All-dielectric structural coloration empowered by bound states in the continuum
The technological requirements of low-power and high-fidelity color displays have been instrumental in driving research into advanced coloration technologies. At the forefront of these developments is the implementation of dye-free approaches, which overcome previous constraints related to color resolution and fading. Resonant dielectric nanostructures have emerged as a promising paradigm, showing great potential for high efficiency, high color saturation, wide gamut palette, and image reproduction. However, they still face limitations related to color accuracy, purity, and simultaneous brightness tunability. Here, we demonstrate an all-dielectric metasurface empowered by photonic bound states in the continuum (BICs), which supports sharp resonances throughout the visible spectral range, ideally suited for producing a wide range of structural colors. The metasurface design consists of TiO ellipses with carefully controlled sizes and geometrical asymmetry, allowing versatile and on-demand variation of the brightness and hue of the output colors, respectively.
Highly sensitive volumetric single-molecule imaging
Volumetric subcellular imaging has long been essential for studying structures and dynamics in cells and tissues. However, due to limited imaging speed and depth of field, it has been challenging to perform live-cell imaging and single-particle tracking. Here we report a 2.5D fluorescence microscopy combined with highly inclined illumination beams, which significantly reduce not only the image acquisition time but also the out-of-focus background by ∼2-fold compared to epi-illumination. Instead of sequential -scanning, our method projects a certain depth of volumetric information onto a 2D plane in a single shot using multi-layered glass for incoherent wavefront splitting, enabling high photon detection efficiency. We apply our method to multi-color immunofluorescence imaging and volumetric super-resolution imaging, covering ∼3-4 µm thickness of samples without -scanning. Additionally, we demonstrate that our approach can substantially extend the observation time of single-particle tracking in living cells.
Phase-matched third-harmonic generation in silicon nitride waveguides
Third-harmonic generation (THG) in silicon nitride waveguides is an ideal source of coherent visible light, suited for ultrafast pulse characterization, telecom signal monitoring and self-referenced comb generation due to its relatively large nonlinear susceptibility and CMOS compatibility. We demonstrate third-harmonic generation in silicon nitride waveguides where a fundamental transverse mode at 1,596 nm is phase-matched to a TM mode at 532 nm, confirmed by the far-field image. We experimentally measure the waveguide width-dependent phase-matched wavelength with a peak-power-normalized conversion efficiency of 5.78 × 10 %/W over a 660-μm-long interaction length.
Dirac exciton-polariton condensates in photonic crystal gratings
Bound states in the continuum have recently been utilized in photonic crystal gratings to achieve strong coupling and ultralow threshold condensation of exciton-polariton quasiparticles with atypical Dirac-like features in their dispersion relation. Here, we develop the single- and many-body theory of these new effective relativistic polaritonic modes and describe their mean-field condensation dynamics facilitated by the interplay between protection from the radiative continuum and negative-mass optical trapping. Our theory accounts for tunable grating parameters giving full control over the diffractive coupling properties between guided polaritons and the radiative continuum, unexplored for polariton condensates. In particular, we discover stable cyclical condensate solutions mimicking a driven-dissipative analog of the effect characterized by coherent superposition of ballistic and trapped polariton waves. We clarify important distinctions between the polariton nearfield and farfield explaining recent experiments on the emission characteristics of these long lived nonlinear Dirac polaritons.
Gouy phase effects on photocurrents in plasmonic nanogaps driven by single-cycle pulses
The investigation of optical phenomena in the strong-field regime requires few-cycle laser pulses at field strengths exceeding gigavolts per meter (GV/m). Surprisingly, such conditions can be reached by tightly focusing pJ-level pulses with nearly octave spanning optical bandwidth onto plasmonic nanostructures, exploiting the field-enhancement effect. In this situation, the Gouy phase of the focused beam can deviate significantly from the monochromatic scenario. Here, we study the effect of the Gouy phase of a pulse exploited to drive coherent strong-field photocurrents within a plasmonic gap nanoantenna. While the influence of the specific Gouy phase profile in the experiment approaches the monochromatic case closely, this scheme may be utilized to identify more intricate phase profiles at sub-diffraction scale. Our results pave the way for Gouy phase engineering at picojoule (pJ) pulse energy levels, enabling the optimization of strong-field optical phenomena.
