Gap Plasmon Research Articles

Numerical Study of the Wide‐angle Polarization‐Independent Ultra‐Broadband Efficient Selective Solar Absorber in the Entire Solar Spectrum

Increasing the absorption efficiency of solar radiation has great significance for the renewable energy applications, such as residential water heating, seawater desalination, wastewater treatment and solar thermophotovoltaic devices. Optical absorbers based on metamaterials have been widely investigated using a variety of structural designs. However, the near‐ideal solar thermal absorber has not yet been demonstrated, which has a near unity absorption from the ultraviolet to the near‐infrared region and meanwhile an absorption close to zero in the mid‐infrared region. Here, using FEM and FDTD methods respectively, we propose and numerically demonstrate an ultra‐broadband selective solar absorber with an extremely high absorption efficiency above 99% within the range of 435–1520 nm. And meanwhile the emissivity of the nanostructure is below 20% in mid‐infrared region. The total photothermal conversion efficiency of the proposed solar absorber can reach 91.53%, which is very close to the photothermal conversion efficiency (95.6%) of the ideal cut‐off absorber. The physical mechanisms of the nearly perfect absorption are also investigated and analyzed clearly, which is attributed to the hybridization of localized surface plasmon resonance, gap plasmon resonance, and propagating surface plasmon resonance. Particularly, the near‐ideal efficient selective absorption can still be maintained very well at a wide incident angle regardless of the incident light polarization. Owing to the characteristics such as polarization and angle independence, broadband operation, near‐perfect absorption and strong spectral selectivity, the solar absorbers are promising candidates for solar energy harvesting, stealth technology, and thermo‐photovoltaic energy conversion.

Active coherent control of nanoscale light confinement: Modulation of plasmonic modes and position of hotspots for surface-enhanced Raman scattering detection

Multistep plasmonic nanostructures can induce the deep modulation of electromagnetic-field interactions on the nanoscale for positioning hotspots, and this generation of enhanced fields is important in many optical applications. In this article, a new strategy is proposed for fabricating a plasmonic doublestacked nanocone (DSC) nanostructure. In the DSC structure, a tunable plasmonic hybrid mode proceeds from the strong coupling of the plasmonic resonance of a fundamental cavity mode with a localized surface plasmon gap mode. In the nanostructure, the far-field response is deeply modulated and the hottest spots can be effectively positioned on the top surface of the DSC nanostructure. A controllable and cost-effective mask-reconfiguration technique for manufacturing the multiscale nanostructure is developed, which guarantees the generation of the introduced crucial stage on the DSC nanostructure. To evaluate the features of the plasmonic resonance, the DSC nanostructure is used as a surface-enhanced Raman scattering (SERS) substrate for detecting 4-mercaptopyridine molecules under specific excitation conditions. Its good performance, with an average measured SERS enhancement factor as high as 108, demonstrates its strong plasmonic-mode hybridization and extreme field enhancement.

Third-order gap plasmon based metasurfaces for visible light.

Efficient control and manipulation of light using metasurfaces requires high fabrication accuracy that becomes progressively demanding when decreasing the operation wavelength. Considering gap surface plasmon (GSP) based metasurfaces, we demonstrate that the metasurfaces, which utilize the third-order GSP resonance and thereby involve relatively large nanobricks, can successfully be used for efficient polarization-controlled steering of visible light. The reflection amplitude and phase maps for a 450 nm period array of 50 nm thick nanobricks placed atop a 40 nm thick silica layer supported by an optically thick gold film are calculated for the operation wavelength of 633 nm. Exploiting the occurrence of the third-order GSP resonance for nanobricks having their lengths close to 300 nm, we design the phase-gradient metasurface, representing an array of (450 x 2250 nm2) supercells made of 5 nanobricks with different dimensions, to operate as a polarization beam splitter for linearly polarized light. The fabricated polarization beam splitter is characterized using a supercontinuum light source at the normal light incidence and found to exhibit a polarization contrast ratio of up to 40 dB near the design wavelength of 633 nm while showing better than 20 dB contrast in the range of 550 - 650 nm for both polarizations. The diffraction efficiency experimentally measured at normal incidence exceeds 10% (20% in simulations) at the design wavelength of 633 nm, with the performance for the TE polarization (electric field perpendicular to the plane of diffraction) being significantly better (experimentally > 20% and theoretically > 40%) than for the TM polarization. This difference becomes even more pronounced for the light incidence deviating from normal. Finally, we discuss possible improvements of the performance of polarization beam splitters based on third-order GSP resonance as well as other potential applications of the suggested approach.

