arXiv subjects

P. James Schuck

Publications and source records attributed to P. James Schuck.

At least 19 recordsLinked to original sources

arXiv2026

All-optical switching of nonlinear structured light in crystal-engineered van der Waals materials

The orbital angular momentum (OAM) of light is a discrete, unbounded degree of freedom that underpins mode-multiplexed communications and high-dimensional quantum photonics. Yet, dynamic OAM control remains dependent on bulky free-space optics or cascaded architectures that separate switching from wavefront shaping, hindering nanoscale integration. Here, we engineer artificial van der Waals crystals from rhombohedrally stacked (3R) MoS$_2$, in which spatial control of the local crystal orientation imprints a nonlinear geometric phase onto the second-harmonic (SH) field, enabling background-free generation of SH vortex beams in an ultrathin (46 nm) van der Waals platform. Leveraging the C$_{3v}$ symmetry of 3R-MoS$_2$, we demonstrate monolithic, all-optical switching with sub-optical-cycle precision between Hermite-Gauss-like and Laguerre-Gaussian vortex SH beams with opposite topological charges ($l=\pm1$). Our results establish artificial 3R-MoS$_2$ crystals as a monolithic platform for the generation and all-optical reconfiguration of nonlinear structured light at the nanoscale, advancing active nanophotonic sources for integrated classical and quantum photonic technologies.

physics.optics↗

arXiv2026

Scaling native entanglement generation in layered semiconductors with quasi-phase matching

Efficient generation of entangled photons typically relies on spontaneous parametric down-conversion (SPDC) in phase-matched macroscopic nonlinear media. However, generating entanglement under phase-matching constraints requires additional bulk optics or interferometers. In contrast, ultrathin van der Waals semiconductors - such as transition metal dichalcogenides (TMDs) - exhibit strong enough optical nonlinearities for SPDC to be observed from subwavelength-thick media, thereby bypassing conventional phase-matching constraints. In this microscopic domain, the intrinsic crystal symmetry governs the nonlinear optical response, enabling the native generation of polarization-entangled photon pairs. However, generating these states efficiently has been fundamentally restricted by the material's coherence length ($L_c$), which limits the attainable conversion efficiency. Here, we investigate periodically-poled TMDs (PPTMDs) designed to scale up this interaction via quasi-phase matching. We demonstrate that mechanically flipping the sign of the nonlinearity at precise intervals of $L_c$ introduces quasi-phase matching, that scales the pair-production rate while preserving the pristine, symmetry-generated polarization entanglement, with fidelities exceeding 99%. Backed by a rigorous theoretical model, our work clarifies the interplay between crystal symmetry and propagation effects in thin nonlinear media, providing a new avenue for engineering quantum light in nanophotonic systems.

quant-ph↗

arXiv2026

Giant optical spin-orbit interactions in ferroelectric van der Waals waveguides

Optical spin-orbit interactions (SOI) link photonic spin to momentum, offering a route toward on-chip polarization control and beam steering. Nevertheless, achieving sufficient optical SOI and nonlinearities on sub-micrometer scales - a prerequisite for dense photonic integration - remains an outstanding challenge. Here, we show that highly birefringent van der Waals (vdW) waveguides provide an ideal, chip-compatible platform to address this limitation. We focus on the ferroelectric semiconductor NbOI2, which exhibits record optical nonlinearities and dielectric anisotropy. Using femtosecond optical microscopy, we image light propagation and harmonic conversion beyond the total internal reflection barrier over tens of micrometers in NbOI2 slab waveguides. We report giant optical spin-splitting through the optical spin Hall effect, which facilitates spatial separation of optical spin currents on sub-micrometer scales, in quantitative agreement with a microscopic light-matter interaction model. We further leverage optical spin-momentum locking to realize polarization-controlled waveguide steering. We generalize these observations across various vdW waveguides and empirically confirm a scaling law linking dielectric anisotropy to geometric spin-splitting. Our results establish highly anisotropic vdW waveguides as an ideal platform for densely integrated opto-spintronic technologies.

cond-mat.mtrl-sci↗

arXiv2026

Polar enhancement of optical nonlinearities and domain-driven second harmonic contrast in bismuth telluro-halide van der Waals crystals