Reconfigurable quantum photonic circuits based on quantum dots
Quantum photonic integrated circuits, composed of linear-optical elements, offer an efficient way for encoding and processing quantum information on-chip. At their core, these circuits rely on reconfigurable phase shifters, typically constructed from classical components such as thermo- or electro-optical materials, while quantum solid-state emitters such as quantum dots are limited to acting as single-photon sources. Here, we demonstrate the potential of quantum dots as reconfigurable phase shifters. We use numerical models based on established literature parameters to show that circuits utilizing these emitters enable high-fidelity operation and are scalable. Despite the inherent imperfections associated with quantum dots, such as imperfect coupling, dephasing, or spectral diffusion, we show that circuits based on these emitters may be optimized such that these do not significantly impact the unitary infidelity. Specifically, they do not increase the infidelity by more than 0.001 in circuits with up to 10 modes, compared to those affected only by standard nanophotonic losses and routing errors. For example, we achieve fidelities of 0.9998 in quantum-dot-based circuits enacting controlled-phase and - not gates without any redundancies. These findings demonstrate the feasibility of quantum emitter-driven quantum information processing and pave the way for cryogenically-compatible, fast, and low-loss reconfigurable quantum photonic circuits.
From weak to strong coupling: quasi-BIC metasurfaces for mid-infrared light-matter interactions
Thanks to their giant, yet tunable, -factor resonances, all-dielectric metasurfaces supporting the quasi-bound states in the continuum (q-BIC) resonances are well-suited to provide a promising platform for quantum-coherent light-matter interactions. Yet, the strong coupling regime, characterized by the hybrid light-matter states - polaritons, has not yet been fully explored in the mid-infrared regime. This paper investigates the parameter space of vibrational strong coupling (VSC) between material and metasurface cavities supporting q-BIC resonances in the mid-infrared spectral range. We outline the effects of transition dipole strength, damping rate, and the number of molecules coupled to a single cavity, as well as the cavity damping rates, to understand their respective impacts on VSC. By tuning the -factor of the metasurface and material parameters, a new transition light-matter coupling zone is introduced, bridging the gap between weak and strong coupling, where polaritons form but their linewidths prohibit their spectral identification. The study further identifies the effects of cavity linewidth on polariton peak separability in strongly coupled systems, highlighting that the cavities with smaller nonradiative losses and narrower linewidths facilitate better polariton separability. Moreover, we found that matching cavity and material loss, satisfying the critical strong coupling condition, enhances the coupling strength between cavity and material. Overall, these findings can guide the design of photonic cavities suited for VSC experiments, contributing to the burgeoning fields of polaritonic chemistry, light-mediated modulation of chemical reactivity, and highly sensitive molecular spectroscopy.
Enhancing metasurface fabricability through minimum feature size enforcement
The metasurfaces have shown great potential for miniaturizing conventional optics while offering extended flexibility. Recently, there has been considerable interest in using algorithms to generate meta-atom shapes for these metasurfaces, as they offer vast design freedom and not biased by the human intuition. However, these complex designs significantly increase the difficulty of fabrication. To address this, we introduce a design process that rigorously enforces the fabricability of both the material-filled (fill) and empty (void) regions in a metasurface design. This process takes into account specific constraints regarding the minimum feature size for each region. Additionally, it corrects any violations of these constraints across the entire device, ensuring only minimal impact on performance. Our method provides a practical way to create metasurface designs that are easy to fabricate, even with complex shapes, hence improving the overall production yield of these advanced meta-optical components.
Strong coupling of metamaterials with cavity photons: toward non-Hermitian optics
The investigation of strong coupling between light and matter is an important field of research. Its significance arises not only from the emergence of a plethora of intriguing chemical and physical phenomena, often novel and unexpected, but also from its provision of important tool sets for the design of core components for novel chemical, electronic, and photonic devices such as quantum computers, lasers, amplifiers, modulators, sensors and more. Strong coupling has been demonstrated for various material systems and spectral regimes, each exhibiting unique features and applications. In this perspective, we will focus on a sub-field of this domain of research and discuss the strong coupling between and . The metamaterials, themselves electromagnetic resonators, serve as "artificial atoms". We provide a concise overview of recent advances and outline possible research directions in this vital and impactful field of interdisciplinary science.
