arXiv subjects

P. James Schuck

Publications and source records attributed to P. James Schuck.

At least 37 records · Page 2Linked to original sources

arXiv2023

A generalized approach to photon avalanche upconversion in luminescent nanocrystals

Photon avalanching nanoparticles (ANPs) exhibit extremely nonlinear upconverted emission valuable for sub-diffraction imaging, nanoscale sensing, and optical computing. Avalanching has been demonstrated with Tm3+, Nd3+ or Pr3+-doped nanocrystals, but their emission is limited to 600 and 800 nm, restricting applications. Here, we utilize Gd3+-assisted energy migration to tune the emission wavelengths of Tm3+-sensitized ANPs and generate highly nonlinear emission of Eu3+, Tb3+, Ho3+, and Er3+ ions. The upconversion intensities of these spectrally discrete ANPs scale with the nonlinearity factor s = 10-17 under 1064 nm excitation at power densities as low as 6 kW/cm2. This strategy for imprinting avalanche behavior on remote emitters can be extended to fluorophores adjacent to ANPs, as we demonstrate with CdS/CdSe/CdS core/shell/shell quantum dots. ANPs with rationally designed energy transfer networks provide the means to transform conventional linear emitters into a highly nonlinear ones, expanding the use of photon avalanching in biological, chemical, and photonic applications.

physics.optics↗

arXiv2023

Programmable Nanowrinkle-Induced Room-Temperature Exciton Localization in Monolayer WSe2

Localized states in two-dimensional (2D) transition metal dichalcogenides (TMDCs) have been the subject of intense study, driven by potential applications in quantum information science. Despite the rapidly growing knowledge surrounding these emitters, their microscopic nature is still not fully understood, limiting their production and application. Motivated by this challenge, and by recent theoretical and experimental evidence showing that nanowrinkles generate localized room-temperature emitters, we demonstrate a method to intentionally induce wrinkles with collections of stressors, showing that long-range wrinkle direction and position are controllable with patterned array design. Nano-photoluminescence (nano-PL) imaging combined with detailed strain modeling based on measured wrinkle topography establishes a correlation between wrinkle properties, particularly shear strain, and localized exciton emission. Beyond the array-induced super-wrinkles, nano-PL spatial maps further reveal that the strain environment around individual stressors is heterogeneous due to the presence of fine wrinkles that are less deterministic. Detailed nanoscale hyperspectral images uncover a wide range of low-energy emission peaks originating from these fine wrinkles, and show that the states can be tightly confined to regions < 10 nm, even in ambient conditions. These results establish a promising potential route towards realizing room temperature quantum emission in 2D TMDC systems.

cond-mat.mes-hall↗

arXiv2023

Charge and Energy Transfer Dynamics of Hybridized Exciton-Polaritons in 2D Halide Perovskites

Excitons, bound electron-hole pairs, in Two-Dimensional Hybrid Organic Inorganic Perovskites (2D HOIPs) are capable of forming hybrid light-matter states known as exciton-polaritons (E-Ps) when the excitonic medium is confined in an optical cavity. In the case of 2D HOIPs, they can self-hybridize into E-Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the excitons. However, the fundamental properties of these self-hybridized E-Ps in 2D HOIPs, including their role in ultrafast energy and/or charge transfer at interfaces, remain unclear. Here, we demonstrate that > 0.5 um thick 2D HOIP crystals on Au substrates are capable of supporting multiple-orders of self-hybridized E-P modes. These E-Ps have high Q factors (> 100) and modulate the optical dispersion for the crystal to enhance sub-gap absorption and emission. Through varying excitation energy and ultrafast measurements, we also confirm energy transfer from higher energy upper E-Ps to lower energy, lower E-Ps. Finally, we also demonstrate that E-Ps are capable of charge transport and transfer at interfaces. Our findings provide new insights into charge and energy transfer in E-Ps opening new opportunities towards their manipulation for polaritonic devices.

cond-mat.mes-hall↗

arXiv2023

In-plane anisotropy in biaxial ReS2 crystals probed by nano-optical imaging of waveguide modes

Near-field imaging has emerged as a reliable probe of the dielectric function of van der Waals crystals. In principle, analyzing the propagation patterns of subwavelength waveguide modes (WMs) allows for extraction of the full dielectric tensor. Yet previous studies have mostly been restricted to high-symmetry materials or narrowband probing. Here, we resolve in-plane anisotropic WMs in thin rhenium disulfide (ReS2) crystals across a wide range of near-infrared frequencies. By tracing the evolution of these modes as a function of crystallographic direction, polarization of the electric field and sample thickness, we have determined the anisotropic dielectric tensor including the elusive out-of-plane response. The excitonic absorption at ~1.5 eV manifests itself as a clear backbending feature in the WM dispersion and a reduction of the quality factors as fully supported by numerical calculations. Our results extend the sensitivity of near-field microscopy towards biaxial anisotropy and provide key insights into the optoelectronic properties of ReS2.

