The Effect of Nanoparticle Composition on the Surface-Enhanced Raman Scattering Performance of Plasmonic DNA Origami Nanoantennas.

A versatile generation of plasmonic nanoparticle dimers for surface-enhanced Raman scattering (SERS) is presented by combining a DNA origami nanofork and spherical and nonspherical Au or Ag nanoparticles. Combining different nanoparticle species with a DNA origami nanofork to form DNA origami nanoantennas (DONAs), the plasmonic nanoparticle dimers can be optimized for a specific excitation wavelength in SERS. The preparation of such nanoparticle dimers is robust enough to enable the characterization of SERS intensities and SERS enhancement factors of dye-modified DONAs on a single dimer level by measuring in total several thousands of dimers from five different dimer designs, each functionalized with three different Raman reporter molecules and measured at four different excitation wavelengths. Based on these data, SERS enhancement factor (EF) distributions have been determined for each dimer design and excitation wavelengths. The structures and measurement conditions with the highest EFs are suitable for single-molecule SERS (SM-SERS), which is realized by placing single dye molecules into hot spots. We demonstrate that the probability of placing single molecules in a strongly enhancing hot spot for SM-SERS can be increased by using anisotropic nanoparticles with several sharp edges, such as nanoflowers. Combining a Ag nanoparticle with a Au particle in one dimer structure allows for a broadband excitation covering almost the whole visible range. The most versatile plasmonic dimer structure for SERS combines a spherical Ag nanoparticle with a Au nanoflower. Employing the discontinuous Galerkin time domain method, we numerically investigate the bare, symmetric dimers with respect to spectral and near-field properties, showing that, indeed, the nanoflowers induce multiple hot spots located at the edges which surpass the intensity of the spherical dimers, indicating the possibility for SM-SERS. The presented DONA structures and SERS data provide a robust basis for applying such designs as versatile SERS tags and as substrates for SM-SERS measurements.

Optical convolutional neural network with atomic nonlinearity.

Due to their high degree of parallelism, fast processing speeds and low power consumption, analog optical functional elements offer interesting routes for realizing neuromorphic computer hardware. For instance, convolutional neural networks lend themselves to analog optical implementations by exploiting the Fourier-transform characteristics of suitable designed optical setups. However, the efficient implementation of optical nonlinearities for such neural networks still represents challenges. In this work, we report on the realization and characterization of a three-layer optical convolutional neural network where the linear part is based on a 4f-imaging system and the optical nonlinearity is realized via the absorption profile of a cesium atomic vapor cell. This system classifies the handwritten digital dataset MNIST with 83.96% accuracy, which agrees well with corresponding simulations. Our results thus demonstrate the viability of utilizing atomic nonlinearities in neural network architectures with low power consumption.

Enhanced Faraday rotation by dielectric metasurfaces with Bayesian shape-optimized scatterers.

In this Letter, we demonstrate how to optimize the magneto-optic response of a Huygens metasurface composed of square arrays of all-dielectric nano-disk scatterers. We compare cylindrical and shape-modified disks. Both provide a strongly enhanced Faraday rotation that is accompanied by almost 100% transmittance. The shape modification obtained via a Bayesian optimization algorithm results in a 50% increase in the magneto-optic response compared to the best cylindrical disk, providing 15° of polarization rotation for a 260 nm thick metasurface.

Topological protection versus degree of entanglement of two-photon light in photonic topological insulators.

Topological insulators combine insulating properties in the bulk with scattering-free transport along edges, supporting dissipationless unidirectional energy and information flow even in the presence of defects and disorder. The feasibility of engineering quantum Hamiltonians with photonic tools, combined with the availability of entangled photons, raises the intriguing possibility of employing topologically protected entangled states in optical quantum computing and information processing. However, while two-photon states built as a product of two topologically protected single-photon states inherit full protection from their single-photon "parents", a high degree of non-separability may lead to rapid deterioration of the two-photon states after propagation through disorder. In this work, we identify physical mechanisms which contribute to the vulnerability of entangled states in topological photonic lattices. Further, we show that in order to maximize entanglement without sacrificing topological protection, the joint spectral correlation map of two-photon states must fit inside a well-defined topological window of protection.

