We present an all-dielectric germanium nanosystem exhibiting a strong third order nonlinear response and efficient third harmonic generation in the optical regime. A thin germanium nanodisk shows a ...pronounced valley in its scattering cross section at the dark anapole mode, while the electric field energy inside the disk is maximized due to high confinement within the dielectric. We investigate the dependence of the third harmonic signal on disk size and pump wavelength to reveal the nature of the anapole mode. Each germanium nanodisk generates a high effective third order susceptibility of χ(3) = 4.3 × 10–9 esu, corresponding to an associated third harmonic conversion efficiency of 0.0001% at an excitation wavelength of 1650 nm, which is 4 orders of magnitude greater than the case of an unstructured germanium reference film. Furthermore, the nonlinear conversion via the anapole mode outperforms that via the radiative dipolar resonances by about 1 order of magnitude, which is consistent with our numerical simulations. These findings open new possibilities for the optimization of upconversion processes on the nanoscale through the appropriate engineering of suitable dielectric materials.
Benefiting from large intrinsic nonlinearities, low absorption, and high field enhancement abilities, all-dielectric nanoantennas are considered essential for efficient nonlinear processes at ...subwavelength volumes. In particular, when the dielectric nanoantenna supports the nonradiating anapole mode, characterized by a minimum in the extinction cross section and a maximum electric energy within the material, third harmonic generation (THG) processes can be greatly enhanced. In this work, we demonstrate that a higher-order anapole mode in a 200 nm thick germanium nanodisk delivers the highest THG efficiency on the nanoscale at optical frequencies. By doubling the diameter of a disk supporting the fundamental anapole mode, we discover the emergence of an anapole mode of higher order, with a valley in the extinction cross section significantly narrower than that of the fundamental anapole. Under this condition, we observe a highly improved electric field confinement effect within the dielectric disk, leading to THG conversion efficiencies as large as 0.001% at a third harmonic wavelength of 550 nm. In addition, by mapping the THG emission across the nanodisk, we are able to unveil the anapole near-field intensity distributions, which show excellent agreement with numerical simulations. Our findings remarkably expand contemporary knowledge on localized modes in dielectric nanosystems, revealing crucial elements for the elaboration of highly efficient frequency upconversion nanodevices.
Efficient optical frequency mixing typically must accumulate over large interaction lengths because nonlinear responses in natural materials are inherently weak. This limits the efficiency of mixing ...processes owing to the requirement of phase matching. Here, we report efficient four-wave mixing (FWM) over micrometer-scale interaction lengths at telecommunications wavelengths on silicon. We used an integrated plasmonic gap waveguide that strongly confines light within a nonlinear organic polymer. The gap waveguide intensifies light by nanofocusing it to a mode cross-section of a few tens of nanometers, thus generating a nonlinear response so strong that efficient FWM accumulates over wavelength-scale distances. This technique opens up nonlinear optics to a regime of relaxed phase matching, with the possibility of compact, broadband, and efficient frequency mixing integrated with silicon photonics.
Materials with large optical nonlinearity, especially in the visible spectral region, are in great demand for applications in all‐optical information processing and quantum optics. 2D hybrid ...Ruddlesden−Popper‐type halide perovskites (RPPs) with tunable ultraviolet‐to‐visible direct bandgaps exhibit large nonlinear optical responses due to the strong excitonic effects present in their multiple quantum wells. Using a microscopic Z‐scan setup with femtosecond laser pulses tunable across the visible spectrum, it is demonstrated that single‐crystalline lead halide RPP nanosheets possess unprecedentedly large nonlinear refraction and absorption coefficients near excitonic resonances. A room‐temperature insulator (exciton)–metal (plasma) Mott transition is found to occur near the exciton resonance of the thinnest qunatum‐well RPPs, boosting the nonlinear response. Owing to the rapidly changing refractive index near resonance, a single RPP crystal can exhibit different nonlinear functionalities across the excitation spectrum. The results suggest that RPPs are efficient nonlinear materials in the visible waveband, indicating their potential use in integrated nonlinear photonic applications such as optical modulation and switching.
Large excitonic optical nonlinearity in single‐crystalline 2D Ruddlesden–Popper perovskite (RPP) nanosheets characterized by a microscopic Z‐scan setup is reported. A room‐temperature excitonic Mott transition occurs near the exciton resonance of the thinnest quantum‐well RPPs, boosting the nonlinear response. The magnitude and sign of the nonlinear coefficients vary strongly with the excitation wavelength offering various nonlinear functionalities in the visible waveband.
Mass spectrometry-based metabolomics approaches can enable detection and quantification of many thousands of metabolite features simultaneously. However, compound identification and reliable ...quantification are greatly complicated owing to the chemical complexity and dynamic range of the metabolome. Simultaneous quantification of many metabolites within complex mixtures can additionally be complicated by ion suppression, fragmentation and the presence of isomers. Here we present guidelines covering sample preparation, replication and randomization, quantification, recovery and recombination, ion suppression and peak misidentification, as a means to enable high-quality reporting of liquid chromatography- and gas chromatography-mass spectrometry-based metabolomics-derived data.
