Double-sided asymmetric metasurfaces achieving sub-microscale focusing from a GaN green laser diode.

We proposed and demonstrated a highly efficient sub-microscale focusing from a GaN green laser diode (LD) integrated with double-sided asymmetric metasurfaces. The metasurfaces consist of two nanostructures in a GaN substrate: nanogratings on one side and a geometric phase based metalens on the other side. When it was integrated on the edge emission facet of a GaN green LD, linearly polarized emission was firstly converted to the circularly polarized state by the nanogratings functioning as a quarter-wave plate, the phase gradient was then controlled by the metalens on the exit side. In the end, the double-sided asymmetric metasurfaces achieve a sub micro-focusing from linearly polarized states. Experimental results show the full width at half maximum of the focused spot size is about 738 nm at the wavelength 520 nm and the focusing efficiency is about 72.8%. Our results lay a foundation for the multi-functional applications in optical tweezers, laser direct writing, visible light communication, and biological chip.

Highly sensitive surface plasmon resonance sensor with surface modified MoSe2/ZnO composite film for non-enzymatic glucose detection.

The rapid and accurate assessment of glucose concentration has been demonstrated to play a significant role in human health, such as the diagnosis and treatment of diabetes, pharmaceutical research and quality monitoring in the food industry, necessitating further development of the performance for glucose sensor especially at low concentrations. However, glucose oxidase-based sensors suffer from crucial restriction in bioactivity because of their poor environmental tolerance. Recently, catalytic nanomaterials with enzyme-mimicking activity, known as nanozymes, have gained considerable interest to overcome the drawback. In this scenario, we report an inspiring surface plasmon resonance (SPR) sensor for non-enzymatic glucose detection employing ZnO nanoparticles and MoSe2 nanosheets composite (MoSe2/ZnO) as sensing film, featuring desirable advantages of high sensitivity and selectivity, lab-free and low cost. The ZnO was used to specifically recognize and bind glucose, and further signal amplification was realized by incorporating of MoSe2 owing to its larger specific surface area and favorable bio-compatibility, as well as high electron mobility. These unique features of MoSe2/ZnO composite film result in an obvious improvement of sensitivity for glucose detection. Experimental results show that the measurement sensitivity of the proposed sensor could reach 72.17 nm/(mg/mL) and a detection limit of 4.16 µg/mL by appropriately optimizing the componential constitutions of MoSe2/ZnO composite. In addition, the favorable selectivity, repeatability and stability are demonstrated as well. This facile and cost-effective work provides a novel strategy for constructing high-performance SPR sensor for glucose detection and a prospective application in biomedicine and human health monitoring.

Origin of Zenneck-like waves excited by optical nanoantennas in non-plasmonic transition metals.

The scattering properties of metallic optical antennas are typically examined through the lens of their plasmonic resonances. However, non-plasmonic transition metals also sustain surface waves in the visible. We experimentally investigate in this work the far-field diffraction properties of apertured optical antennas milled on non-plasmonic W films and compare the results with plasmonic references in Ag and Au. The polarization-dependent diffraction patterns and the leakage signal emerging from apertured antennas in both kinds of metals are recorded and analyzed. This thorough comparison with surface plasmon waves reveals that surface waves are launched on W and that they have the common abilities to confine the visible light at metal-dielectric interfaces offering the possibility to tailor the far-field emission. The results have been analyzed through theoretical models accounting for the propagation of a long range surface mode launched by subwavelength apertures, that is scattered in free space by the antenna. This surface mode on W can be qualitatively described as an analogy in the visible of the Zenneck wave in the radio regime. The nature of the new surface waves have been elucidated from a careful analysis of the asymptotic expansion of the electromagnetic propagators, which provides a convenient representation for explaining the Zenneck-like character of the excited waves and opens new ways to fundamental studies of surface waves at the nanoscale beyond plasmonics.

Dynamical manipulation of a dual-polarization plasmon-induced transparency employing an anisotropic graphene-black phosphorus heterostructure.

Dynamical tunable plasmon-induced transparency (PIT) possesses the unique characteristics of controlling light propagation states, which promises numerous potential applications in efficient optical signal processing chips and nonlinear optical devices. However, previously reported configurations are sensitive to polarization and can merely operate under specific single polarization. In this work we propose an anisotropic PIT metamaterial device based on a graphene-black phosphorus (G-BP) heterostructure to realize a dual-polarization tunable PIT effect. The destructive interference coupling between the bright mode and dark modes under the orthogonal polarization state pronounced anisotropic PIT phenomenon. The coupling strength of the PIT system can be modulated by dynamically manipulating the Fermi energy of the graphene via the external electric field voltage. Moreover, the three-level plasmonic system and the coupled oscillator model are employed to explain the underlying mechanism of the PIT effect, and the analytical results show good consistency with the numerical calculations. Compared to the single-polarization PIT devices, the proposed device offers additional degrees of freedom in realizing universal tunable functionalities, which could significantly promote the development of next-generation integrated optical processing chips, optical modulation and slow light devices.