Dispersion control in a near-infrared subwavelength resonator with a tailored hyperbolic metamaterial.

We demonstrate experimentally and computationally an intricate cavity size dependence of the anomalous near-infrared mode spectrum of an ordinary optical resonator that is combined with a ZnO:Ga-based hyperbolic metamaterial (HMM). Specifically, we reveal the existence of a resonance in subwavelength-sized cavities and demonstrate control over the first-order cavity mode dispersion. We elaborate that these effects arise due to the HMM combining the mode dispersions of purely metallic and purely dielectric cavity cores into a distinct intermediate regime. By tailoring the HMM fill factor, this unique dispersion of a subwavelength resonator can be freely tuned between these two limiting cases.

On the applicability of quantum-optical concepts in strong-coupling nanophotonics.

Rooted in quantum optics and benefiting from its well-established foundations, strong coupling in nanophotonics has experienced increasing popularity in recent years. With nanophotonics being an experiment-driven field, the absence of appropriate theoretical methods to describe ground-breaking advances has often emerged as an important issue. To address this problem, the temptation to directly transfer and extend concepts already available from quantum optics is strong, even if a rigorous justification is not always available. In this review we discuss situations where, in our view, this strategy has indeed overstepped its bounds. We focus on exciton-plasmon interactions, and particularly on the idea of calculating the number of excitons involved in the coupling. We analyse how, starting from an unfounded interpretation of the term N/V that appears in theoretical descriptions at different levels of complexity, one might be tempted to make independent assumptions for what the number N and the volume V are, and attempt to calculate them separately. Such an approach can lead to different, often contradictory results, depending on the initial assumptions (e.g. through different treatments of V as the-ambiguous in plasmonics-mode volume). We argue that the source of such contradictions is the question itself-How many excitons are coupled?, which disregards the true nature of the coupled components of the system, has no meaning and often not even any practical importance. If one is interested in validating the quantum nature of the system-which appears to be the motivation driving the pursuit of strong coupling with small N-one could instead focus on quantities such as the photon emission rate or the second-order correlation function. While many of the issues discussed here may appear straightforward to specialists, our target audience is predominantly newcomers to the field, either students or scientists specialised in different disciplines. We have thus tried to minimise the occurrence of proofs and overly-technical details, and instead provide a qualitative discussion of analyses that should be avoided, hoping to facilitate further growth of this promising area.

Importance of substrates for the visibility of "dark" plasmonic modes.

Dark plasmonic modes have interesting properties, including longer lifetimes and narrower linewidths than their radiative counterpart, and little to no radiative losses. However, they have not been extensively studied yet due to their optical inaccessibility. In this work, we systematically investigated the dark radial breathing modes (RBMs) in monocrystalline gold nanodisks, specifically their outcoupling behavior into the far-field by cathodoluminescence spectroscopy. Increasing the substrate thickness resulted in an up to 4-fold enhanced visibility. This is attributed to breaking the mirror symmetry by the high-index substrate, creating an effective dipole moment. Furthermore, the resonance energy of the dark RMBs can be easily tuned by varying the nanodisk diameter, making them promising candidates for nanophotonic applications.

Broadband Spectrometer with Single-Photon Sensitivity Exploiting Tailored Disorder.

Harnessing tailored disorder for broadband light scattering enables high-resolution signal analysis in nanophotonic spectrometers with a small device footprint. Multiple scattering events in the disordered medium enhance the effective path length which leads to increased resolution. Here we demonstrate an on-chip random spectrometer cointegrated with superconducting single-photon detectors suitable for photon-scarce environments. We combine an efficient broadband fiber-to-chip coupling approach with a random scattering area and broadband transparent silicon nitride waveguides to operate the spectrometer in a diffusive regime. Superconducting nanowire single-photon detectors at each output waveguide are used to perform spectral-to-spatial mapping via the transmission matrix at the system, allowing us to reconstruct a given probe signal. We show operation over a wide spectral range with sensitivity down to powers of -111.5 dBm in the telecom band.

