial spin-orbit coupling and time-reversal symmetry breaking via the exchange interaction from magnetization are responsible for the emergence of the in-plane AHE. Our work highlights the importance of system symmetries and exchange interaction in low-dimensional heterostructures for designing novel and tunable Hall effects in layered quantum systems.

cond-mat.mes-hall

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