Nonlinear Optical Components Research Articles

Dielectric metasurface evolution from bulk to monolayer by strong coupling of quasi-BICs for second harmonic boosting

2D materials are promising candidates as nonlinear optical components for on-chip devices due to their ultrathin structure. In general, their nonlinear optical responses are inherently weak due to the short interaction thickness with light. Recently, there has been great interest in using quasi-bound states in the continuum (q-BICs) of dielectric metasurfaces, which are able to achieve remarkable optical near-field enhancement for elevating the second harmonic generation (SHG) emission from 2D materials. However, most studies focus on the design of combining bulk dielectric metasurfaces with unpatterned 2D materials, which suffer considerable radiation loss and limit near-field enhancement by high-quality q-BIC resonances. Here, we investigate the dielectric metasurface evolution from bulk silicon to monolayer molybdenum disulfide (MoS2), and discover the critical role of meta-atom thickness design on enhancing near-field effects of two q-BIC modes. We further introduce the strong-coupling of the two q-BIC modes by oblique incidence manipulation, and enhance the localized optical field on monolayer MoS2 dramatically. In the ultraviolet and visible regions, the MoS2 SHG enhancement factor of our design is 105 times higher than that of conventional bulk metasurfaces, leading to an extremely high nonlinear conversion efficiency of 5.8%. Our research will provide an important theoretical guide for the design of high-performance nonlinear devices based on 2D materials.

229 nm far-ultraviolet second harmonic generation in a vertical polarity inverted AlN bilayer channel waveguide

Far-UV light sources have attracted much attention for human-safe viral inactivation and bacterial disinfection. Due to large optical nonlinearity and transparency to this wavelength region, AlN is a promising material for compact and low-cost far-UV second harmonic generation (SHG) devices. In this study, a transverse quasi-phase-matched AlN channel waveguide with vertical polarity inversion was designed and fabricated. From wavelength spectra and a pump power dependence of an SH intensity, far-UV SHG via the largest nonlinear optical tensor component d 33 was successfully confirmed under ultrashort pulse laser excitation.

Giant Nonlinear Optical Response via Coherent Stacking ofIn-Plane Ferroelectric Layers.

Thin ferroelectric materials hold great promise for compact nonvolatile memory and nonlinear optical and optoelectronic devices. Herein, an ultrathin in-plane ferroelectric material that exhibits a giant nonlinear optical effect, group-IV monochalcogenide SnSe, is reported. Nanometer-scale ferroelectric domains with ≈90°/270° twin boundaries or ≈180° domain walls are revealed in physical-vapor-deposited SnSe by lateral piezoresponse force microscopy. Atomic structure characterization reveals both parallel and antiparallel stacking of neighboring van der Waals ferroelectric layers, leading to ferroelectric or antiferroelectric ordering. Ferroelectric domains exhibit giant nonlinear optical activity due to coherent enhancement of second-harmonic fields and the as-resulted second-harmonic generationwasobserved to be 100 times more intense than monolayer WS2 . This work demonstratesin-plane ferroelectric ordering and giant nonlinear optical activity in SnSe, which paves the way for applications in on-chip nonlinear optical components and nonvolatile memory devices.

Displacement current sources as nonlinear interactions in optical nanocircuits

Optical lumped circuit elements are the building blocks in the metatronics paradigm, whose goal is to extend the rules of RF circuit design into the field of nanophotonics by providing the advantages of lumpedness and modularity. In this paper, we aim at modeling within this framework nonlinear optical processes, based on the concept of optical lumped circuit elements. Displacement current sources are added to the previously introduced optical lumped elements in order to endow metatronics with nonlinear functionalities. This model not only simplifies the analysis of the nonlinear processes, but paves the road to develop nonlinear optical components and devices in this paradigm. Second- and third-order nonlinearities are investigated analytically in the case of a nanosphere. A step by step example of modeling a LiNbO3 nanorod, which is close to a practically realizable structure, is also presented. The results are compared with those of a full-wave simulation and the significance of the proposed model is discussed.