Negative asymmetry parameter in plasmonic core-shell nanoparticles.

Plasmonic nanoparticles with a dielectric-metal core-shell morphology exhibit hybridized modes where the surface plasmon polaritons at the outer and inner surfaces of the shell couple. We demonstrate that suitably tailoring the interference of such hybrid surface plasmon polariton modes leads to composite subwavelength nanospheres with negative asymmetry parameters and strong scattering in the optical frequency range. As a result, for a low density collection of scatterers an anomalous regime occurs, where the extinction mean free path is longer than the transport mean free path. Explicit results for silver-coated nanospheres are presented.

Quantization of Quasinormal Modes for Open Cavities and Plasmonic Cavity Quantum Electrodynamics.

We introduce a second quantization scheme based on quasinormal modes, which are the dissipative modes of leaky optical cavities and plasmonic resonators with complex eigenfrequencies. The theory enables the construction of multiplasmon or multiphoton Fock states for arbitrary three-dimensional dissipative resonators and gives a solid understanding to the limits of phenomenological dissipative Jaynes-Cummings models. In the general case, we show how different quasinormal modes interfere through an off-diagonal mode coupling and demonstrate how these results affect cavity-modified spontaneous emission. To illustrate the practical application of the theory, we show examples using a gold nanorod dimer and a hybrid dielectric-metal cavity structure.

Design study of random spectrometers for applications at optical frequencies.

Compact spectrometers based on disordered planar waveguides exhibit a rather high resolution with a relatively small footprint compared to conventional spectrometers. This is achieved by multiple scattering of light, which-if properly engineered-significantly enhances the effective optical path length. Here a design study of random spectrometers for TE- and TM-polarized light is presented that combines the results of Mie theory, multiple-scattering theory, and full electromagnetic simulations. It is shown that the performance of such random spectrometers depends on single-scattering quantities, notably on the overall scattering efficiency and the asymmetry parameter. Further, the study shows that a well-developed diffusive regime is not required in practice and that a standard integrated-optical layout is sufficient to obtain efficient devices even for rather weakly scattering systems consisting of low index inclusions in high-index matrices, such as pores in planar silicon-nitride-based waveguides. This allows for both significant reductions in footprint with acceptable losses in resolution and for device operation in the visible and near-infrared frequency range.

Mid-infrared beam splitter for ultrashort pulses.

A design is presented for a beam splitter suitable for ultrashort pulses in the mid-infrared and terahertz spectral range consisting of a structured metal layer on a diamond substrate. Both the theory and experiment show that this beam splitter does not distort the temporal pulse shape.

Near-field study on the transition from localized to propagating plasmons on 2D nano-triangles.

In this manuscript we report on a near field study of two-dimensional plasmonic gold nano-triangles using electron energy loss spectroscopy in combination with scanning transmission electron microscopy, as well as discontinuous Galerkin time-domain computations. With increasing nano-triangle size, we observe a transition from localized surface plasmons on small nano-triangles to non-resonant propagating surface plasmon polaritons on large nano-triangles. Furthermore we demonstrate that nano-triangles with a groove cut can support localized as well as propagating plasmons in the same energy range.

Limitations of Particle-Based Spasers.

We present a semiclassical analytic model for spherical core-shell surface plasmon lasers. Within this model, we drop the widely used one-mode approximations in favor of fully electromagnetic Mie theory. This allows for incorporation of realistic gain relaxation rates that so far are massively underestimated. Especially, higher order modes can undermine and even reverse the beneficial effects of the strong Purcell effect in such systems. Our model gives a clear view on gain and resonator requirements, as well as on the output characteristics that will help experimenters to design more efficient particle-based spasers.

Growth and characterization of SiGeSn quantum well photodiodes.