Multiple-band perfect absorbers based on the combination of Fabry-Perot resonance and the gap plasmon resonance

To realize multiple-band perfect absorption, a novel nanostructure consisting of subwavelength periodic metallic grating and a thick metallic substrate, separated by a thin dielectric spacer(MGDM), is proposed in this paper. Compared with the structures without the dielectric spacer, the designed MGDM nanostructure not only possesses the absorption peaks caused by the Fabry-Perot resonance in the grating slits, but also possesses additional absorption peaks. Numerical simulation results show that the additional absorption peaks are caused by the gap plasmon resonance in the dielectric spacer. Besides, the influence of structural parameters on the absorption properties of MGDM are also thoroughly investigated. The combination of Fabry-Perot resonance and the gap plasmon resonance in the proposed MGDM provide another route for designing multiple-band perfect absorber nanostructures, which have an extensive applications in photo-detecting, photo-conversion or photo-harvesting.

Mode Modification of Plasmonic Gap Resonances Induced by Strong Coupling with Molecular Excitons

Plasmonic cavities can be used to control the atom-photon coupling process at the nanoscale, since they provide an ultrahigh density of optical states in an exceptionally small mode volume. Here we demonstrate strong coupling between molecular excitons and plasmonic resonances (so-called plexcitonic coupling) in a film-coupled nanocube cavity, which can induce profound and significant spectral and spatial modifications to the plasmonic gap modes. Within the spectral span of a single gap mode in the nanocube-film cavity with a 3 nm wide gap, the introduction of narrow-band J-aggregate dye molecules not only enables an anticrossing behavior in the spectral response but also splits the single spatial mode into two distinct modes that are easily identified by their far-field scattering profiles. Simulation results confirm the experimental findings, and the sensitivity of the plexcitonic coupling is explored using digital control of the gap spacing. Our work opens up a new perspective to study the strong coupling process, greatly extending the functionality of nanophotonic systems, with the potential to be applied in cavity quantum electrodynamic systems.

Switchable Metal-Insulator Phase Transition Metamaterials.

We investigate the switching of a gap plasmon tunnel junction between conducting and insulating states. Hysteresis is observed in the second and the third harmonic generation power dependence, which arises by thermally induced disorder ("melting") of a two-carbon self-assembled monolayer between an ultraflat gold surface and metal nanoparticles. The hysteresis is observed for a variety of nanoparticle sizes, but not for larger tunnel junctions where there is no appreciable tunneling. By combining quantum corrected finite-difference time-domain simulations with nonlinear scattering theory, we calculate the changes in the harmonic generation between the tunneling and the insulating states, and good agreement is found with the experiments. This paves the way to a new class of metal-insulator phase transition switchable metamaterials, which may provide next-generation information processing technologies.

Nonresonant 104 Terahertz Field Enhancement with 5-nm Slits

Transmission of Terahertz (THz) electromagnetic wave through a substrate is encumbered because of scattering, multiple reflections, absorption, and Fabry–Perot effects when the wave interacts with the substrate. We present the experimental realization of nonresonant electromagnetic field enhancement by a factor of almost 104 in substrate-free 5-nm gold nanoslits. Our nanoslits yielded greater than 90% normalized electric field transmission in the low-frequency THz region; the slit width was 5 nm, and the gap coverage ratio was 10−4 of the entire membrane, 0.42 mm2. This large field enhancement was attributed to gap plasmons generated by the THz wave, which squeezes the charge cross-section, thus enabling very highly dense oscillating charges and strong THz field transmission from the nanoslits.