A Combined Experimental and Theoretical DFT (B3LYP and CAMB3LYP) Study on Spectral Features (FT-IR, NMR, and UV-Visible), First-order Hyperpolarizability, NBO and HOMO-LUMO Analysis of 4-(dimethylamino)-1,5-dimethyl-2-phenyl-1H-pyrazol-3(2H)-one

Abstract: The pyrazolone subordinate, aminopyrine, has been broken down tentatively and hypothetically for its vibrational frequencies. The chemical shift values and symphonious vibrational frequencies as obtained at B3LYP/CAM-B3LYP/6-31G after employing proper scaling techniques appear to match acceptably with the test perceptions. The hypothetical spectrograms for NMR, FT-IR and UV spectra of aminopyrine have been likewise developed and contrasted with the trial spectra. Determined hyperpolarizability (4.531 ×10-30 esu) showed that the particle might have a nonlinear optical (NLO) component with non-zero qualities. An investigation of hydrogen bonding, utilizing mathematical and topological boundaries, has additionally been conducted.

Role of deposition temperature on non-linear optical properties of spray-coated Zn0.95Nd0.05O films

The influence of deposition temperature on the structure and optical (linear and nonlinear) properties of Zn0.95Nd0.05O thin films grown on glass substrates by using the spray pyrolysis method is studied. The X-ray diffraction spectra reveal the hexagonal wurtzite structure with a reduction in peak intensity as deposition temperature increases. With increasing temperature, the prominent peak intensity changes, and the dislocation density increases. Concomitantly, the surface morphology transitions from a nanoflake to a needle-like structure. With increasing deposition temperature, the optical transmittance of the films in the visible region improves, while the energy bandgap, refractive index and extinction coefficient values decrease. The reduction of refractive index and extinction coefficient values is ascribed to decreased scattering and uniformity of the films. Further, the films exhibit saturable absorption and films deposited at 300 ℃ show a maximum for third-order nonlinear susceptibility, which is quite appealing for nonlinear optical devices and components.

Giant second-harmonic generation in ferroelectric NbOI2

Implementing nonlinear optical components in nanoscale photonic devices is challenged by phase-matching conditions requiring thicknesses in the order of hundreds of wavelengths, and is disadvantaged by the short optical interaction depth of nanometre-scale materials and weak photon–photon interactions. Here we report that ferroelectric NbOI2 nanosheets exhibit giant second-harmonic generation with conversion efficiencies that are orders of magnitude higher than commonly reported nonlinear crystals. The nonlinear response scales with layer thickness and is strain- and electrical-tunable; a record >0.2% absolute SHG conversion efficiency and an effective nonlinear susceptibility $$\chi _{\mathrm{eff}}^{(2)}$$ in the order of 10−9 m V−1 are demonstrated at an average pump intensity of 8 kW cm–2. Due to the interplay between anisotropic polarization and excitonic resonance in NbOI2, the spatial profile of the polarized SHG response can be tuned by the excitation wavelength. Our results represent a new paradigm for ultrathin, efficient nonlinear optical components. Strained NbOI2 flakes with a thickness of 20 nm exhibit a record SHG absolute conversion efficiency of >0.2% and an effective bulk-like nonlinear susceptibility of 1.1 × 10−9 m V−1 at the fundamental wavelength of 1,050 nm. The spatial profile of the polarized second-harmonic generation response can be tuned by the fundamental wavelength.

Fock state-enhanced expressivity of quantum machine learning models

The data-embedding process is one of the bottlenecks of quantum machine learning, potentially negating any quantum speedups. In light of this, more effective data-encoding strategies are necessary. We propose a photonic-based bosonic data-encoding scheme that embeds classical data points using fewer encoding layers and circumventing the need for nonlinear optical components by mapping the data points into the high-dimensional Fock space. The expressive power of the circuit can be controlled via the number of input photons. Our work sheds some light on the unique advantages offered by quantum photonics on the expressive power of quantum machine learning models. By leveraging the photon-number dependent expressive power, we propose three different noisy intermediate-scale quantum-compatible binary classification methods with different scaling of required resources suitable for different supervised classification tasks.

