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Yueh-Chun Wu

Publications and source records attributed to Yueh-Chun Wu.

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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

Understanding multiscale disorder in superconducting nanowire single photon detectors

Superconducting nanowire single-photon detectors are central to applications across quantum information science. Yet, their performance is limited by the effects of disorder and electrodynamic inhomogeneities that are not well understood. By combining DC transport, dark-count measurements, and bias-dependent microwave transmission spectroscopy in the presence of controlled nanoscale disorder introduced through helium-ion irradiation, we distinguish local instability-driven processes from intrinsic superconducting depairing and kinetic inductance nonlinearities. This approach enables systematic tuning of kinetic inductance, depairing currents, microwave dissipation, and mode structure within a single device. Bias- and temperature-dependent resonance shifts quantify disorder-induced modifications of the superconducting density of states through the nonlinear kinetic inductance, while the emergence of multiple resonant modes reveals the formation of electrodynamically distinct superconducting regions. Comparing depairing under current, field, and temperature isolates the dominant microwave loss mechanisms, separating vortex, quasiparticle, and two-level-system contributions, thus providing a robust multifunctional foundation for disorder engineering of superconducting nanowire detectors and resonators.

quant-ph

Detecting half-quantum superconducting vortices by spin-qubit relaxometry

Half-quantum vortices in spin-triplet superconductors are predicted to harbor Majorana zero modes and may provide a viable avenue to topological quantum computation. Here, we introduce a novel approach for directly measuring the half-integer-quantized magnetic fluxes, $Φ= h / (4e)$, carried by such half-quantum vortices via spin-qubit relaxometry. We consider a superconducting strip with a narrow pinch point at which vortices cross quasi-periodically below a spin qubit as a result of a bias current. We demonstrate that the relaxation rate of the spin qubit exhibits a pronounced peak if the vortex-crossing frequency matches the transition frequency of the spin qubit and conclude that the magnetic flux $Φ$ of a single vortex can be obtained by dividing the corresponding voltage along the strip with the transition frequency. We discuss experimental constraints on implementing our proposed setup in spin-triplet candidate materials like UTe$_2$, UPt$_3$, and URhGe.

cond-mat.supr-con

Sub-Terahertz Spin Relaxation Dynamics of Boron-Vacancy Centers in Hexagonal Boron Nitride

Quantum sensors based on spin-defect relaxation have become powerful tools for detecting faint magnetic signals, yet their operation has remained largely confined to low magnetic fields and gigahertz frequencies. Extending such sensors into high-field ($> 0.3$ T) and sub-terahertz regimes would enable quantum metrology across a wide range of electromagnetic phenomena and scientific applications, but has proven challenging. Here, we demonstrate that negatively charged boron vacancies ($\mathrm{V_B^-}$) in two-dimensional hexagonal boron nitride can function as relaxation-based quantum sensors operating up to 0.2 terahertz. Their uniform spin-orientation and persistent spin-contrast at high fields enable direct measurement of intrinsic spin relaxation across previously unexplored temperature and frequency regimes. We also reveal a crossover in relaxation behavior \textemdash initially decreasing at low fields before rising at higher fields \textemdash consistent with the emergence of single-phonon-induced resonant noise that becomes significant at sub-terahertz frequencies. These results establish $\mathrm{V_B^-}$ centers as a versatile platform for quantum sensing in the sub-terahertz, high-field regime.

quant-ph

Probing the Nanoscale Excitonic Landscape and Quantum Confinement of Excitons in Gated Monolayer Semiconductors