physics.optics↗

arXiv2022

Indefinite and Bidirectional Near Infrared Nanocrystal Photoswitching

Materials whose luminescence can be switched by optical stimulation drive technologies ranging from superresolution imaging1-4, nanophotonics5, and optical data storage6-8, to targeted pharmacology, optogenetics, and chemical reactivity9. These photoswitchable probes, including organic fluorophores and proteins, are prone to photodegradation, and often require phototoxic doses of ultraviolet (UV) or visible light. Colloidal inorganic nanoparticles have significant stability advantages over existing photoswitchable materials, but the ability to switch emission bidirectionally, particularly with NIR light, has not been reported with nanoparticles. Here, we present 2-way, near-infrared (NIR) photoswitching of avalanching nanoparticles (ANPs), showing full optical control of upconverted emission using phototriggers in the NIR-I and NIR-II spectral regions useful for subsurface imaging. Employing single-step photodarkening10-13 and photobrightening12,14-18, we demonstrate indefinite photoswitching of individual nanoparticles (>1000 cycles over 7 h) in ambient or aqueous conditions without measurable photodegradation. Critical steps of the photoswitching mechanism are elucidated by modeling and by measuring the photon avalanche properties of single ANPs in both bright and dark states. Unlimited, reversible photoswitching of ANPs enables indefinitely rewritable 2D and 3D multi-level optical patterning of ANPs, as well as optical nanoscopy with sub-Å localization superresolution that allows us to distinguish individual ANPs within tightly packed clusters.

physics.optics↗

arXiv2022

Ultra Localized Optoelectronic Properties of Nanobubbles in 2D Semiconductors

The optical properties of transition metal dichalcogenides have previously been modified at the nanoscale by using mechanical and electrical nanostructuring. However, a clear experimental picture relating the local electronic structure with emission properties in such structures has so far been lacking. Here, we use a combination of scanning tunneling microscopy (STM) and near-field photoluminescence (nano-PL) to probe the electronic and optical properties of single nano-bubbles in bilayer heterostructures of WSe2 on MoSe2. We show from tunneling spectroscopy that there are electronic states deeply localized in the gap at the edge of such bubbles, which are independent of the presence of chemical defects in the layers. We also show a significant change in the local bandgap on the bubble, with a continuous evolution to the edge of the bubble over a length scale of ~20 nm. Nano-PL measurements observe a continuous redshift of the interlayer exciton on entering the bubble, in agreement with the band to band transitions measured by STM. We use self-consistent Schrödinger-Poisson (SP) simulations to capture the essence of the experimental results and find that strong doping in the bubble region is a key ingredient to achieving the observed localized states, together with mechanical strain.

cond-mat.mes-hall↗

arXiv2022

Direct Nano-Imaging of Light-Matter Interactions in Nanoscale Excitonic Emitters

Strong light-matter interactions in localized nano-emitters when placed near metallic mirrors have been widely reported via spectroscopic studies in the optical far-field. Here, we report a near-field nano-spectroscopic study of the localized nanoscale emitters on a flat Au substrate. We observe strong-coupling of the excitonic dipoles in quasi 2-dimensional CdSe/CdxZnS1-xS nanoplatelets with gap mode plasmons formed between the Au tip and substrate. We also observe directional propagation on the Au substrate of surface plasmon polaritons launched from the excitons of the nanoplatelets as wave-like fringe patterns in the near-field photoluminescence maps. These fringe patterns were confirmed via extensive electromagnetic wave simulations to be standing-waves formed between the tip and the emitter on the substrate plane. We further report that both light confinement and the in-plane emission can be engineered by tuning the surrounding dielectric environment of the nanoplatelets. Our results lead to renewed understanding of in-plane, near-field electromagnetic signal transduction from the localized nano-emitters with profound implications in nano and quantum photonics as well as resonant optoelectronics.