Second harmonic generation in glass-based metasurfaces using tailored surface lattice resonances

Abstract Dielectric metasurfaces have shown prominent applications in nonlinear optics due to strong field enhancement and low dissipation losses at the nanoscale. Chalcogenide glasses are one of the promising materials for the observation of nonlinear effects thanks to their high intrinsic nonlinearities. Here, we demonstrate, experimentally and theoretically, that significant second harmonic generation (SHG) can be obtained within amorphous Selenium (Se)-based chalcogenide metasurfaces by exploiting the coupling between lattice and particle resonances. We further show that the high-quality factor resonance at the origin of the SHG can be tuned over a wide wavelength range using a simple and versatile fabrication approach. The measured second harmonic intensity is orders of magnitude higher than that from a dewetted Se film consisting of random Se nanoparticles. The achieved conversion efficiency in the resonance region is of the order of 10−6 which is comparable with direct bandgap materials and at least two orders of magnitude higher than that of conventional plasmonics- and Si-based structures. Fabricated via a simple and scalable technique, these all-dielectric architectures are ideal candidates for the design of flat nonlinear optical components on flexible substrates.

Difference-frequency generation in an AlGaAs Bragg-reflection waveguide using an on-chip electrically-pumped quantum dot laser

Nonlinear frequency conversion is ubiquitous in laser engineering and quantum information technology. A long-standing goal in photonics is to integrate on-chip semiconductor laser sources with nonlinear optical components. Engineering waveguide lasers with spectra that phase-match to nonlinear processes on the same device is a formidable challenge. Here, we demonstrate difference-frequency generation in an AlGaAs Bragg reflection waveguide which incorporates the gain medium for the pump laser in its core. We include quantum dot layers in the waveguide that generate electrically driven laser light at ∼790 nm, and engineer the structure to facilitate nonlinear processes at this wavelength. We perform difference-frequency generation between 1540 nm and 1630 nm using the on-chip laser, which is enabled by the broad modal phase-matching of the AlGaAs waveguide, and measure normalized conversion efficiencies up to ()% W−1 cm−2. Our work demonstrates a pathway towards devices that utilize on-chip active elements and strong optical nonlinearities to enable highly integrated photonic systems-on-chip.

Recurrent Neural Network Soft-Demapping for Nonlinear ISI in 800Gbit/s DWDM Coherent Optical Transmissions

High speed optical transmission systems suffer from intersymbol interference (ISI) and colored noise induced by nonlinear bandwidth limited optical and electrical components. As a countermeasure, this article investigates deep neural network soft-demappers. In particular, we propose a bidirectional recurrent neural network soft-demapper (BRNN-SD) and benchmarked its performance against a time delay neural network soft-demapper (TDNN-SD) and a reference digital signal processing (DSP) scheme consisting of a Volterra nonlinear equalizer accompanied by a symbol-spaced whitening filter and a BCJR detector. On coherent 92GBd dual polarization (DP)-32QAM back-to-back measurements, the proposed soft-demapper matches the performance of the reference DSP. In 800 Gb/s 96GBd DP-32QAM 32-channel dense wavelength division multiplexing (DWDM) transmission over a 600 km fiber link the proposed approach outperforms the reference DSP.

Attractive and Repulsive Exciton-Polariton Interactions Mediated by an Electron Gas.

Realizing strong photon-photon interactions in a solid-state setting is a major goal with far reaching potential for optoelectronic applications. Using Landau's quasiparticle framework combined with a microscopic many-body theory, we explore the interactions between exciton-polaritons and trions in a two-dimensional semiconductor injected with an electron gas inside a microcavity. We show that particle-hole excitations in the electron gas mediate an attractive interaction between the polaritons, whereas the interaction between trions and polaritons mediated by the exchange of an electron can be either repulsive or attractive. These mediated interactions are intrinsic to the quasiparticles and are also present in the absence of light. Importantly, they can be tuned to be more than an order of magnitude stronger than the direct polariton-polariton interaction in the absence of the electron gas, thereby providing a promising outlook for nonlinear optical components. Finally, we compare our theoretical predictions to two recent experiments.

Hyperpolarizability of Plasmonic Meta-Atoms in Metasurfaces.

Plasmonic metasurfaces are promising as enablers of nanoscale nonlinear optics and flat nonlinear optical components. Nonlinear optical responses of such metasurfaces are determined by the nonlinear optical properties of individual plasmonic meta-atoms. Unfortunately, no simple methods exist to determine the nonlinear optical properties (hyperpolarizabilities) of the meta-atoms hindering the design of nonlinear metasurfaces. Here, we develop the equivalent RLC circuit (resistor, inductor, capacitor) model of such meta-atoms to estimate their second-order nonlinear optical properties, that is, the first-order hyperpolarizability in the optical spectral range. In parallel, we extract from second-harmonic generation experiments the first-order hyperpolarizabilities of individual meta-atoms consisting of asymmetrically shaped (elongated) plasmonic nanoprisms, verified with detailed calculations using both nonlinear hydrodynamic-FDTD and nonlinear scattering theory. All three approaches, analytical, experimental, and computational, yield results that agree very well. Our empirical RLC model can thus be used as a simple tool to enable an efficient design of nonlinear plasmonic metasurfaces.