The BiTeX family of polar van der Waals (vdW) semiconductors offers a unique platform for exploring the interplay between polar crystalline structure and nonlinear optical phenomena. Here, we utilize second harmonic generation (SHG) polarimetry to demonstrate giant anisotropic optical nonlinearities in BiTeBr and BiTeI driven by contributions to the crystals' nonlinear polarizability originating from their permanent dipole moment. In addition, using SHG microscopy, we show that BiTeI displays a distinctive SHG spatial texture consisting of thread-like regions of reduced harmonic intensity. These features demark the boundaries between phase and anti-phase polar domains, confirmed via piezoresponse force microscopy and are attributable to disorder-driven restoration of inversion symmetry and concomitant optical interference effects. Our results unveil the power of polarization-resolved SHG microscopy in elucidating the intricate relationship between structure, symmetry, and nonlinear optical responses in polar vdW materials and highlight the promise of BiTeX as a material platform for domain-engineered nanoscale nonlinear photonics.

physics.optics↗

arXiv2025

Purcell enhancement of photogalvanic currents in a van der Waals plasmonic self-cavity

Cavities provide a means to manipulate the optical and electronic responses of quantum materials by selectively enhancing light-matter interaction at specific frequencies and momenta. While cavities typically involve external structures, exfoliated flakes of van der Waals (vdW) materials can form intrinsic self-cavities due to their small finite dimensions, confining electromagnetic fields into plasmonic cavity modes, characterized by standing-wave current distributions. While cavity-enhanced phenomena are well-studied at optical frequencies, the impact of self-cavities on nonlinear electronic responses--such as photogalvanic currents--remains largely unexplored, particularly in the terahertz regime, critical for emerging ultrafast optoelectronic technologies. Here, we report a self-cavity-induced Purcell enhancement of photogalvanic currents in the vdW semimetal WTe$_2$. Using ultrafast optoelectronic circuitry, we measured coherent near-field THz emission resulting from nonlinear photocurrents excited at the sample edges. We observed enhanced emission at finite frequencies, tunable via excitation fluence and sample geometry, which we attribute to plasmonic interference effects controlled by the cavity boundaries. We developed an analytical theory that captures the cavity resonance conditions and spectral response across multiple devices. Our findings establish WTe$_2$ as a bias-free, geometry-tunable THz emitter and demonstrate the potential of self-cavity engineering for controlling nonlinear, nonequilibrium dynamics in quantum materials.

cond-mat.mes-hall↗

arXiv2025

Flat band excitons in a three-dimensional supertwisted spiral transition metal dichalcogenide

A new frontier in van der Waals twistronics is the development of three-dimensional (3D) supertwisted materials, where each successive atomic layer rotates by the same angle. While two-dimensional (2D) moire systems have been extensively studied, the unique phenomena arising from 3D twistronics remain largely unexplored. In this work, we report the discovery of flat-band excitons in 3D supertwisted WS2, revealed by systematic photoluminescence (PL) experiments and electronic structure calculations. These excitons retain key features of 2D moire transition metal dichalcogenides (TMDs)-such as layer confinement, moire-driven localization, and strong Coulomb interactions-while also offering advantages in scalability and enhanced optical responses in three dimensions. Beyond the PL signatures reminiscent of 2D A excitons, we observe novel direct and indirect exciton emission uniquely tied to the supertwist geometry. Using generalized Bloch band theory and local density of states calculations that incorporate screw rotational symmetry, we uncovered the coexistence of 2D and 3D flatband gaps. These flat-band excitons serve as sensitive probes of the electronic properties of 3D supertwisted semiconductors and open new pathways for applications in quantum optoelectronics.

physics.app-ph↗

arXiv2025

Van der Waals waveguide quantum electrodynamics probed by infrared nano-photoluminescence

Atomically layered van der Waals (vdW) materials exhibit remarkable properties, including highly-confined infrared waveguide modes and the capacity for infrared emission in the monolayer limit. Here, we engineered structures that leverage both of these nano-optical functionalities. Specifically, we encased a photoluminescing atomic sheet of MoTe2 within two bulk crystals of WSe2, forming a vdW waveguide for the embedded light-emitting monolayer. The modified electromagnetic environment offered by the WSe2 waveguide alters MoTe2 spontaneous emission, a phenomenon we directly image with our interferometric nano-photoluminescence technique. We captured spatially-oscillating nanoscale patterns prompted by spontaneous emission from MoTe2 into waveguide modes of WSe2 slabs. We quantify the resulting Purcell-enhanced emission rate within the framework of a waveguide quantum electrodynamics (QED) model, relating the MoTe2 spontaneous emission rate to the measured waveguide dispersion. Our work marks a significant advance in the implementation of all-vdW QED waveguides.