Dynamically tunable coherent perfect absorption in topological insulators at oblique incidence.

The effective engineering of light absorption has been the focus of intensive research to realize the novel optoelectronic devices based on a topological insulator, a unique topologically protected surface Dirac-state quantum material with excellent prospects in electronics and photonics. Here, we theoretically proposed a versatile platform for manipulating the light-matter interaction employing the dynamically tunable coherent perfect absorption (CPA) in the topological insulator Bi1.5Sb0.5Te1.8Se1.2(BSTS). By simply varying the phase difference between two coherent counter-propagating beams, the BSTS-based CPA device can be continuously switched from the high transparency state to the strong absorption state, leading to the modulation of absorption ranging from 0.2% to 99.998%. Under the illumination of TE-polarized wave, the high absorption (>90%) can be implemented within a broad range from 0.47 to 1.51 µm through a proper incident angle alteration. In addition, the quasi-CPA wavelength can be flexibly selected by tuning the bulk thickness of BSTS film while maintaining high modulation depth of 104. Such BSTS-based CPA device with flexible tunability, wide absorption modulation range, and high modulation depth is expected to be utilized in a wide range of potential applications such as in next-generation coherent detectors, coherent modulators, all-optical switches, and signal processors.

Highly sensitive detection of Hg2+ employing SPR sensor modified with chitosan/poly (vinyl alcohol)/SnO2 film.

Water contamination by mercury ions (Hg2+) causes irreversible and serious effect on the ambient environment, ecological systems, and human health, necessitating further improvement of Hg2+ monitoring at low concentrations. Here, we proposed a novel surface plasmon resonance (SPR) sensor for Hg2+ detection with desirable advantages of high sensitivity, simple operation, label-free, and low cost, in which the chitosan/poly (vinyl alcohol)/SnO2 composite film was modified on sensing surface as the active layer for sensitivity enhancement. Benefiting from the relatively high refractive index of SnO2 nanoparticles, the evanescent field generated at the metal-solution interface can be significantly enhanced, which results in a 5 times improvement of sensitivity. Through appropriate optimization in the aspects of componential constitutions, the sensor exhibits excellent sensitivity of 25.713 nm/µg/L and ultra-low calculated detection limit of 6.61 ng/L(32.95 pM). Such detection limit is strikingly lower than the limitation (10 nM) in drinking water set by the US Environmental Protection Agency. In addition, the as-prepared sensor presents relatively high selectivity for Hg2+, attributing to plenty of binding sites for specific adsorption produced by functionalized chitosan/poly (vinyl alcohol) composites, which have been furtherly verified by characterization of FTIR and XPS spectra. The proposed sensor also exhibits great repeatability and good time stability for 15 days. This work provides a promising strategy for developing high-performance SPR sensor for Hg2+ detection and a prospective application in environmental monitoring.

Resolved Infrared Spectroscopy of Aqueous Molecules Employing Tunable Graphene Plasmons in an Otto Prism.

Real-time and in situ detection of aqueous solution is essential for bioanalysis and chemical reactions. However, it is extremely challenging for infrared microscopic measurement because of the large background of water absorption. Here, we proposed a wideband-tunable graphene plasmonic infrared biosensor to detect biomolecules in an aqueous environment, employing attenuated total reflection in an Otto prism configuration and tightly confined plasmons in graphene nanoribbons. Benefiting from the graphene plasmonic electric field enhancement, such a biosensor is able to identify the molecular chemical fingerprints without the interference of water absorption. As a proof of concept, the recombinant protein AG and goat anti-mouse immunoglobulin G (IgG) are used as the sensing analytes, of which the vibrational modes (1669 and 1532 cm-1) are very close to the OH-bending mode of water (1640 cm-1). Simulation results show that the fingerprints of protein molecules in the water environment can be selectively enhanced. Therefore, the water absorption is successfully suppressed so that two protein modes can be resolved by sweeping graphene Fermi energy in a wide waveband. By further optimizing the incident angle and graphene mobility to improve the mode energy of graphene plasmons, maximum enhancement factors of 112 and 130 can be achieved for amide I and II bands. Our work provides an effective approach for the highly sensitive and selective in situ identification of aqueous-phase molecular fingerprints in fields of healthcare, food safety, and biochemical sensing.