Toward new frontiers for terahertz quantum cascade laser frequency combs

AbstractBroadband, quantum-engineered, quantum cascade lasers (QCLs) are the most powerful chip-scale sources of optical frequency combs (FCs) across the mid-infrared and the terahertz (THz) frequency range. The inherently short intersubband upper state lifetime spontaneously allows mode proliferation, with large quantum efficiencies, as a result of the intracavity four-wave mixing. QCLs can be easily integrated with external elements or engineered for intracavity embedding of nonlinear optical components and can inherently operate as quantum detectors, providing an intriguing technological platform for on-chip quantum investigations at the nanoscale. The research field of THz FCs is extremely vibrant and promises major impacts in several application domains crossing dual-comb spectroscopy, hyperspectral imaging, time-domain nanoimaging, quantum science and technology, metrology and nonlinear optics in a miniaturized and compact architecture. Here, we discuss the fundamental physical properties and the technological performances of THz QCL FCs, highlighting the future perspectives of this frontier research field.

Characterization of pathological thyroid tissue using polarization-sensitive second harmonic generation microscopy

AbstractPolarization-sensitive second harmonic generation (SHG) microscopy is an established imaging technique able to provide information related to specific molecular structures including collagen. In this investigation, polarization-sensitive SHG microscopy was used to investigate changes in the collagen ultrastructure between histopathology slides of normal and diseased human thyroid tissues including follicular nodular disease, Grave's disease, follicular variant of papillary thyroid carcinoma, classical papillary thyroid carcinoma, insular or poorly differentiated carcinoma, and anaplastic or undifferentiated carcinoma ex vivo. The second-order nonlinear optical susceptibility tensor component ratios, χ(2)zzz′/χ(2)zxx′ and χ(2)xyz′/χ(2)zxx′, were obtained, where χ(2)zzz′/χ(2)zxx′ is a structural parameter and χ(2)xyz′/χ(2)zxx′ is a measure of the chirality of the collagen fibers. Furthermore, the degree of linear polarization (DOLP) of the SHG signal was measured. A statistically significant increase in χ(2)zzz′/χ(2)zxx′ values for all the diseased tissues except insular carcinoma and a statistically significant decrease in DOLP for all the diseased tissues were observed compared to normal thyroid. This finding indicates a higher ultrastructural disorder in diseased collagen and provides an innovative approach to discriminate between normal and diseased thyroid tissues that is complementary to standard histopathology.Polarization-second harmonic microscopy was utilized to investigate whether collagen ultrastructure in thyroid due to four carcinoma types and Graves' disease could be differentiated in human histopathology samples. Three parameters were extracted, revealing that the degree of linear polarization and χ(2)zzz/χ(2)zxx were effective in differentiating some diseases, while the parameter χ(2)xyz/χ(2)zxx was less effective.

Investigation of the trajectory uniformity in water dissolution ultraprecision continuous polishing of large-sized KDP crystal

Large-sized potassium dihydrogen phosphate (KDP) crystals are an irreplaceable nonlinear optical component in an inertial confinement fusion project. Restricted by the size, previous studies have been aimed mainly at the removal principle and surface roughness of small-sized KDP crystals, with less research on flatness. Due to its low surface damage and high machining efficiency, water dissolution ultraprecision continuous polishing (WDUCP) has become a good technique for processing large-sized KDP crystals. In this technique, the trajectory uniformity of water droplets can directly affect the surface quality, such as flatness and roughness. Specifically, uneven trajectory distribution of water droplets on the surface of KDP crystals derived from the mode of motion obviously affects the surface quality. In this study, the material removal mechanism of WDUCP was introduced. A simulation of the trajectory of water droplets on KDP crystals under different eccentricity modes of motion was then performed. Meanwhile, the coefficient of variation (CV) was utilized to evaluate the trajectory uniformity. Furthermore, to verify the reliability of the simulation, some experimental tests were also conducted by employing a large continuous polisher. The results showed that the CV varied from 0.67 to 2.02 under the certain eccentricity mode of motion and varied from 0.48 to 0.65 under the uncertain eccentricity mode of motion. The CV of uncertain eccentricity is always smaller than that of certain eccentricity. Hence, the uniformity of trajectory was better under uncertain eccentricity. Under the mode of motion of uncertain eccentricity, the initial surface texture of the 100 mm × 100 mm × 10 mm KDP crystal did achieve uniform planarization. The surface root mean square roughness was reduced to 2.182 nm, and the flatness was reduced to 22.013 μm. Therefore, the feasibility and validity of WDUCP for large-sized KDP crystal were verified.