physics.optics↗

arXiv2022

Atomically imprinted graphene plasmonic cavities

Plasmon polaritons in van der Waals (vdW) materials hold promise for next-generation photonics. The ability to deterministically imprint spatial patterns of high carrier density in cavities and circuitry with nanoscale features underlies future progress in nonlinear nanophotonics and strong light-matter interactions. Here, we demonstrate a general strategy to atomically imprint low-loss graphene plasmonic structures using oxidation-activated charge transfer (OCT). We cover graphene with a monolayer of WSe$_2$, which is subsequently oxidized into high work-function WOx to activate charge transfer. Nano-infrared imaging reveals low-loss plasmon polaritons at the WOx/graphene interface. We insert WSe$_2$ spacers to precisely control the OCT-induced carrier density and achieve a near-intrinsic quality factor of plasmons. Finally, we imprint canonical plasmonic cavities exhibiting laterally abrupt doping profiles with single-digit nanoscale precision via programmable OCT. Specifically, we demonstrate technologically appealing but elusive plasmonic whispering-gallery resonators based on free-standing graphene encapsulated in WOx. Our results open avenues for novel quantum photonic architectures incorporating two-dimensional materials.

physics.optics↗

arXiv2022

Infrared Plasmons Propagate through a Hyperbolic Nodal Metal

Metals are canonical plasmonic media at infrared and optical wavelengths, allowing one to guide and manipulate light at the nano-scale. A special form of optical waveguiding is afforded by highly anisotropic crystals revealing the opposite signs of the dielectric functions along orthogonal directions. These media are classified as hyperbolic and include crystalline insulators, semiconductors and artificial metamaterials. Layered anisotropic metals are also anticipated to support hyperbolic waveguiding. Yet this behavior remains elusive, primarily because interband losses arrest the propagation of infrared modes. Here, we report on the observation of propagating hyperbolic waves in a prototypical layered nodal-line semimetal ZrSiSe. The observed waveguiding originates from polaritonic hybridization between near-infrared light and nodal-line plasmons. Unique nodal electronic structures simultaneously suppress interband loss and boost the plasmonic response, ultimately enabling the propagation of infrared modes through the bulk of the crystal.

cond-mat.mes-hall↗

arXiv2022

Towards compact phase-matched and waveguided nonlinear optics in atomically layered semiconductors

Nonlinear frequency conversion provides essential tools for light generation, photon entanglement, and manipulation. Transition metal dichalcogenides (TMDs) possess huge nonlinear susceptibilities and 3R-stacked TMD crystals further combine broken inversion symmetry and aligned layering, representing ideal candidates to boost the nonlinear optical gain with minimal footprint. Here, we report on the efficient frequency conversion of 3R-MoS2, revealing the evolution of its exceptional second-order nonlinear processes along the ordinary (in-plane) and extraordinary (out-of-plane) directions. By measuring second harmonic generation (SHG) of 3R-MoS2 with various thickness - from monolayer (~0.65 nm) to bulk (~1 μm) - we present the first measurement of the in-plane SHG coherence length (~530 nm) at 1520 nm and achieve record nonlinear optical enhancement from a van der Waals material, >10^4 stronger than a monolayer. It is found that 3R-MoS2 slabs exhibit similar conversion efficiencies of lithium niobate, but within propagation lengths >100-fold shorter at telecom wavelengths. Furthermore, along the extraordinary axis, we achieve broadly tunable SHG from 3R-MoS2 in a waveguide geometry, revealing the coherence length in such structure for the first time. We characterize the full refractive index spectrum and quantify both birefringence components in anisotropic 3R-MoS2 crystals with near-field nano-imaging. Empowered with these data we assess the intrinsic limits of the conversion efficiency and nonlinear optical processes in 3R-MoS2 attainable in waveguide geometries. Our analysis highlights the potential of 3R-stacked TMDs for integrated photonics, providing critical parameters for designing highly efficient on-chip nonlinear optical devices including periodically poled structures, resonators, compact optical parametric oscillators and amplifiers, and optical quantum circuits.

physics.optics↗

arXiv2021

Nanoscale Optical Imaging of 2D Semiconductor Stacking Orders by Exciton-Enhanced Second Harmonic Generation

Second harmonic generation (SHG) is a nonlinear optical response arising exclusively from broken inversion symmetry in the electric-dipole limit. Recently, SHG has attracted widespread interest as a versatile and noninvasive tool for characterization of crystal symmetry and emerging ferroic or topological orders in quantum materials. However, conventional far-field optics is unable to probe local symmetry at the deep subwavelength scale. Here, we demonstrate near-field SHG imaging of 2D semiconductors and heterostructures with the spatial resolution down to 20 nm using a scattering-type nano-optical apparatus. We show that near-field SHG efficiency is greatly enhanced by excitons in atomically thin transition metal dichalcogenides. Furthermore, by correlating nonlinear and linear scattering-type nano-imaging, we resolve nanoscale variations of interlayer stacking order in bilayer WSe2, and reveal the stacking-tuned excitonic light-matter-interactions. Our work demonstrates nonlinear optical interrogation of crystal symmetry and structure-property relationships at the nanometer length scales relevant to emerging properties in quantum materials.