Gap-plasmon of Fe3O4@Ag core-shell nanostructures for highly enhanced fluorescence detection of Rhodamine B

A novel gap-plasmon of Fe3O4@Ag core-shell nanoparticles for surface enhanced fluorescence detection of Rhodamine B (RB) was developed. Fe3O4@Ag core-shell nanostructures with Ag shell and Fe3O4 core were synthetized by self-assembled method with the assistance of 3-mercaptopropyl trimethoxy silane (MPTS). To study the RB fluorescence enhanced by gap-plasmon, the fluorescence properties of RB on the substrates with different nanogap densities were systematically investigated, and the results showed that the fluorescence intensity of RB on Fe3O4@Ag core-shell NPs substrate was much stronger than that on bare glass substrate, and the fluorescence intensity was further improved by using multilayer Fe3O4@Ag core-shell NPs substrate which had higher nanogap density. Different from the mechanism that is based on the maximum overlap of the surface plasmon resonance (SPR) band and emission band, the mechanism of the fluorescence enhancement in our work is based on the localized surface plasmon (LSP) and the gap plasmon near-field coupling with the Fe3O4@Ag core-shell NPs. Besides, the detection limit obtained was as low as 1×10-7 mol/L, and the Fe3O4@Ag core-shell NPs substrate had high selectivity for RB fluorophores. It was demonstrated that the Fe3O4@Ag core-shell NPs substrate had activity, good stability, and selectivity for fluorescence detection of RB. And the detection of RB by the surface plasmon enhanced fluorescence was more convenient and rapid than the traditional detection methods in previous works.

Converting State of Polarization With a Miniaturized Metasurface Device

We have designed and experimentally demonstrated a radial and azimuthal polarization converter, which is a plasmonic metasurface with a radius of not more than $5~\mu \text{m}$ . The metasurface is composed of an array of metal–insulator–metal gap plasmon resonators, each of which reflects the incident local electric field to a predesignated polarization angle. The simulation results show effective polarization conversion within a broad band from 700 to 930 nm.

Replacing noble metals with alternative materials in plasmonics and metamaterials: how good an idea?

Noble metals that currently dominate the fields of plasmonics and metamaterials suffer from large ohmic losses. Some of the new plasmonic materials, such as doped oxides and nitrides, have smaller material loss, and using them in place of metals carries the promise of reduced-loss plasmonic and metamaterial structures, with sharper resonances and higher field concentrations. This promise is put to a rigorous analytical test in this work, which reveals that having low material loss is not sufficient to have reduced modal loss in plasmonic structures. To reduce the modal loss, it is absolutely necessary for the plasma frequency to be significantly higher than the operational frequency. Using examples of nanoparticle plasmons and gap plasmons one comes to the conclusion that, even in the mid-infrared spectrum, metals continue to hold an advantage over alternative media when it comes to propagation distances and field enhancements. Of course, the new materials still have an application niche where high absorption loss is beneficial, e.g. in medicine and thermal photovoltaics.This article is part of the themed issue 'New horizons for nanophotonics'.

Coulomb Blockade Plasmonic Switch.

Tunnel resistance can be modulated with bias via the Coulomb blockade effect, which gives a highly nonlinear response current. Here we investigate the optical response of a metal-insulator-nanoparticle-insulator-metal structure and show switching of a plasmonic gap from insulator to conductor via Coulomb blockade. By introducing a sufficiently large charging energy in the tunnelling gap, the Coulomb blockade allows for a conductor (tunneling) to insulator (capacitor) transition. The tunnelling electrons can be delocalized over the nanocapacitor again when a high energy penalty is added with bias. We demonstrate that this has a huge impact on the plasmonic resonance of a 0.51 nm tunneling gap with ∼70% change in normalized optical loss. Because this structure has a tiny capacitance, there is potential to harness the effect for high-speed switching.