We present an experimental demonstration of a new class of hybrid gap plasmon waveguides on the silicon-on-insulator (SOI) platform. Created by the hybridization of the plasmonic mode of a gap in a ...thin metal sheet and the transverse-electric (TE) photonic mode of an SOI slab, this waveguide is designed for efficient adiabatic nanofocusing simply by varying the gap width. For gap widths greater than 100 nm, the mode is primarily photonic in character and propagation lengths can be many tens of micrometers. For gap widths below 100 nm, the mode becomes plasmonic in character with field confinement predominantly within the gap region and with propagation lengths of a few microns. We estimate the electric field intensity enhancement in hybrid gap plasmon waveguide tapers at 1550 nm by three-photon absorption of selectively deposited CdSe/ZnS quantum dots within the gap. Here, we show electric field intensity enhancements of up to 167 ± 26 for a 24 nm gap, proving the viability of low loss adiabatic nanofocusing on a commercially relevant photonics platform.
The one-dimensional photovoltaic absorber material Sb2S3 requires crystal orientation engineering to enable efficient carrier transport. In this work, we adopted the vapor transport deposition (VTD) ...method to fabricate vertically aligned Sb2S3 on a CdS buffer layer. Our work shows that such a preferential vertical orientation arises from the sulfur deficit of the CdS surface, which creates a beneficial bonding environment between exposed Cd2+ dangling bonds and S atoms in the Sb2S3 molecules. The CdS/VTD-Sb2S3 interface recombination is suppressed by such properly aligned ribbons at the interface. Compared to typical 120-oriented Sb2S3 films deposited on CdS by the rapid thermal evaporation (RTE) method, the VTD-Sb2S3 thin film is highly 211- and 121-oriented and the performance of the solar cell is increased considerably. Without using any hole transportation layer, a conversion efficiency of 4.73% is achieved with device structure of indium tin oxide (ITO)/CdS/Sb2S3/Au. This work provides a potential way to obtain vertically aligned thin films on different buffer layers.
The HR 8799 system uniquely harbors four young super-Jupiters whose orbits can provide insights into the system's dynamical history and constrain the masses of the planets themselves. Using the ...Gemini Planet Imager, we obtained down to one milliarcsecond precision on the astrometry of these planets. We assessed four-planet orbit models with different levels of constraints and found that assuming the planets are near 1:2:4:8 period commensurabilities, or are coplanar, does not worsen the fit. We added the prior that the planets must have been stable for the age of the system (40 Myr) by running orbit configurations from our posteriors through N-body simulations and varying the masses of the planets. We found that only assuming the planets are both coplanar and near 1:2:4:8 period commensurabilities produces dynamically stable orbits in large quantities. Our posterior of stable coplanar orbits tightly constrains the planets' orbits, and we discuss implications for the outermost planet b shaping the debris disk. A four-planet resonance lock is not necessary for stability up to now. However, planet pairs d and e, and c and d, are each likely locked in two-body resonances for stability if their component masses are above 6 MJup and 7 MJup, respectively. Combining the dynamical and luminosity constraints on the masses using hot-start evolutionary models and a system age of 42 5 Myr, we found the mass of planet b to be 5.8 0.5 MJup, and the masses of planets c, d, and e to be each.
Two-dimensional (2D) hybrid organic–inorganic Ruddlesden–Popper perovskites (RPPs) have been recently shown to exhibit large nonlinear optical properties due to the strong excitonic effects present ...in their multiple quantum wells. In this work, we use nondegenerate pump–probe spectroscopy in the 600–1000 nm wavelength range to study the influence of nonlinear effects on the ultrafast dynamics of 2D RPP thin flakes. We find that, under sub-bandgap excitation, ∼100 nm thick perovskite sheets allow up to ∼2% reflectivity modulation within a 20 fs period, due to the nonlinear optical Kerr effect and two-photon absorption, surpassing by a factor of ∼5 the reported nonlinear performance of photonic metasurfaces and single nanoantennas. When the excitation is resonant with the excitonic absorption, the ultrafast nature of the nonlinear response is lost due to the presence of linear absorption creating long-lived free carriers. Our results suggest that 2D RPPs are potential nanoscale all-optical modulators in the visible/near-infrared waveband for applications such as ultrafast information processing, optical data transmission, and high-performance computing.
Dielectric nanoantennas have recently emerged as promising elements for nonlinear and ultrafast nanophotonics due to their ability to concentrate light on the nanometer scale with low losses, while ...exhibiting large nonlinear susceptibilities. In this work, we demonstrate that single Si nanodisks covered with a thin 30 nm thick layer of Au can generate positive and negative sub-20 fs reflectivity modulations of ∼0.3% in the vicinity of the first-order anapole mode, when excited around the second-order anapole mode. The experimental results, characterized in the visible to near-infrared spectral range, suggest that the nonlinear optical Kerr effect is the responsible mechanism for the observed all-optical switching phenomena. These findings represent an important step toward nanoscale ultrafast all-optical signal processing.
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