physics.optics↗

arXiv2025

Quasi-phase-matched up- and down-conversion in periodically poled layered semiconductors

Nonlinear optics lies at the heart of classical and quantum light generation. The invention of periodic poling revolutionized nonlinear optics and its commercial applications by enabling robust quasi-phase-matching in crystals such as lithium niobate. However, reaching useful frequency conversion efficiencies requires macroscopic dimensions, limiting further technology development and integration. Here we realize a periodically poled van der Waals semiconductor (3R-MoS$_2$). Due to its exceptional nonlinearity, we achieve macroscopic frequency conversion efficiency of 0.03% at the relevant telecom wavelength over a microscopic thickness of 3.4$μ$m (that is, 3 poling periods), $10-100\times$ thinner than current systems with similar performances. Due to unique intrinsic cavity effects, the thickness-dependent quasi-phase-matched second harmonic signal surpasses the usual quadratic enhancement by $50\%$. Further, we report the broadband generation of photon pairs at telecom wavelengths via quasi-phase-matched spontaneous parametric down-conversion, showing a maximum coincidence-to-accidental-ratio of $638 \pm 75$. This work opens the new and unexplored field of phase-matched nonlinear optics with microscopic van der Waals crystals, unlocking applications that require simple, ultra-compact technologies such as on-chip entangled photon-pair sources for integrated quantum circuitry and sensing.

physics.optics↗

arXiv2024

Spatiotemporal imaging of nonlinear optics in van der Waals waveguides

Van der Waals (vdW) semiconductors have emerged as promising platforms for efficient nonlinear optical conversion, including harmonic and entangled photon generation. Although major efforts are devoted to integrating vdW materials in nanoscale waveguides for miniaturization, the realization of efficient, phase-matched conversion in these platforms remains challenging. To address this challenge, we develop a far-field ultrafast imaging method to track the propagation of both fundamental and harmonic waves within vdW waveguides with extreme spatiotemporal resolution. Our approach allows systematic optimization of nonlinear conversion by determining the phase-matching angles, mode profiles, and losses in waveguides without a priori knowledge of material properties. We focus on light propagation in slab waveguides of rhombohedral-stacked MoS2, an emerging vdW semiconductor with giant nonlinear susceptibility. Our results reveal that these waveguides support birefringent phase-matching, demonstrating the material's potential for efficient on-chip nonlinear optics. This work establishes spatiotemporal imaging of light propagation in waveguides as an incisive and general method to identify new materials and architectures for efficient nonlinear nanophotonics.

cond-mat.mtrl-sci↗

arXiv2024

Intrinsic Optical Bistability of Photon Avalanching Nanocrystals

Optically bistable materials respond to a single input with two possible optical outputs, contingent upon excitation history. Such materials would be ideal for optical switching and memory, yet limited understanding of intrinsic optical bistability (IOB) prevents development of nanoscale IOB materials suitable for devices. Here, we demonstrate IOB in Nd3+-doped KPb2Cl5 avalanching nanoparticles (ANPs), which switch with high contrast between luminescent and non-luminescent states, with hysteresis characteristic of bistability. We elucidate a nonthermal mechanism in which IOB originates from suppressed nonradiative relaxation in Nd3+ ions and from the positive feedback of photon avalanching, resulting in extreme, >200th-order optical nonlinearities. Modulation of laser pulsing tunes hysteresis widths, and dual-laser excitation enables transistor-like optical switching. This control over nanoscale IOB establishes ANPs for photonic devices in which light is used to manipulate light.

physics.optics↗

arXiv2024

Optical Band Engineering of Monolayer WSe2 in a Scanning Tunneling Microscope

Intense electromagnetic fields can result in dramatic changes in the electronic properties of solids. These changes are commonly studied using optical probes of the modified electronic structure. Here we use optical-scanning tunneling microscopy (optical-STM) equipped with near-field continuous wave (CW) laser excitation to directly measure the electronic structure of light-dressed states in a monolayer transition metal dichalcogenide (TMD) semiconductor, WSe2. We find that the effective tunneling gap and tunneling density of states are strongly influenced by the intensity of the electromagnetic field when the applied field is resonant with the bandgap of the semiconductor. Our findings indicate that CW laser excitation can be used to generate light-dressed electronic states of quantum materials when confined strongly to the nanoscale.