How Light Is Emitted by Plasmonic Metals.

The mechanism by which light is emitted from plasmonic metals such as gold and silver has been contentious, particularly at photon energies below direct interband transitions. Using nanoscale plasmonic cavities, blue-pumped light emission is found to directly track dark-field scattering on individual nanoconstructs. By exploiting slow atomic-scale restructuring of the nanocavity facets to spectrally tune the dominant gap plasmons, this correlation can be measured from 600 to 900 nm in gold, silver, and mixed constructs ranging from spherical to cube nanoparticles-on-mirror. We show that prompt electronic Raman scattering is responsible and confirm that "photoluminescence", which implies phase and energy relaxation, is not the right description. Our model suggests how to maximize light emission from metals.

Low-dimensional gap plasmons for enhanced light-graphene interactions

Graphene plasmonics has become a highlighted research area due to the outstanding properties of deep-subwavelength plasmon excitation, long relaxation time, and electro-optical tunability. Although the giant conductivity of a graphene layer enables the low-dimensional confinement of light, the atomic scale of the layer thickness is severely mismatched with optical mode sizes, which impedes the efficient tuning of graphene plasmon modes from the degraded light-graphene overlap. Inspired by gap plasmon modes in noble metals, here we propose low-dimensional hybrid graphene gap plasmon waves for large light-graphene overlap factor. We show that gap plasmon waves exhibit improved in-plane and out-of-plane field concentrations on graphene compared to those of edge or wire-like graphene plasmons. By adjusting the chemical property of the graphene layer, efficient and linear modulation of hybrid graphene gap plasmon modes is also achieved. Our results provide potential opportunities to low-dimensional graphene plasmonic devices with strong tunability.

Wide Field-of-view and Broadband Terahertz Beam Steering Based on Gap Plasmon Geodesic Antennas

Despite a plethora of applications ranging from wireless communications to sensing and spectroscopy, the current terahertz beam steering technologies suffer from tremendous insert loss, stringent control of electric bias, limited scanning angle, relatively complicated configuration and narrow operation bandwidth, preventing further practical application. We propose and demonstrate a conceptually new approach for terahertz beam steering by virtue of gap plasmon geodesic antennas. By adjusting the geometric dimension of the gap plasmon geodesic antennas, all gap plasmon modes add coherently along a peculiar direction that depends on the geodesic mean surface. Consequently, high directive beams are generated through the antenna, whose direction could be changed within a wide-angle range spanning ±45° by lateral motion of the feed. Furthermore, an assembled antenna structure consisting of four-element geodesic antennas array is proposed for full 360° beam steering, which can operate in a broadband range from 0.8 THz to 1.2 THz.

Imaging out-of-plane polarized emission patterns on gap mode SERS substrates: from high molecular coverage to the single molecule regime.

Gap mode surface-enhanced Raman scattering (SERS) substrates are created when a single nanoparticle is deposited on a thin metal film, creating a region of significant electromagnetic field enhancement in the gap between the nanoparticle and the film due to excitation of a vertically-oriented, out-of-plane dipole plasmon mode, e.g. the gap plasmon. When molecules are located in the gap and couple to the gap plasmon mode, the resulting emission is polarized perpendicular to the thin film, generating SERS emission patterns that have a characteristic donut shape. We analyze these SERS emission patterns using a dipole emission model and extract out-of-plane and in-plane emission angles associated with the gap plasmon mode. Fluctuations in both of these angles reveal dynamic heterogeneity due to molecular motion within the hot spot that changes as a function of molecular coverage. We also reveal static heterogeneity associated with structural defects in the thin film component of the gap mode substrates, indicating that even nanometer-scale surface roughness can impact the quality of gap mode emission.

