Volume 8, Issue 9 - Special Issue: Interdisciplinary Nanophotonics; Guest Editors: E. Di Fabrizio and M. Stockman

By means of time-resolved photoluminescence (TR-PL) spectroscopy, we present a detailed investigation of the carrier relaxation dynamics in a CsPbBr 3 bulk sample and microcrystal ensemble at cryogenic temperature on a picosecond time scale. We provide evidence of a long temperature-dependent cooling rate for the excitons and free carriers population, with an initial cooling time constant of a few tens of picoseconds. A relaxation bottleneck in the thermalization process was found that cannot be explained by the Auger effect or hot phonon population, since we address a very low excitation regime, not commonly investigated in literature, where such processes are not effective. Adding a continuous wave optical bias to the picosecond excitation, we probed the photoinduced PL decrease of the localized states and the photoinduced PL increase of the population in the high energy states. A long recovery time from the photoinduced PL decrease was found for localized states and quite significant differences were detected, depending on the resonance/off resonance bias used in the experiment.

Silver nanoparticles (AgNPs) show an extraordinary strong interaction with light, which enables confinement and field enhancement at the nanoscale. However, despite their localized nature, such phenomena are often sought to be exploited on a larger device length scale, for example, in sensors, solar cells, or photocatalytic cells. Unfortunately, this is often limited by strong absorption. One way to reduce these losses is to first focus light with low loss dielectric optics and then to place the AgNPs in that focus. Here, we present a clear experimental proof that growth of AgNPs from the liquid phase at a substrate surface can be controlled by light. Violet light of 405 nm and 1.5 W/cm 2 is coupled into thin film resonators and locally focused at their surface. The AgNPs grow at the focus position with sub-Abbe alignment accuracy. Numerical simulations confirm that this alignment causes an increased field enhancement within the AgNPs and is therefore expected to lead to an improved performance of the resulting hybrid devices.

The inherent ability of plasmonic bowtie nanoapertures (NAs) to localize the electromagnetic field at a subwavelength scale was exploited to engineer the H removal process in dilute nitrides at the nanometer level. Dilute nitride semiconductor alloys (e.g. GaAsN with a small percentage of nitrogen) are characterized by peculiar optoelectronic properties and, most importantly, by an even more peculiar response to hydrogen incorporation. In this class of materials, it is indeed possible to tune post-growth the alloy bandgap energy by a controlled incorporation of hydrogen atoms. The formation of N-H complexes neutralizes all the effects N has on the host matrix, among which is the strong narrowing of bandgap energy. In the present work, bowtie NAs resonant to the N-H complex dissociation energy were numerically modeled by finite element method simulations, realized by a lithographic approach, and characterized by scanning probe microscopy and resonant scattering spectroscopies. The conditions to get the maximum field enhancement at a specific position below the metal/semiconductor interface, namely at the dilute nitride quantum well position, were identified, demonstrating the ability to achieve a plasmon-assisted spatially selective hydrogen removal in a GaAsN/GaAs quantum well sample. Hydrogen removal through bowtie NAs turns out to be way more efficient (approximately two orders of magnitude) than through the plain surface, thus indicating that bandgap engineering through plasmonic nanostructures can be optimized for future efficient realization of site-controlled single-photon emitters and for their deterministic integration in plasmonic devices.

Surface-enhanced Raman scattering (SERS) sensors using specific aptamers often show difficulties in quantitative analysis because the instable aptamer structures show fluctuated background signals. In this communication, we address the quantitative analysis of the SERS spectra of manganese superoxide dismutase (MnSOD) in different concentrations over the signal arisen from its specific aptamer using multivariate statistical analysis. MnSOD is a primary antioxidant enzyme protecting normal tissue against oxidative stress and is known as a cancer biomarker. By applying principal component analysis, SERS spectra were distinguished when MnSOD was present in a specimen even at 10 p m . The relation between SERS spectra and MnSOD concentrations calculated by partial least-squares regression predicted MnSOD concentrations within one order of magnitude. Moreover, statistically obtained spectral correlations reveal that spectral differences did not originate from additional peaks of MnSOD but from the thermodynamic stability of the aptamer structures. These results open new paths for detection and analytical strategies of SERS-based bio-sensors using aptamers.