cond-mat.mtrl-sci↗

arXiv2024

Mathematical Optimization of Resolution Improvement in Structured Light data by Periodic Scanning Motion: Application for Feedback during Lunar Landing

This research explores the enhancement of lunar landing precision through an advanced structured light system, integrating machine learning, Iterative Learning Control (ILC) and Structured Illumination Microscopy (SIM) techniques. By employing Moire fringe patterns for high-precision scanning maneuvers, the study addresses the limitations of conventional structured light systems. A nonlinear mathematical optimization model is developed to refine the world model, optimizing oscillation frequency and amplitude to improve resolution. The findings suggest that this approach can double the conventional resolution, promising significant advancements in the accuracy of lunar landings, with potential real-time application.

eess.SY↗

arXiv2024

Increased formation of trions and charged biexcitons by above-gap excitation in single-layer $WSe_2$

Two-dimensional semiconductors exhibit pronounced many-body effects and intense optical responses due to strong coulombic interactions. Consequently, subtle differences in photoexcitation conditions can strongly influence how the material dissipates energy during thermalization. Here, using multiple excitation spectroscopies, we show that a distinct thermalization pathway emerges at elevated excitation energies, enhancing the formation of trions and charged biexcitons in single-layer WSe2 by up to 2x and 5x, respectively. Power- and temperature-dependent measurements lend insight into the origin of the enhancement. These observations underscore the complexity of excited state relaxation in monolayer semiconductors, provide insight for the continued development of carrier thermalization models, and highlight the potential to precisely control excitonic yields and probe non-equilibrium dynamics in 2D semiconductors.

cond-mat.mtrl-sci↗

arXiv2024

Quantum Noise Spectroscopy of Criticality in an Atomically Thin Magnet

Dynamic critical fluctuations in magnetic materials encode important information about magnetic ordering in the associated critical exponents. Using nitrogen-vacancy centers in diamond, we implement $T_2$ (spin-decoherence) noise magnetometry to study critical dynamics in a 2D Van der Waals magnet CrSBr. By analyzing NV decoherence on time scales approaching the characteristic correlation time $τ_c$ of critical fluctuations, we extract the critical exponent $ν$ for the correlation length. Our result deviates from the Ising prediction and highlights the role of long-range dipolar interactions in 2D CrSBr. Furthermore, analyzing the divergence of the correlation length suggests the possibility of 2D-XY criticality in CrSBr in a temperature window near $T_C$ where static magnetic domains are absent. Our work provides a first demonstration of $T_2$ noise magnetometry to quantitatively analyze critical scaling behavior in 2D materials.

cond-mat.mes-hall↗

arXiv2024

Uniaxial plasmon polaritons $\textit{via}$ charge transfer at the graphene/CrSBr interface

Graphene is a privileged 2D platform for hosting confined light-matter excitations known as surface plasmon-polaritons (SPPs), as it possesses low intrinsic losses with a high degree of optical confinement. However, the inherently isotropic optical properties of graphene limit its ability to guide and focus SPPs, making it less suitable than anisotropic elliptical and hyperbolic materials as a platform for polaritonic lensing and canalization. Here, we present the graphene/CrSBr heterostructure as an engineered 2D interface that hosts highly anisotropic SPP propagation over a wide range of frequencies in the mid-infrared and terahertz. Using a combination of scanning tunneling microscopy (STM), scattering-type scanning near-field optical microscopy (s-SNOM), and first-principles calculations, we demonstrate mutual doping in excess of 10$^{13}$ cm$^{-2}$ holes/electrons between the interfacial layers of graphene/CrSBr heterostructures. SPPs in graphene activated by charge transfer interact with charge-induced anisotropic intra- and interband transitions in the interfacial doped CrSBr, leading to preferential SPP propagation along the quasi-1D chains that compose each CrSBr layer. This multifaceted proximity effect both creates SPPs and endows them with anisotropic transport and propagation lengths that differ by an order-of-magnitude between the two in-plane crystallographic axes of CrSBr.