Engineering and probing excitonic properties at the nanoscale remains a central challenge in quantum photonics and optoelectronics. While exciton confinement via electrical control and strain engineering has been demonstrated in 2D semiconductors, substantial nanoscale heterogeneity limits the scalability of 2D quantum photonic device architectures. In this work, we use cathodoluminescence spectroscopy to probe the excitonic landscape of monolayer $WS_2$ under electrostatic gating. Exploiting the high spatial resolution of the converged electron beam, we resolve a homojunction arising between gated and ungated regions. Moreover, we reveal an exciton confinement channel arising from an unconventional doping mechanism driven by the interplay between the electron beam and the applied gate fields. These findings offer new insights into the optoelectronic behavior of monolayer semiconductors under the combined influence of electron-beam excitation and electrostatic gating. Our approach provides a pathway for exciton manipulation at the nanoscale and opens opportunities for controlling quantum-confined exciton transport in two-dimensional materials.

cond-mat.mes-hall

Programmable phase selection between altermagnetic and non-centrosymmetric polymorphs of MnTe on InP via molecular beam epitaxy

Phase selecting nearly degenerate crystalline polymorphs during epitaxial growth can be challenging yet is critical to targeting physical properties for specific applications. Here, we establish how phase selectivity of altermagnetic and non-centrosymmetric polymorphs of MnTe with high structural quality and phase purity can be programmed by subtle changes to the surface of lattice-matched InP substrates in molecular beam epitaxial (MBE) growth. Bulk altermagnetic MnTe is thermodynamically stable in the hexagonal NiAs-structure and is synthesized here on the (111)A surface (In-terminated) of InP, while the non-centrosymmetric, cubic ZnS-structure with wide band gap (> 3eV) is stabilized on the (111)B surface (P-terminated). Here we use electron microscopy, photoemission spectroscopy, and reflection high-energy electron diffraction, which together indicate that the phase selection is triggered at the interface and proceeds along the growing surface. First principles calculations suggest that interfacial termination and strain have a significant effect on the interfacial energy; stabilizing the NiAs polymorph on the In-terminated surface and the ZnS structure on the P-terminated surface. Selectively grown, high-quality films of MnTe polymorphs are key platforms that will enable our understanding of the novel properties of these materials, thereby facilitating their use in new applications ranging from spintronics to microelectronic devices.

cond-mat.mtrl-sci

Raman Fingerprints of Phase Transitions and Ferroic Couplings in Van der Waals Material CuCrP$_2$S$_6$

CuCrP$_2$S$_6$ (CCPS), a type-II multiferroic material, exhibits unique phase transitions involving ferroelectric, antiferroelectric, and antiferromagnetic ordering. In this study, we conduct a comprehensive investigation on the intricate phase transitions and their multiferroic couplings in CCPS across a wide temperature range from 4 to 345 K through Raman spectroscopic measurements down to 5 cm$^{-1}$. We first assign the observed Raman modes with the support of theoretical calculations and angle-resolved polarized Raman measurements. We further present clear signatures of phase transitions from analyses of temperature-dependent Raman spectral parameters. Particularly, two low-frequency soft modes are observed at 36.1 cm$^{-1}$ and 70.5 cm$^{-1}$ below 145 K, indicating the antiferroelectric to quasi-antiferroelectric transition. Moreover, phonon modes hardening is observed when the temperature increases from 4 to 65 K, suggesting negative thermal expansion (NTE) and strong magnetoelastic coupling below 65 K. These findings advance the understanding of vdW multiferroic CCPS, paving the way for future design and engineering of multiferroicity in cutting-edge technologies, such as spintronics and quantum devices.

cond-mat.mtrl-sci

Defect Engineering in Large-Scale CVD-Grown Hexagonal Boron Nitride: Formation, Spectroscopy, and Spin Relaxation Dynamics