Slow light is a very important concept in nanophotonics, especially in the context of photonic crystals. In this work, we apply our previous design of band-edge slow light in silicon waveguide gratings [M. Passoni et al, Opt. Express 26, 8470 (2018)] to Mach-Zehnder modulators based on the plasma dispersion effect. The key idea is to employ an interleaved p-n junction with the same periodicity as the grating, in order to achieve optimal matching between the electromagnetic field profile and the depletion regions of the p-n junction. The resulting modulation efficiency is strongly improved as compared to common modulators based on normal rib waveguides, even in a bandwidth of 20–30 nm near the band edge, while the total insertion loss due to free carriers is not increased. The present concept is promising in view of realizing slow-light modulators for silicon photonics with reduced energy dissipation.

Deoxyribonucleic acid (DNA) detection is essential for the accurate and early diagnosis of a disease. In this study, a femtomolar DNA detection method based on the exploitation of the localized surface plasmon (LSP) resonance of gold nanoparticles (AuNPs) was developed. We prepared Poly Ethylen Glycol (PEG) functionalized AuNPs with a specific DNA capture probe (CP) directly modified on the gold surface. Two strategies are proposed using different kinds of CP to detect the target DNA (tDNA). In the first strategy, CP is the complementary of the complete sequence of the DNA (CCP method). For the second strategy, we used two CPs, which were half complementary to tDNA, and these were hybridized with tDNA to form sandwich structures (MIX method). The results showed that our detection methods are highly sensitive and that the limits of detection of 124 a m and 2.54 f m tDNA can be reached when using the CCP and MIX methods, respectively. In addition, the specificity of our two strategies is also demonstrated with mismatched DNAs. The proposed method provides a simple, fast, sensitive and specific DNA biosensor, which has the potential to be used for point-of-care tests (POCT).

The coupling between multiple nanocavities in close vicinity leads to the hybridization of their modes. Stacked metal-insulator-metal (MIM) nanocavities constitute a highly versatile and very interesting model system to study and engineer such mode coupling, as they can be realized by lithography-free fabrication methods with fine control on the optical and geometrical parameters. The resonant modes of such MIM cavities are epsilon-near-zero (ENZ) resonances, which are appealing for nonlinear photophysics and a variety of applications. Here, we study the hybridization of ENZ resonances in MIMIM nanocavities, obtaining a very large mode splitting reaching 0.477 eV, Q -factors of the order of 40 in the visible spectral range, and fine control on the resonance wavelength and mode linewidth by tuning the thickness of the dielectric and metallic layers. A semiclassical approach that analyzes the MIMIM structure as a double quantum well system allows to derive the exact analytical dispersion relation of the ENZ resonances, achieving perfect agreement with numerical simulations and experiments. Interestingly, the asymmetry of the mode splitting in a symmetric MIMIM cavity is not reflected in the classical model of coupled oscillators, which can be directly related to quantum mechanical tunneling for the coupling of the two cavities. Interpreting the cavity resonances as resonant tunneling modes elucidates that they can be excited without momentum matching techniques. The broad tunability of high-quality ENZ resonances together with their strong coupling efficiency makes such MIMIM cavities an ideal platform for exploring light-matter interaction, for example, by the integration of quantum emitters in dielectric layers.

Hybrid cavity-antenna systems have been proposed to combine the sub-wavelength light confinement of plasmonic antennas with microcavity quality factors Q . Here, we examine what confinement and Q can be reached in these hybrid systems, and we address their merits for various applications in classical and quantum optics. Specifically, we investigate their applicability for quantum-optical applications at noncryogenic temperatures. To this end we first derive design rules for hybrid resonances from a simple analytical model. These rules are benchmarked against full-wave simulations of hybrids composed of state-of-the-art nanobeam cavities and plasmonic-dimer gap antennas. We find that hybrids can outperform the plasmonic and cavity constituents in terms of Purcell factor, and additionally offer freedom to reach any Q at a similar Purcell factor. We discuss how these metrics are highly advantageous for a high Purcell factor, yet weak-coupling applications, such as bright sources of indistinguishable single photons. The challenges for room-temperature strong coupling, however, are far more daunting: the extremely high dephasing of emitters implies that little benefit can be achieved from trading confinement against a higher Q , as done in hybrids. An attractive alternative could be strong coupling at liquid nitrogen temperature, where emitter dephasing is lower and this trade-off can alleviate the stringent fabrication demands required for antenna strong coupling. For few-emitter strong-coupling, high-speed and low-power coherent or incoherent light sources, particle sensing and vibrational spectroscopy, hybrids provide the unique benefit of very high local optical density of states, tight plasmonic confinement, yet microcavity Q .