Active control of polariton-enabled long-range energy transfer
Optical control is achieved on the excited state energy transfer between spatially separated donor and acceptor molecules, both coupled to the same optical mode of a cavity. The energy transfer occurs through the formed hybrid polaritons and can be switched on and off by means of ultraviolet and visible light. The control mechanism relies on a photochromic component used as donor, whose absorption and emission properties can be varied reversibly through light irradiation, whereas in-cavity hybridization with acceptors through polariton states enables a 6-fold enhancement of acceptor/donor contribution to the emission intensity with respect to a reference multilayer. These results pave the way for synthesizing effective gating systems for the transport of energy by light, relevant for light-harvesting and light-emitting devices, and for photovoltaic cells.
Identifying the origin of delayed electroluminescence in a polariton organic light-emitting diode
Modifying the energy landscape of existing molecular emitters is an attractive challenge with favourable outcomes in chemistry and organic optoelectronic research. It has recently been explored through strong light-matter coupling studies where the organic emitters were placed in an optical cavity. Nonetheless, a debate revolves around whether the observed change in the material properties represents novel coupled system dynamics or the unmasking of pre-existing material properties induced by light-matter interactions. Here, for the first time, we examined the effect of strong coupling in polariton organic light-emitting diodes via time-resolved electroluminescence studies. We accompanied our experimental analysis with theoretical fits using a model of coupled rate equations accounting for all major mechanisms that can result in delayed electroluminescence in organic emitters. We found that in our devices the delayed electroluminescence was dominated by emission from trapped charges and this mechanism remained unmodified in the presence of strong coupling.
Few-emitter lasing in single ultra-small nanocavities
Lasers are ubiquitous for information storage, processing, communications, sensing, biological research and medical applications. To decrease their energy and materials usage, a key quest is to miniaturise lasers down to nanocavities. Obtaining the smallest mode volumes demands plasmonic nanocavities, but for these, gain comes from only a single or few emitters. Until now, lasing in such devices was unobtainable due to low gain and high cavity losses. Here, we demonstrate a form of 'few emitter lasing' in a plasmonic nanocavity approaching the single-molecule emitter regime. The few-emitter lasing transition significantly broadens, and depends on the number of molecules and their individual locations. We show this non-standard few-emitter lasing can be understood by developing a theoretical approach extending previous weak-coupling theories. Our work paves the way for developing nanolaser applications as well as fundamental studies at the limit of few emitters.
Strong coupling in molecular systems: a simple predictor employing routine optical measurements
We provide a simple method that enables readily acquired experimental data to be used to predict whether or not a candidate molecular material may exhibit strong coupling. Specifically, we explore the relationship between the hybrid molecular/photonic (polaritonic) states and the bulk optical response of the molecular material. For a given material, this approach enables a prediction of the maximum extent of strong coupling (vacuum Rabi splitting), irrespective of the nature of the confined light field. We provide formulae for the upper limit of the splitting in terms of the molar absorption coefficient, the attenuation coefficient, the extinction coefficient (imaginary part of the refractive index) and the absorbance. To illustrate this approach, we provide a number of examples, and we also discuss some of the limitations of our approach.
Enhancement of the internal quantum efficiency in strongly coupled P3HT-C organic photovoltaic cells using Fabry-Perot cavities with varied cavity confinement
The short exciton diffusion length in organic semiconductors results in a strong dependence of the conversion efficiency of organic photovoltaic (OPV) cells on the morphology of the donor-acceptor bulk-heterojunction blend. Strong light-matter coupling provides a way to circumvent this dependence by combining the favorable properties of light and matter via the formation of hybrid exciton-polaritons. By strongly coupling excitons in P3HT-C OPV cells to Fabry-Perot optical cavity modes, exciton-polaritons are formed with increased propagation lengths. We exploit these exciton-polaritons to enhance the internal quantum efficiency of the cells, determined from the external quantum efficiency and the absorptance. Additionally, we find a consistent decrease in the Urbach energy for the strongly coupled cells, which indicates the reduction of energetic disorder due to the delocalization of exciton-polaritons in the optical cavity.