Magnesium-and-Zinc-Doped Lithium Niobate Crystals: Preparation and Characterization

Double-doping technology for growing lithium niobate crystals (LiNbO3:Mg:Zn) was developed. The crystals were highly homogeneous and had high optical damage resistance, so they show promise for use as photonic and nonlinear optical components. The crystals were grown from the LiNbO3:0.145 wt % Mg:1.98 wt % Zn batch. The batch was prepared by homogeneous doping. The proposed flowsheet can serve as the basis for a large-scale technology of doped lithium niobate single crystals.

Lead sulfide nanoparticles for dual-wavelength ultrashort pulse generation

Nanoparticle materials have many potential applications in the area of electronics and optoelectronics due to their unique and versatile properties. In particular, lead sulfide nanoparticles (PbS NPs) have shown excellent ultrafast photonics and can be applied to communication systems because of their low bandgap, high thermal damage threshold and stability. The wavelength division multiplexor (WDM) technique is vital to fiber optical communication, which allows the transmission of many different-wavelength signals in one fiber cable. However, PbS NPs for multi-wavelength pulse generation has not been reported until now. In this work, PbS NPs have been investigated and successfully applied in an Er-doped fiber laser as a saturable absorber (SA) to generate a dual-wavelength short pulse for the first time. A picosecond-level ultrashort pulse at center wavelengths of 1545 and 1585 nm can be achieved simultaneously or respectively. It is worth mentioning that the two wavelengths are separated up to 40 nm, which can significantly expand the optical communication capacity. The result suggests that PbS NPs as smart nonlinear optical components have wide applications in optical communications, short-pulse lasers, and even high-performance photodectors.

Modal Symmetry Controlled Second-Harmonic Generation by Propagating Plasmons.

A new concept for second-harmonic generation (SHG) in an optical nanocircuit is proposed. We demonstrate both theoretically and experimentally that the symmetry of an optical mode alone is sufficient to allow SHG even in centro-symmetric structures made of centro-symmetric material. The concept is realized using a plasmonic two-wire transmission-line (TWTL), which simultaneously supports a symmetric and an antisymmetric mode. We first confirm that emission of second-harmonic light into the symmetric mode of the waveguide is symmetry-allowed when the fundamental excited waveguide modes are either purely symmetric or antisymmetric. We further switch the emission into the antisymmetric mode when a controlled mixture of the fundamental modes is excited simultaneously. Our results open up a new degree of freedom into the designs of nonlinear optical components and should pave a new avenue toward multifunctional nanophotonic circuitry.

An all-optical photorefractive miktoarm star polymer synthesized via a combination of RAFT polymerization and click reaction

Aiming to obtain effective calix[4]resorcinarene (CRA)-based photorefractive (PR) materials, three star polymers CRA-PCAH4, CRA-PCAH8 and CRA-PCAH4-PCH4 were prepared via a combination of reversible addition-fragmentation chain transfer (RAFT) polymerization and click reaction. CRA-PCAH4 and CRA-PCAH8 bearing only carbazole-azo-nitrobenzene-based polymeric arms exhibited poor solubility in low boiling point solvents because of the strong interchain electrostatic interactions. While the miktoarm star polymer CRA-PCAH4-PCH4, which was prepared based on CRA-PCAH4 by introducing some carbazole-based polymer arms (PCH) as buffering chains to isolate the nonlinear optical (NLO) components in the CRA core, exhibited good solubility in tetrahydrofuran (THF). A composite based on CRA-PCAH4-PCH4 showed much better PR performance than that of the corresponding PCAH arm tested via a two-beam coupling (TBC) experiment under zero electric field without pre-poling.