We report on the fabrication and electro-optical characterization of SiGeSn multi-quantum well PIN diodes. Two types of PIN diodes, in which two and four quantum wells with well and barrier thicknesses of 10 nm each are sandwiched between B- and Sb-doped Ge-regions, were fabricated as single-mesa devices, using a low-temperature fabrication process. We discuss measurements of the diode characteristics, optical responsivity and room-temperature electroluminescence and compare with theoretical predictions from band structure calculations.

Scanning single quantum emitter fluorescence lifetime imaging: quantitative analysis of the local density of photonic states.

Their intrinsic properties render single quantum systems as ideal tools for quantum enhanced sensing and microscopy. As an additional benefit, their size is typically on an atomic scale that enables sensing with very high spatial resolution. Here, we report on utilizing a single nitrogen vacancy center in nanodiamond for performing three-dimensional scanning-probe fluorescence lifetime imaging microscopy. By measuring changes of the single emitter's lifetime, information on the local density of optical states is acquired at the nanoscale. Three-dimensional ab initio discontinuous Galerkin time-domain simulations are used in order to verify the results and to obtain additional insights. This combination of experiment and simulations to gather quantitative information on the local density of optical states is of direct relevance for the understanding of fundamental quantum optical processes as well as for the engineering of novel photonic and plasmonic devices.

Quantitative spectroscopy on individual wire, slot, bow-tie, rectangular, and square-shaped optical antennas.

By using a recently introduced approach combining a focus-modulation technique with a common-path interferometer, we measure quantitatively the extinction, scattering, and absorption cross-section spectra of individual optical antennas. The experimental results on thin-wire antennas, slot antennas, bow-tie antennas, rectangular antennas, and square-shaped antennas resonating at around 1.4 µm wavelength are discussed. We find increased resonant scattering cross sections for the latter four antennas compared to the thin-wire antenna, both in absolute terms and relative to the absorption cross section. The square-shaped antenna's resonant extinction cross section approaches the limit of a coherent point dipole. However, the ratio of the resonant extinction cross section to the geometrical cross section of 38 is largest for the simple thin-wire antenna.

Correlated photons in one-dimensional waveguides.

We study two-photon transport in a one-dimensional waveguide with a side-coupled two-level system. Depending on the momentum of the incoming photons, we find that the nature of the scattering process changes considerably. We further show that bunching behavior can be found in the scattered light. As a result, we find that the waveguide dispersion has a strong influence on the photon correlations. By modifying the momentum of the pulse, the nature of the correlations can therefore be altered or optimized.

Simple magneto-optic transition metal models for time-domain simulations.

Efficient modelling of the magneto-optic effects of transition metals such as nickel, cobalt and iron is a topic of growing interest within the nano-optics community. In this paper, we present a general discussion of appropriate material models for the linear dielectric properties for such metals, provide parameter fits and formulate the anisotropic response in terms of auxiliary differential equations suitable for time-domain simulations. We validate both our material models and their implementation by comparing numerical results obtained with the Discontinuous Galerkin time-domain (DGTD) method to analytical results and previously published experimental data.

B-spline modal method: a polynomial approach compared to the Fourier modal method.

A detailed analysis of the B-spline Modal Method (BMM) for one- and two-dimensional diffraction gratings and a comparison to the Fourier Modal Method (FMM) is presented. Owing to its intrinsic capability to accurately resolve discontinuities, BMM avoids the notorious problems of FMM that are associated with the Gibbs phenomenon. As a result, BMM facilitates significantly more efficient eigenmode computations. With regard to BMM-based transmission and reflection computations, it is demonstrated that a novel Galerkin approach (in conjunction with a scattering-matrix algorithm) allows for an improved field matching between different layers. This approach is superior relative to the traditional point-wise field matching. Moreover, only this novel Galerkin approach allows for an competitive extension of BMM to the case of two-dimensional diffraction gratings. These improvements will be very useful for high-accuracy grating computations in general and for the analysis of associated electromagnetic field profiles in particular.