Toward "super-scintillation" with nanomaterials and nanophotonics
Following the discovery of X-rays, scintillators are commonly used as high-energy radiation sensors in diagnostic medical imaging, high-energy physics, astrophysics, environmental radiation monitoring, and security inspections. Conventional scintillators face intrinsic limitations including a low extraction efficiency of scintillated light and a low emission rate, leading to efficiencies that are less than 10 % for commercial scintillators. Overcoming these limitations will require new materials including scintillating nanomaterials ("nanoscintillators"), as well as new photonic approaches that increase the efficiency of the scintillation process, increase the emission rate of materials, and control the directivity of the scintillated light. In this perspective, we describe emerging nanoscintillating materials and three nanophotonic platforms: (i) plasmonic nanoresonators, (ii) photonic crystals, and (iii) high-Q metasurfaces that could enable high performance scintillators. We further discuss how a combination of nanoscintillators and photonic structures can yield a "super scintillator" enabling ultimate spatio-temporal resolution while enabling a significant boost in the extracted scintillation emission.
Direct electron beam patterning of electro-optically active PEDOT:PSS
The optical and electronic tunability of the conductive polymer poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) has enabled emerging applications as diverse as bioelectronics, flexible electronics, and micro- and nano-photonics. High-resolution spatial patterning of PEDOT:PSS opens up opportunities for novel active devices in a range of fields. However, typical lithographic processes require tedious indirect patterning and dry etch processes, while solution-processing methods such as ink-jet printing have limited spatial resolution. Here, we report a method for direct write nano-patterning of commercially available PEDOT:PSS through electron-beam induced solubility modulation. The written structures are water stable and maintain the conductivity as well as electrochemical and optical properties of PEDOT:PSS, highlighting the broad utility of our method. We demonstrate the potential of our strategy by preparing prototypical nano-wire structures with feature sizes down to 250 nm, an order of magnitude finer than previously reported direct write methods, opening the possibility of writing chip-scale microelectronic and optical devices. We finally use the high-resolution writing capabilities to fabricate electrically-switchable optical diffraction gratings. We show active switching in this archetypal system with >95 % contrast at CMOS-compatible voltages of +2 V and -3 V, offering a route towards highly-miniaturized dynamic optoelectronic devices.
Sculpting ultrastrong light-matter coupling through spatial matter structuring
The central theme of cavity quantum electrodynamics is the coupling of a single optical mode with a single matter excitation, leading to a doublet of cavity polaritons which govern the optical properties of the coupled structure. Especially in the ultrastrong coupling regime, where the ratio of the vacuum Rabi frequency and the quasi-resonant carrier frequency of light, Ω/ , approaches unity, the polariton doublet bridges a large spectral bandwidth 2Ω, and further interactions with off-resonant light and matter modes may occur. The resulting multi-mode coupling has recently attracted attention owing to the additional degrees of freedom for designing light-matter coupled resonances, despite added complexity. Here, we experimentally implement a novel strategy to sculpt ultrastrong multi-mode coupling by tailoring the spatial overlap of multiple modes of planar metallic THz resonators and the cyclotron resonances of Landau-quantized two-dimensional electrons, on subwavelength scales. We show that similarly to the selection rules of classical optics, this allows us to suppress or enhance certain coupling pathways and to control the number of light-matter coupled modes, their octave-spanning frequency spectra, and their response to magnetic tuning. This offers novel pathways for controlling dissipation, tailoring quantum light sources, nonlinearities, correlations as well as entanglement in quantum information processing.
Continuous-wave GaAs/AlGaAs quantum cascade laser at 5.7 THz
Design strategies for improving terahertz (THz) quantum cascade lasers (QCLs) in the 5-6 THz range are investigated numerically and experimentally, with the goal of overcoming the degradation in performance that occurs as the laser frequency approaches the band. Two designs aimed at 5.4 THz were selected: one optimized for lower power dissipation and one optimized for better temperature performance. The active regions exhibited broadband gain, with the strongest modes lasing in the 5.3-5.6 THz range, but with other various modes observed ranging from 4.76 to 6.03 THz. Pulsed and continuous-wave (cw) operation is observed up to temperatures of 117 K and 68 K, respectively. In cw mode, the ridge laser has modes up to 5.71 THz - the highest reported frequency for a THz QCL in cw mode. The waveguide loss associated with the doped contact layers and metallization is identified as a critical limitation to performance above 5 THz.