Recently, numerous techniques have been reported for generating optically active defects in exfoliated hexagonal boron nitride (hBN), which hold transformative potential for quantum photonic devices. However, achieving on-demand generation of desirable defect types in scalable hBN films remains a significant challenge. Here, we demonstrate that formation of negative boron vacancy defects, VB-, in suspended, large-area CVD-grown hBN is strongly dependent on the type of bombarding particles (ions, neutrons, and electrons) and irradiation conditions. In contrast to suspended hBN, defect formation in substrate-supported hBN is more complex due to the uncontrollable generation of secondary particles from the substrate, and the outcome strongly depends on the thickness of the hBN. We identify different defect types by correlating spectroscopic and optically detected magnetic resonance features, distinguishing boron vacancies (formed by light ions and neutrons) from other optically active defects emitting at 650 nm assigned to anti-site nitrogen vacancy (NBVN) and reveal the presence of additional dark paramagnetic defects that influence spin-lattice relaxation time (T1) and zero-field splitting parameters, all of which strongly depend on the defect density. These results underscore the potential for precisely engineered defect formation in large-scale CVD-grown hBN, paving the way for the scalable fabrication of quantum photonic devices.

cond-mat.mtrl-sci

Highly tunable valley polarization of potential-trapped moiré excitons in WSe2/WS2 heterojunctions

Moiré superlattices created by stacking atomic layers of transition metal dichalcogenide semiconductors have emerged as a class of fascinating artificial photonic and electronic materials. An appealing attribute of these structures is the inheritance of the valley degree of freedom from the constituent monolayers. Recent studies show evidence that the valley polarization of the moiré excitons is highly tunable. In heterojunctions of WSe2/WS2, marked improvement in valley polarization is observed by increasing optical excitation power, a behavior that is quite distinct from the monolayers, and lacks a clear understanding so far. In this work, we show that this highly tunable valley property arises from filling of the moiré superlattice, which provides an intriguing mechanism for engineering these quantum opto-valleytronic platforms. Our data further demonstrate that the long-range electron-hole exchange interaction, despite being significantly weakened in the junctions, is the dominant source of moiré exciton intervalley scattering at low population. Using magnetic field tuning, we quantitatively determine the exchange interaction strength to be 0.03 meV and 0.24 meV for 0- and 60-degrees twisted samples respectively in our experiments, about one order of magnitude weaker than that in the monolayers.

cond-mat.mes-hall

Non-perturbative cathodoluminescence microscopy of beam-sensitive materials

Cathodoluminescence microscopy is now a well-established and powerful tool for probing the photonic properties of nanoscale materials, but in many cases, nanophotonic materials are easily damaged by the electron-beam doses necessary to achieve reasonable cathodoluminescence signal-to-noise ratios. Two-dimensional materials have proven particularly susceptible to beam-induced modifications, yielding both obstacles to high spatial-resolution measurement and opportunities for beam-induced patterning of quantum photonic systems. Here pan-sharpening techniques are applied to cathodoluminescence microscopy in order to address these challenges and experimentally demonstrate the promise of pan-sharpening for minimally-perturbative high-spatial-resolution spectrum imaging of beam-sensitive materials.

physics.optics

Nanoscale magnetic ordering dynamics in a high Curie temperature ferromagnet

Thermally driven transitions between ferromagnetic and paramagnetic phases are characterized by critical behavior with divergent susceptibilities, long-range correlations, and spin dynamics that can span kHz to GHz scales as the material approaches the critical temperature $\mathrm{T_c}$, but it has proven technically challenging to probe the relevant length and time scales with most conventional measurement techniques. In this study, we employ scanning nitrogen-vacancy center based magnetometry and relaxometry to reveal the critical behavior of a high-$\mathrm{T_c}$ ferromagnetic oxide near its Curie temperature. Cluster analysis of the measured temperature-dependent nanoscale magnetic textures points to a 3D universality class with a correlation length that diverges near $\mathrm{T_c}$. Meanwhile, the temperature-dependent spin dynamics, measured through all optical relaxometry suggest that the phase transition is in the XY universality class. Our results capture both static and dynamic aspects of critical behavior, providing insights into universal properties that govern phase transitions in magnetic materials.