Nonlinear plasmon-exciton coupling enhances sum-frequency generation from a hybrid metal/semiconductor nanostructure.

The integration of metallic plasmonic nanoantennas with quantum emitters can dramatically enhance coherent harmonic generation, often resulting from the coupling of fundamental plasmonic fields to higher-energy, electronic or excitonic transitions of quantum emitters. The ultrafast optical dynamics of such hybrid plasmon-emitter systems have rarely been explored. Here, we study those dynamics by interferometrically probing nonlinear optical emission from individual porous gold nanosponges infiltrated with zinc oxide (ZnO) emitters. Few-femtosecond time-resolved photoelectron emission microscopy reveals multiple long-lived localized plasmonic hot spot modes, at the surface of the randomly disordered nanosponges, that are resonant in a broad spectral range. The locally enhanced plasmonic near-field couples to the ZnO excitons, enhancing sum-frequency generation from individual hot spots and boosting resonant excitonic emission. The quantum pathways of the coupling are uncovered from a two-dimensional spectrum correlating fundamental plasmonic excitations to nonlinearly driven excitonic emissions. Our results offer new opportunities for enhancing and coherently controlling optical nonlinearities by exploiting nonlinear plasmon-quantum emitter coupling.

Generating Ultrabroadband Deep-UV Radiation and Sub-10 nm Gap by Hybrid-Morphology Gold Antennas.

We experimentally investigate the interaction between hybrid-morphology gold optical antennas and a few-cycle Ti:sapphire laser up to ablative intensities, demonstrating rich nonlinear plasmonic effects and promising applications in coherent frequency upconversion and nanofabrication technology. The two-dimensional array of hybrid antennas consists of elliptical apertures combined with bowties in its minor axis. The plasmonic resonance frequency of the bowties is red-shifted with respect to the laser central frequency and thus mainly enhances the third harmonic spectrum at long wavelengths. The gold film between two neighboring elliptical apertures forms an hourglass-shaped structure, which acts as a "plasmonic lens" and thus strongly reinforces surface currents into a small area. This enhanced surface current produces a rotating magnetic field that deeply penetrates into the substrate. At resonant frequency, the magnetic field is further intensified by the bowties. The resonant frequency of the hourglass is blueshifted with respect to the laser central frequency. Consequently, it spectacularly extends the third harmonic spectrum toward short wavelengths. The resultant third harmonic signal ranges from 230 to 300 nm, much broader than the emission from a sapphire crystal. In addition, the concentration of surface current within the neck of the hourglass antenna results in a structural modification through laser ablation, producing sub-10 nm sharp metallic gaps. Moreover, after laser illumination the optical field hotspots are imprinted around the antennas, allowing us to confirm the subwavelength enhancement of the electric near-field intensity.

Graphene-assisted multilayer structure employing hybrid surface plasmon and magnetic plasmon for surface-enhanced vibrational spectroscopy.

A graphene-assisted vertical multilayer structure is proposed for high performance surface-enhanced Raman scattering (SERS) and surface-enhanced infrared absorption (SEIRA) spectroscopies on a single substrate, employing simultaneous localized surface plasmon in the visible region and magnetic plasmon resonance in the mid-infrared region. Such multilayer structure consists of a monolayer graphene sandwiched between Ag nanoparticles (NPs) and a metal-insulator-metal (MIM) microstructure, which can be easily fabricated by a standard surface micromachining process. Benefiting from the large near field enhancement by the hybrid plasmons in both visible and mid-infrared regions, a high enhancement factor of up to 107 for SERS and 105 for SEIRA can be achieved. Additionally, the strong magnetic resonance of the MIM microstructure can be tuned in broadband to selectively enhance the desired vibration modes of molecules. The strong SERS and SEIRA enhancement together with easy fabrication provides new opportunities for developing integrated plasmonic devices for multispectral detection of molecules on the same substrate.

Strong Spatial and Spectral Localization of Surface Plasmons in Individual Randomly Disordered Gold Nanosponges.

Porous nanosponges, percolated with a three-dimensional network of 10 nm sized ligaments, recently emerged as promising substrates for plasmon-enhanced spectroscopy and (photo)catalysis. Experimental and theoretical work suggests surface plasmon localization in some hot-spot modes as the physical origin of their unusual optical properties, but so far the existence of such hot-spots has not been proven. Here we use scattering-type scanning near-field nanospectroscopy on individual gold nanosponges to reveal spatially and spectrally confined modes at 10 nm scale by recording local near-field scattering spectra. High quality factors of individual hot-spots of more than 40 are demonstrated, predicting high Purcell factors up to 106. The observed field localization and enhancement make such nanosponges an appealing platform for a variety of applications ranging from nonlinear optics to strong-coupling physics.