Numerical Analysis on the Multilayer Nanoring Waveguide Pair

We propose a multilayer nanoring waveguide pair and investigate the surface plasmon modes and gap field enhancement between the two multilayer nanoring waveguides. Due to the strongly coupled electric fields between multilayer nanoring waveguides, a field enhancement contrast ratio over $10^{8}$ can be obtained. The mode refractive indices and the propagation lengths are analyzed by the commercial software COMSOL Multiphysics. We also demonstrate the influences of varied structure parameters on gap field enhancement. Moreover, graphene is replaced by gold in the multilayer nanoring waveguide pair to discuss the properties change. Thanks to the tunable surface conductivity, the gap field enhancement can be controlled by adjusting the chemical potentials of graphene. The application of multilayer nanoring waveguide pair may have a great prospect in photoelectric devices and bio-sensing.

Gap Plasmons Multiple Mirroring from Spheres in Pyramids for Surface-Enhanced Raman Scattering

A reliable fabrication technique for obtaining a high density of regular nanogaps is critical for ultrasensitive surface-enhanced Raman scattering (SERS). However, nanogaps produced between nanostructures have suffered from the lack of controllability. Taking the sphere–film structure as a starting point for its straightforward fabrication technique and well-controlled gaps, we propose a novel nanostructure by combining Au nanospheres and inverse pyramidal holes. The proposed nanostructure is obtained by trapping Au nanospheres in inverse pyramidal hole arrays to create multiple, uniform, and reproducible geometrical gaps near the contact points between the nanospheres and the inverse pyramids. The combined nanostructure, referred to as SIP (spheres in pyramids), supports augmented plasmon hybridization due to mirroring of gap plasmons and induces much stronger electromagnetic enhancement at normal incidence when compared to the contacting sphere–film structure. In contrast to the sphere–film structure ex...

Fluorescence Enhancement and Spectral Shaping of Silicon Quantum Dot Monolayer by Plasmonic Gap Resonances

A monolayer of silicon quantum dots (Si-QDs) 2.8 and 3.9 nm in diameter is placed in a gap between a gold (Au) thin film and a Au nanoparticle, and the photoluminescence (PL) properties are studied. By the metal nanoparticle over mirror (MNPoM) structure, the PL spectra of Si-QDs are strongly modified; the full width at half-maximum is reduced to ∼170 meV, which is less than half of that of Si-QDs on a silica substrate. The spectral shape coincides almost perfectly with that of the scattering spectrum of the MNPoM structure, indicating efficient coupling of the luminescence of Si-QDs with the gap surface plasmon modes. The luminescence intensity of Si-QDs in the gap is estimated to be enhanced about 700-fold compared to those on a Au film.

Electron energy-loss spectroscopy of branched gap plasmon resonators.

The miniaturization of integrated optical circuits below the diffraction limit for high-speed manipulation of information is one of the cornerstones in plasmonics research. By coupling to surface plasmons supported on nanostructured metallic surfaces, light can be confined to the nanoscale, enabling the potential interface to electronic circuits. In particular, gap surface plasmons propagating in an air gap sandwiched between metal layers have shown extraordinary mode confinement with significant propagation length. In this work, we unveil the optical properties of gap surface plasmons in silver nanoslot structures with widths of only 25 nm. We fabricate linear, branched and cross-shaped nanoslot waveguide components, which all support resonances due to interference of counter-propagating gap plasmons. By exploiting the superior spatial resolution of a scanning transmission electron microscope combined with electron energy-loss spectroscopy, we experimentally show the propagation, bending and splitting of slot gap plasmons.

Coherent perfect absorption mediated enhancement of transverse spin in a gap plasmon guide

We consider a symmetric gap plasmon guide (a folded Kretschmann configuration) supporting both symmeric and antisymmetric coupled surface plasmons. We calculate the transverse spin under illumination from both the sides like in coherent perfect absorption (CPA), whereby all the incident light can be absorbed to excite one of the modes of the structure. Significant enhancement in the transverse spin is shown to be possible when the CPA dip and the mode excitation are at the same frequency. The enhancement results from CPA-mediated total transfer of the incident light to either of the coupled modes and the associated large local fields. The transverse spin is localized in the structure since in the ambient dielectric there are only incident plane waves lacking any structure.