cond-mat.mtrl-sci

Axial Higgs Mode Detected by Quantum Pathway Interference in RTe3

The observation of the Higgs boson solidified the standard model of particle physics. However, explanations of anomalies (e.g. dark matter) rely on further symmetry breaking calling for an undiscovered axial Higgs mode. In condensed matter the Higgs was seen in magnetic, superconducting and charge density wave(CDW) systems. Uncovering a low energy mode's vector properties is challenging, requiring going beyond typical spectroscopic or scattering techniques. Here, we discover an axial Higgs mode in the CDW system RTe3 using the interference of quantum pathways. In RTe3 (R=La,Gd), the electronic ordering couples bands of equal or different angular momenta. As such, the Raman scattering tensor associated to the Higgs mode contains both symmetric and antisymmetric components, which can be excited via two distinct, but degenerate pathways. This leads to constructive or destructive interference of these pathways, depending on the choice of the incident and Raman scattered light polarization. The qualitative behavior of the Raman spectra is well-captured by an appropriate tight-binding model including an axial Higgs mode. The elucidation of the antisymmetric component provides direct evidence that the Higgs mode contains an axial vector representation (i.e. a pseudo-angular momentum) and hints the CDW in RTe3 is unconventional. Thus we provide a means for measuring collective modes quantum properties without resorting to extreme experimental conditions.

physics.optics

Enhancement of Exciton Valley Polarization in Monolayer MoS2 Induced by Scattering

We report on scattering induced valley polarization enhancement in monolayer molybdenum disulfide. With thermally activated and charge doping introduced scattering, our sample exhibits seven? and twelve-folds of improvements respectively. This counter-intuitive effect is attributed to disruptions to valley pseudospin precession caused by rapid modulation of exciton momentum and concomitant local exchange interaction field, at time scales much shorter than the precession period. In contrast, the valley coherence is improved by thermally activated scattering, but not by charge doping induced scattering. We propose that this is due to anisotropic pseudospin scattering and generalize the Maialle-Silva-Sham model to quantitatively explain our experimental results. Our work illustrates that cleaner samples with minimal scattering, such as those carefully suspended or protected by hexagonal boron nitride, do not necessarily lead to good valley polarization. Well-controlled scattering can in fact provide an interesting approach for improving valleytronic devices.

physics.optics

Probing the bright exciton state in twisted bilayer graphene via resonant Raman scattering

The band structure of bilayer graphene is tunable by introducing a relative twist angle between the two layers, unlocking exotic phases, such as superconductor and Mott insulator, and providing a fertile ground for new physics. At intermediate twist angles around 10°, highly degenerate electronic transitions hybridize to form excitonic states, a quite unusual phenomenon in a metallic system. We probe the bright exciton mode using resonant Raman scattering measurements to track the evolution of the intensity of the graphene Raman G peak, corresponding to the E2g phonon. By cryogenically cooling the sample, we are able to resolve both the incoming and outgoing resonance in the G peak intensity evolution as a function of excitation energy, a prominent manifestation of the bright exciton serving as the intermediate state in the Raman process. For a sample with twist angle 8.6°, we report a weakly temperature dependent resonance broadening $γ$ ${\approx}$ 0.07 eV. In the limit of small inhomogeneous broadening, the observed $γ$ places a lower bound for the bright exciton scattering lifetime at 10 fs in the presence of charges and excitons excited by the light pulse for Raman measurement, limited by the rapid exciton-exciton and exciton-charge scattering in graphene.

cond-mat.mes-hall

Up- and Down-Conversion between Intra- and Inter-Valley Excitons in Waveguide Coupled Monolayer WSe2