Phthalocyanines are frequently used as probing molecules in the field of single-molecule surface-enhanced Raman spectroscopy (SERS) and tip-enhanced Raman spectroscopy (TERS). In this work, we systematically compare the SERS and TERS spectra from a thin cobalt phthalocyanine (CoPc) film that is deposited on a Au film. The contributions from electromagnetic (EM), resonance, and charge-transfer enhancements are discussed. Radially and azimuthally polarized vector beams are used to investigate the influences of molecular orientation and the localized surface plasmon resonance (SPR). Furthermore, two different excitation wavelengths (636 and 532 nm) are used to study the resonant excitation effect as well as the involvement of the charge-transfer processes between CoPc and the Au substrate. It is shown that the Raman peaks of CoPc are mostly enhanced by 636 nm excitation through a combination of resonant excitation, high EM enhancement, and chemical enhancement via charge transfer from the metal to the molecule. At 532 nm excitation, however, the SERS and TERS spectra are dominated by photoluminescence, which originates from a photo-induced charge-transfer process from the optically excited molecule to the metal. The contributions of the different enhancement mechanisms explain the optical contrasts seen in the TERS images of Au nanodisks covered by the CoPc film. The insight achieved in this work will help to understand the optical contrast in sub- or single-molecule TERS imaging and apply SERS or TERS in the field of photocatalysis.

Two-dimensional semiconductors are considered intriguing materials for photonic applications, thanks to their stunning optical properties and the possibility to manipulate them at the nanoscale. In this review, we focus on transition metal dichalcogenides and low-dimensional hybrid organic-inorganic perovskites, which possess the same characteristics related to planar confinement of their excitons: large binding energies, wide exciton extension, and high oscillator strength. We describe their optoelectronic properties and their capability to achieve strong coupling with light, with particular attention to polariton-polariton interactions. These aspects make them very attractive for polaritonic devices working at room temperature, in view of the realization of all-optical logic circuits in low-cost and easy-to-synthesize innovative materials.

Electro-optic signal modulation provides a key functionality in modern technology and information networks. Photonic integration has not only enabled miniaturizing photonic components, but also provided performance improvements due to co-design addressing both electrical and optical device rules. The millimeter to centimeter footprint of many foundry-ready electro-optic modulators, however, limits density scaling of on-chip photonic systems. To address these limitations, here we experimentally demonstrate a coupling-enhanced electro-absorption modulator by heterogeneously integrating a novel dual-gated indium-tin-oxide phase-shifting tunable absorber placed at a silicon directional coupler region. This concept allows utilizing the normally parasitic Kramers-Kronig relations here in an synergistic way resulting in a strong modulation depth to insertion loss ratio of about 1. Our experimental modulator shows a 2 dB extinction ratio for a just 4 μm short device at 4 V bias. Since no optical resonances are deployed, this device shows spectrally broadband operation as demonstrated here across the entire C-band. In conclusion, we demonstrate a modulator utilizing strong index change from both real and imaginary parts of active material enabling compact and high-performing modulators using semiconductor near-foundry materials.

The luminescence and inner structure of GaAs-AlGaAs quantum well tube (QWT) nanowires were studied using low-temperature cathodoluminescence (CL) spectroscopic imaging, in combination with scanning transmission electron microscopy (STEM) tomography, allowing for the first time a robust correlation between the luminescence properties of these nanowires and their size and inner 3D structure down to the nanoscale. Besides the core luminescence and minor defects-related contributions, each nanowire showed one or more QWT peaks associated with nanowire regions of different diameters. The values of the GaAs shell thickness corresponding to each QWT peak were then determined from the nanowire diameters by employing a multishell growth model upon validation against experimental data (core diameter and GaAs and AlGaAs shell thickness) obtained from the analysis of the 3D reconstructed STEM tomogram of a GaAs-AlGaAs QWT nanowire. We found that QWT peak energies as a function of thus-estimated (3–7 nm) GaAs shell thickness are 40–120 meV below the theoretical values of exciton recombination for uniform QWTs symmetrically wrapped around a central core. However, the analysis of the 3D tomogram further evidenced azimuthal asymmetries as well as (azimuthal and axial) random fluctuations of the GaAs shell thickness, suggesting that the red-shift of QWT emissions is prominently due to carrier localization. The CL mapping of QWT emission intensities along the nanowire axis allowed to directly image the nanoscale localization of the emission, supporting the above picture. Our findings contribute to a deeper understanding of the luminescence-structure relationship in QWT nanowires and will foster their applications as efficient nanolaser sources for future monolithic integration onto silicon.