Magnetic plasmons in a simple metallic nanogroove array for refractive index sensing.

Magnetic plasmons (MPs) refer to the coupling of external electromagnetic waves with a strong magnetic response induced inside the nanostructures. MPs have been widely employed as artificial magnetic atoms to fabricate negative-permeability or negative-refractive-index metamaterials with peculiar electromagnetic properties. Here, we propose a refractive index sensing by utilizing the MP resonances excited in a simple one-dimensional (1D) metallic nanogroove array. We demonstrate a sensitivity up to 1200 nm/RIU with a figure of merit (FOM*) of 15 thanks to the MP resonances that are extremely sensitive to the surrounding media. Importantly, the influence of the local environment effects on the sensing ability is studied. An equivalent inductor-capacitor (LC) model is used to give a precise quantitative description of the sensing performance and reveal the underlying mechanism. Such a MP-based sensor with the ease of fabrication may provide great potentials in designing broadband sensing devices with high performance and compactness.

Mode energy of graphene plasmons and its role in determining the local field magnitudes.

We theoretically study the mode energy of graphene plasmons and its fundamental role in determining the local field magnitudes. While neglecting the magnetic field energy of the mode, we derive a concise expression for the total mode energy, which is independent on the details of the mode field distributions and valid for both propagating and localized modes. We find that the mean square of the local electric fields of a graphene plasmonic mode scales linearly with the light absorption rate of the mode and the electron relaxation time of graphene. The possible strategies for improving the local field magnitudes of graphene plasmons are also discussed. Our theoretical analysis presented here may benefit the design of various graphene-based optical and optoelectronic devices for light-harvesting or energy conversion.

Strong coherent coupling between graphene surface plasmons and anisotropic black phosphorus localized surface plasmons.

The anisotropic plasmons properties of black phosphorus allow for realizing direction-dependent plasmonics devices. Here, we theoretically investigated the hybridization between graphene surface plasmons (GSP) and anisotropic black phosphorus localized surface plasmons (BPLSP) in the strong coupling regime. By dynamically adjusting the Fermi level of graphene, we show that the strong coherent GSP-BPLSP coupling can be achieved in both armchair and zigzag directions, which is attributed to the anisotropic black phosphorus with different in-plane effective electron masses along the two crystal axes. The strong coupling is quantitatively described by calculating the dispersion of the hybrid modes using a coupled oscillator model. Mode splitting energy of 26.5 meV and 19 meV are determined for the GSP-BPLSP hybridization along armchair and zigzag direction, respectively. We also find that the coupling strength can be strongly affected by the distance between graphene sheet and black phosphorus nanoribbons. Our work may provide the building blocks to construct future highly compact anisotropic plasmonics devices based on two-dimensional materials at infrared and terahertz frequencies.

Suppression of Radiative Damping and Enhancement of Second Harmonic Generation in Bull's Eye Nanoresonators.

We report a drastic increase of the damping time of plasmonic eigenmodes in resonant bull's eye (BE) nanoresonators to more than 35 fs. This is achieved by tailoring the groove depth of the resonator and by coupling the confined plasmonic field in the aperture to an extended resonator mode such that spatial coherence is preserved over distances of more than 10 µm. Experimentally, this is demonstrated by probing the plasmon dynamics at the field level using broadband spectral interferometry. The nanoresonator allows us to efficiently concentrate the incident field inside the central aperture of the BE and to tailor its local optical nonlinearity by varying the aperture geometry. By replacing the central circular hole with an annular ring structure, we obtain 50-times higher second harmonic generation efficiency, allowing us to demonstrate the efficient concentration of long-lived plasmonic modes inside nanoapertures by interferometric frequency-resolved autocorrelation. Such a light concentration in a nanoresonator with high quality factor has high potential for sensing and coherent control of light-matter interactions on the nanoscale.

Beaming Visible Light with a Plasmonic Aperture Antenna.

We investigate experimentally the parameter space defining, in the visible range, the far-field diffraction properties of a single circular subwavelength aperture surrounded by periodic circular grooves milled on a metallic film. Diffraction patterns emerging from such an antenna are recorded under parallel- and perpendicular-polarized illumination at a given illumination wavelength. By monitoring the directivity and the gain of the antenna with respect to a single aperture, we point out the role played by the near-field surface plasmon excitations. The results can be analyzed through a Huygens-Fresnel model, accounting for the coherent interaction between the field radiated by the hole and the plasmonic field, propagating along the antenna surface and diffracted away in free space.