The presence of two spin-split valleys in monolayer (1L) transition metal dichalcogenide (TMD) semiconductors supports versatile exciton species classified by their spin and valley quantum numbers. While the spin-0 intravalley exciton, known as the "bright" exciton, is readily observable, other types of excitons, such as the spin-1 intravalley (spin-dark) and spin-0 intervalley (momentum-dark) excitons, are more difficult to access. Here we develop a waveguide coupled 1L tungsten diselenide (WSe2) device to probe these exciton species. In particular, TM coupling to the atomic layer's out-of-plane dipole moments enabled us to not only efficiently collect, but also resonantly populate the spin-1 dark excitons, promising for developing devices with long valley lifetimes. Our work reveals several upconversion processes that bring out an intricate coupling network linking spin-0 and spin-1 intra- and inter-valley excitons, demonstrating that intervalley scattering and spin-flip are very common processes in the atomic layer. These experimental results deepen our understanding of tungsten diselenide exciton physics and illustrate that planar photonic devices are capable of harnessing versatile exciton species in TMD semiconductors.

cond-mat.mes-hall

Ground and Excited Exciton Polarons in Monolayer MoSe2

Monolayer transition metal dichalcogenide semiconductors, with versatile experimentally accessible exciton species, offer an interesting platform for investigating the interaction between excitons and a Fermi sea of charges. Using hexagonal boron nitride encapsulated monolayer MoSe2, we study the impact of charge density tuning on the ground and excited Rydberg states in the atomic layer. Consistent excitonpolaron behavior is revealed in both photoluminescence and reflection spectra of the A exciton 1s (A:1s) Rydberg state, in contrast to previous studies. The A:2s Rydberg state provides an opportunity to understand such interactions with greatly reduced exciton binding energy. We found that the impact of the Fermi sea becomes much more dramatic. With a photoluminescence upconversion technique, we further verify the 2s polaron-like behavior for the repulsive branch of B:2s exciton whose energy is well above the bare bandgap. Our studies show that the polaron-like interaction features are quite generic and highly robust, offering key insights into the dressed manybody state in a Fermi sea.

cond-mat.mes-hall

Environment-insensitive and gate-controllable photocurrent enabled by bandgap engineering of MoS2 junctions

Two-dimensional (2D) materials are composed of atomically thin crystals with an enormous surface-to-volume ratio, and their physical properties can be easily subjected to the change of the chemical environment. Encapsulation with other layered materials, such as hexagonal boron nitride, is a common practice; however, this approach often requires inextricable fabrication processes. Alternatively, it is intriguing to explore methods to control transport properties in the circumstance of no encapsulated layer. This is very challenging because of the ubiquitous presence of adsorbents, which can lead to charged-impurity scattering sites, charge traps, and recombination centers. Here, we show that the short-circuit photocurrent originated from the built-in electric field at the MoS2 junction is surprisingly insensitive to the gaseous environment over the range from a vacuum of 1X10^(-6) Torr to ambient condition. The environmental insensitivity of the short-circuit photocurrent is attributed to the characteristic of the diffusion current that is associated with the gradient of carrier density. Conversely, the photocurrent with bias exhibits typical persistent photoconductivity and greatly depends on the gaseous environment. The observation of environment-insensitive short-circuit photocurrent demonstrates an alternative method to design device structure for 2D-material-based optoelectronic applications.

cond-mat.mes-hall

Extrinsic Origin of Persistent Photoconductivity in Monolayer MoS2 Field Effect Transistors

Recent discoveries of the photoresponse of molybdenum disulfide (MoS2) have shown the considerable potential of these two-dimensional transition metal dichalcogenides for optoelectronic applications. Among the various types of photoresponses of MoS2, persistent photoconductivity (PPC) at different levels has been reported. However, a detailed study of the PPC effect and its mechanism in MoS2 is still not available, despite the importance of this effect on the photoresponse of the material. Here, we present a systematic study of the PPC effect in monolayer MoS2 and conclude that the effect can be attributed to random localized potential fluctuations in the devices. Notably, the potential fluctuations originate from extrinsic sources based on the substrate effect of the PPC. Moreover, we point out a correlation between the PPC effect in MoS2 and the percolation transport behavior of MoS2. We demonstrate a unique and efficient means of controlling the PPC effect in monolayer MoS2, which may offer novel functionalities for MoS2-based optoelectronic applications in the future.

cond-mat.mes-hall