physics.optics↗

arXiv2021

Manipulation of Exciton Dynamics in Single-Layer WSe2 Using a Toroidal Dielectric Metasurface

Recent advances in emerging atomically thin transition metal dichalcogenide semiconductors with strong light-matter interactions and tunable optical properties provide novel approaches for realizing new material functionalities. Coupling two-dimensional semiconductors with all-dielectric resonant nanostructures represents an especially attractive opportunity for manipulating optical properties in both the near-field and far-field regimes. Here, by integrating single-layer WSe2 and titanium oxide (TiO2) dielectric metasurfaces with toroidal resonances, we realized robust exciton emission enhancement over one order of magnitude at both room and low temperatures. Furthermore, we could control exciton dynamics and annihilation by using temperature to tailor the spectral overlap of excitonic and toroidal resonances, allowing us to selectively enhance the Purcell effect. Our results provide rich physical insight into the strong light-matter interactions in single-layer TMDs coupled with toroidal dielectric metasurfaces, with important implications for optoelectronics and photonics applications.

cond-mat.mes-hall↗

arXiv2020

Nonlinear twistoptics at symmetry-broken interfaces

Broken symmetries induce strong nonlinear optical responses in materials and at interfaces. Twist angle can give complete control over the presence or lack of inversion symmetry at a crystal interface, and is thus an appealing knob for tuning nonlinear optical systems. In contrast to conventional nonlinear crystals with rigid lattices, the weak interlayer coupling in van der Waals (vdW) heterostructures allows for arbitrary selection of twist angle, making nanomechanical manipulation of fundamental interfacial symmetry possible within a single device. Here we report highly tunable second harmonic generation (SHG) from nanomechanically rotatable stacks of bulk hexagonal boron nitride (BN) crystals, and introduce the term twistoptics to describe studies of optical properties in dynamically twistable vdW systems. We observe SHG intensity modulated by a factor of more than 50, polarization patterns determined by moiré interface symmetry, and enhanced conversion efficiency for bulk crystals by stacking multiple pieces of BN joined by symmetry-broken interfaces. Our study provides a foundation for compact twistoptics architectures aimed at efficient, scalable, and tunable frequency-conversion, and demonstrates SHG as a robust probe of buried vdW interfaces.

cond-mat.mes-hall↗

arXiv2020

Giant nonlinear optical responses from photon avalanching nanoparticles

Avalanche phenomena leverage steeply nonlinear dynamics to generate disproportionately high responses from small perturbations and are found in a multitude of events and materials, enabling technologies including optical phase-conjugate imaging, infrared quantum counting, and efficient upconverted lasing. However, the photon avalanching (PA) mechanism underlying these optical innovations has been observed only in bulk materials and aggregates, and typically at cryogenic temperatures, limiting its utility and impact. Here, we report the realization of PA at room temperature in single nanostructures--small, Tm-doped upconverting nanocrystals--and demonstrate their use in superresolution imaging at near-infrared (NIR) wavelengths within spectral windows of maximal biological transparency. Avalanching nanoparticles (ANPs) can be pumped by continuous-wave or pulsed lasers and exhibit all of the defining features of PA. These hallmarks include excitation power thresholds, long rise time at threshold, and a dominant excited-state absorption that is >13,000x larger than ground-state absorption. Beyond the avalanching threshold, ANP emission scales nonlinearly with the 26th power of pump intensity. This enables the realization of photon-avalanche single-beam superresolution imaging (PASSI), achieving sub-70 nm spatial resolution using only simple scanning confocal microscopy and before any computational analysis. Pairing their steep nonlinearity with existing superresolution techniques and computational methods, ANPs allow for imaging with higher resolution and at ca. 100-fold lower excitation intensities than is possible with other probes. The low PA threshold and exceptional photostability of ANPs also suggest their utility in a diverse array of applications including sub-wavelength bioimaging, IR detection, temperature and pressure transduction, neuromorphic computing, and quantum optics.