Design and performance of GaSb-based quantum cascade detectors
InAs/AlSb quantum cascade detectors (QCDs) grown strain-balanced on GaSb substrates are presented. This material system offers intrinsic performance-improving properties, like a low effective electron mass of the well material of 0.026 , enhancing the optical transition strength, and a high conduction band offset of 2.28 eV, reducing the noise and allowing for high optical transition energies. InAs and AlSb strain balance each other on GaSb with an InAs:AlSb ratio of 0.96:1. To regain the freedom of a lattice-matched material system regarding the optimization of a QCD design, submonolayer InSb layers are introduced. With strain engineering, four different active regions between 3.65 and 5.5 µm were designed with InAs:AlSb thickness ratios of up to 2.8:1, and subsequently grown and characterized. This includes an optimized QCD design at 4.3 µm, with a room-temperature peak responsivity of 26.12 mA/W and a detectivity of 1.41 × 10 Jones. Additionally, all QCD designs exhibit higher-energy interband signals in the mid- to near-infrared, stemming from the InAs/AlSb type-II alignment and the narrow InAs band gap.
THz quantum gap: exploring potential approaches for generating and detecting non-classical states of THz light
Over the past few decades, THz technology has made considerable progress, evidenced by the performance of current THz sources and detectors, as well as the emergence of several THz applications. However, in the realm of quantum technologies, the THz spectral domain is still in its infancy, unlike neighboring spectral domains that have flourished in recent years. Notably, in the microwave domain, superconducting qubits currently serve as the core of quantum computers, while quantum cryptography protocols have been successfully demonstrated in the visible and telecommunications domains through satellite links. The THz domain has lagged behind in these impressive advancements. Today, the current gap in the THz domain clearly concerns quantum technologies. Nonetheless, the emergence of quantum technologies operating at THz frequencies will potentially have a significant impact. Indeed, THz radiation holds significant promise for wireless communications with ultimate security owing to its low sensitivity to atmospheric disturbances. Moreover, it has the potential to raise the operating temperature of solid-state qubits, effectively addressing existing scalability issues. In addition, THz radiation can manipulate the quantum states of molecules, which are recognized as new platforms for quantum computation and simulation with long range interactions. Finally, its ability to penetrate generally opaque materials or its resistance to Rayleigh scattering are very appealing features for quantum sensing. In this perspective, we will discuss potential approaches that offer exciting prospects for generating and detecting non-classical states of THz light, thereby opening doors to significant breakthroughs in THz quantum technologies.
Isotopic effects on in-plane hyperbolic phonon polaritons in MoO
Hyperbolic phonon polaritons (HPhPs), hybrids of light and lattice vibrations in polar dielectric crystals, empower nanophotonic applications by enabling the confinement and manipulation of light at the nanoscale. Molybdenum trioxide (α-MoO) is a naturally hyperbolic material, meaning that its dielectric function deterministically controls the directional propagation of in-plane HPhPs within its reststrahlen bands. Strategies such as substrate engineering, nano- and heterostructuring, and isotopic enrichment are being developed to alter the intrinsic die ectric functions of natural hyperbolic materials and to control the confinement and propagation of HPhPs. Since isotopic disorder can limit phonon-based processes such as HPhPs, here we synthesize isotopically enriched MoO (Mo: 99.93 %) and MoO (Mo: 99.01 %) crystals to tune the properties and dispersion of HPhPs with respect to natural α-MoO, which is composed of seven stable Mo isotopes. Real-space, near-field maps measured with the photothermal induced resonance (PTIR) technique enable comparisons of inplane HPhPs in α-MoO and isotopically enriched analogues within a reststrahlen band (≈820 cm to ≈ 972 cm). Results show that isotopic enrichment (e.g., MoO and MoO) alters the dielectric function, shifting the HPhP dispersion (HPhP angular wavenumber × thickness vs IR frequency) by ≈-7% and ≈ +9 %, respectively, and changes the HPhP group velocities by ≈ ±12 %, while the lifetimes (≈ 3 ps) in MoO were found to be slightly improved (≈ 20 %). The latter improvement is attributed to a decrease in isotopic disorder. Altogether, isotopic enrichment was found to offer fine control over the properties that determine the anisotropic in-plane propagation of HPhPs in α-MoO, which is essential to its implementation in nanophotonic applications.