cond-mat.mes-hall↗

arXiv2024

Twisted nonlinear optics in monolayer van der Waals crystals

In addition to a plethora of emergent phenomena, the spatial topology of optical vortices enables an array of applications spanning communications to quantum photonics. Nonlinear optics is essential in this context, providing access to an infinitely large set of quantum states associated with the orbital angular momentum of light. Nevertheless, the realization of such processes have failed to keep pace with the ever-growing need to shrink the fundamental length-scale of photonic technologies to the nanometer regime6. Here, we push the boundaries of vortex nonlinear optics to the ultimate limits of material dimensionality. By exploiting second and third-order frequency-mixing processes in semiconducting monolayers, we demonstrate the independent manipulation of the wavelength, orbital angular momentum, and spatial distribution of vortex light-fields. Due to the atomically-thin nature of the host quantum material, this control spans a broad spectral bandwidth in a highly-integrable platform, unconstrained by the traditional limits of bulk nonlinear optical materials. Our work heralds a new avenue for ultra-compact and scalable hybrid nanotechnologies empowered by twisted nonlinear light-matter interactions in van der Waals quantum nanomaterials.

physics.optics↗

arXiv2024

Infrared nanosensors of pico- to micro-newton forces

Mechanical force is an essential feature for many physical and biological processes.1-12 Remote measurement of mechanical signals with high sensitivity and spatial resolution is needed for diverse applications, including robotics,13 biophysics,14-20 energy storage,21-24 and medicine.25-27 Nanoscale luminescent force sensors excel at measuring piconewton forces,28-32 while larger sensors have proven powerful in probing micronewton forces.33,34 However, large gaps remain in the force magnitudes that can be probed remotely from subsurface or interfacial sites, and no individual, non-invasive sensor is capable of measuring over the large dynamic range needed to understand many systems.35,36 Here, we demonstrate Tm3+-doped avalanching nanoparticle37 force sensors that can be addressed remotely by deeply penetrating near-infrared (NIR) light and can detect piconewton to micronewton forces with a dynamic range spanning more than four orders of magnitude. Using atomic force microscopy coupled with single-nanoparticle optical spectroscopy, we characterize the mechanical sensitivity of the photon avalanching process and reveal its exceptional force responsiveness. By manipulating the Tm3+ concentrations and energy transfer within the nanosensors, we demonstrate different optical force-sensing modalities, including mechanobrightening and mechanochromism. The adaptability of these nanoscale optical force sensors, along with their multiscale sensing capability, enable operation in the dynamic and versatile environments present in real-world, complex structures spanning biological organisms to nanoelectromechanical systems (NEMS).

physics.optics↗

arXiv2023

Highly tunable room-temperature plexcitons in monolayer WSe2 /gap-plasmon nanocavities

The advancement of quantum photonic technologies relies on the ability to precisely control the degrees of freedom of optically active states. Here, we realize real-time, room-temperature tunable strong plasmon-exciton coupling in 2D semiconductor monolayers enabled by a general approach that combines strain engineering plus force- and voltage-adjustable plasmonic nanocavities. We show that the exciton energy and nanocavity plasmon resonance can be controllably toggled in concert by applying pressure with a plasmonic nanoprobe, allowing in operando control of detuning and coupling strength, with observed Rabi splittings >100 meV. Leveraging correlated force spectroscopy, nano-photoluminescence (nano-PL) and nano-Raman measurements, augmented with electromagnetic simulations, we identify distinct polariton bands and dark polariton states, and map their evolution as a function of nanogap and strain tuning. Uniquely, the system allows for manipulation of coupling strength over a range of cavity parameters without dramatically altering the detuning. Further, we establish that the tunable strong coupling is robust under multiple pressing cycles and repeated experiments over multiple nanobubbles. Finally, we show that the nanogap size can be directly modulated via an applied DC voltage between the substrate and plasmonic tip, highlighting the inherent nature of the concept as a plexcitonic nano-electro-mechanical system (NEMS). Our work demonstrates the potential to precisely control and tailor plexciton states localized in monolayer (1L) transition metal dichalcogenides (TMDs), paving the way for on-chip polariton-based nanophotonic applications spanning quantum information processing to photochemistry.

physics.optics↗