physics.optics↗

arXiv2020

Planar Aperiodic Arrays as Metasurfaces for Optical Near-Field Patterning

Plasmonic metasurfaces have spawned the field of flat optics using nanostructured planar metallic or dielectric surfaces that can replace bulky optical elements and enhance the capabilities of traditional far-field optics. Furthermore, the potential of flat optics can go far beyond far-field modulation, and can be exploited for functionality in the near-field itself. Here, we design metasurfaces based on aperiodic arrays of plasmonic Au nanostructures for tailoring the optical near-field in the visible and near-infrared spectral range. The basic element of the arrays is a rhomboid that is modulated in size, orientation and position to achieve the desired functionality of the micron-size metasurface structure. Using two-photon-photoluminescence as a tool to probethe near-field profiles in the plane of the metasurfaces, we demonstrate the molding of light into different near-field intensity patterns and active pattern control via the far-field illumination. Finite element method simulations reveal that the near-field modulation occurs via a combination of the plasmonic resonances of the rhomboids and field enhancement in the nanoscale gaps in between the elements. This approach enables optical elements that can switch the near-field distribution across the metasurface via wavelength and polarization of the incident far-field light, and provides pathways for light matter interaction in integrated devices.

physics.app-ph↗

arXiv2020

Imaging strain-localized exciton states in nanoscale bubbles in monolayer WSe2 at room temperature

In monolayer transition metal dichalcogenides, quantum emitters are associated with localized strain that can be deterministically applied to create designer nano-arrays of single photon sources. Despite an overwhelming empirical correlation with local strain, the nanoscale interplay between strain, excitons, defects and local crystalline structure that gives rise to these quantum emitters is poorly understood. Here, we combine room-temperature nano-optical imaging and spectroscopy of excitons in nanobubbles of localized strain in monolayer WSe2 with atomistic structural models to elucidate how strain induces nanoscale confinement potentials that give rise to highly localized exciton states in 2D semiconductors. Nano-optical imaging of nanobubbles in low-defect monolayers reveal localized excitons on length scales of approximately 10 nm at multiple sites along the periphery of individual nanobubbles, which is in stark contrast to predictions of continuum models of strain. These results agree with theoretical confinement potentials that are atomistically derived from measured topographies of existing nanobubbles. Our results provide one-of-a-kind experimental and theoretical insight of how strain-induced confinement - without crystalline defects - can efficiently localize excitons on length scales commensurate with exciton size, providing key nanoscale structure-property information for quantum emitter phenomena in monolayer WSe2.

cond-mat.mes-hall↗

arXiv2020

The ultrafast onset of exciton formation in 2D semiconductors

The equilibrium and non-equilibrium optical properties of single-layer transition metal dichalcogenides (TMDs) are determined by strongly bound excitons. Exciton relaxation dynamics in TMDs have been extensively studied by time-domain optical spectroscopies. However, the formation dynamics of excitons following non-resonant photoexcitation of free electron-hole pairs have been challenging to directly probe because of their inherently fast timescales. Here we use extremely short optical pulses to non-resonantly excite an electron-hole plasma and show the formation of two-dimensional excitons in single-layer MoS2 on the timescale of 30 fs via the induced changes to photo-absorption. These formation dynamics are significantly faster than in conventional 2D quantum wells and are attributed to the intense Coulombic interactions present in 2D TMDs. A theoretical model of a coherent polarization that dephases and relaxes to an incoherent exciton population reproduces the experimental dynamics on the sub-100-fs timescale and sheds light into the underlying mechanism of how the lowest-energy excitons, which are the most important for optoelectronic applications, form from higher-energy excitations. Importantly, a phonon-mediated exciton cascade from higher energy states to the ground excitonic state is found to be the rate-limiting process. These results set an ultimate timescale of the exciton formation in TMDs and elucidate the exceptionally fast physical mechanism behind this process.

cond-mat.mtrl-sci↗

arXiv2019

Broadband optical parametric amplification by two-dimensional semiconductors

Optical parametric amplification is a second-order nonlinear process whereby an optical signal is amplified by a pump via the generation of an idler field. It is the key ingredient of tunable sources of radiation that play an important role in several photonic applications. This mechanism is inherently related to spontaneous parametric down-conversion that currently constitutes the building block for entangled photon pair generation, which has been exploited in modern quantum technologies ranging from computing to communications and cryptography. Here we demonstrate single-pass optical parametric amplification at the ultimate thickness limit; using semiconducting transition-metal dichalcogenides, we show that amplification can be attained over a propagation through a single atomic layer. Such a second-order nonlinear interaction at the 2D limit bypasses phase-matching requirements and achieves ultrabroad amplification bandwidths. The amplification process is independent on the in-plane polarization of the impinging signal and pump fields. First-principle calculations confirm the observed polarization invariance and linear relationship between idler and pump powers. Our results pave the way for the development of atom-sized tunable sources of radiation with applications in nanophotonics and quantum information technology.

physics.optics↗