The Effect of Inserted Gold Nanosphere on the Second Harmonic Generation (SHG) Enhancement Factor of Three-Layered Dielectric-Gold Nanoshell

The tunable second harmonic generation (SHG) enhancement factor of gold-dielectric-gold three-layered nanoshells has been theoretically studied using the theory of quasi-static electrodynamics and plasmon hybridization. Because of the local surface plasmon resonance (LSPR)-induced local field effect, the SHG response corresponding to both fundamental frequency and second harmonic has been greatly enhanced. By changing the geometry parameters and local dielectric environment of the three-layered nanostructure, the intensity and shift of the SHG factor peaks could be fine tuned. As the radius of the inner gold sphere is increased, both the fundamental and the second harmonic SHG peaks from the anti-symmetric coupling between the outer bonding shell plasmon and the inner sphere plasmon decrease, whereas the SHG peaks from the symmetric coupling between the outer shell and the inner sphere get intense. These radius-dependent intensity changes of the SHG peaks also depend on the dielectric constant of the separate layer and outer surrounding. Thus, the number of SHG peak could be tuned from two to four. Furthermore, the wavelength gaps between the SHG peaks corresponding to anti-symmetric and symmetric coupling could be greatly reduced by increasing the thickness of the outer gold shell. Therefore, the nonmonotonous intensity change could be observed because of the switching of the SHG peaks. The corresponding physical origin has been illuminated by analyzing the plasmon hybridization and the polarization fields in the nanostructure.

     

Tuning the Dipolar Plasmon Hybridization of Multishell Metal-Dielectric Nanostructure: Gold Nanosphere in a Gold Nanoshell

Because of the interaction between dipole resonances of the inner gold sphere and the outer gold shell, gold-dielectric-gold multishells with sub-50 nm diameter may at most have three hybridization modes of surface plasmon resonance (SPR). Theoretical calculations based on quasi-static theory indicate that there are blending and splitting of SPR bands in the absorption spectra, which makes the number of absorption peak tunable by changing the radius of inserted gold sphere, thickness of gold shell, dielectric constant of middle dielectric shell or outer environment. The two absorption peaks at longer wavelength, which correspond to the hybridization from the bonding shell plasmon and the sphere plasmon, are usually intense and well tunable. The absorption peak at shorter wavelength, which corresponds to the symmetric coupling between the anti-bonding shell plasmon and the sphere plasmon, is relative weak and only occurs with large dielectric constant of the middle shell, small dielectric constant of the outer surrounding, large inner radius of the gold shell, and small radius of the inner gold sphere. Furthermore, the physical origin of these plasmon hybridizations in gold-dielectric-gold multishells nanostructure has also been illuminated by analyzing the local electric field distributions.     

Design and Research of Enhanced LED Performance Based on Graphical Substrate with Multilayer Hyperbolic Metamaterials

This paper mainly studies the influence of multilayer hyperbolic metamaterials (HMMs) with different structural parameters on the intensity of spontaneous radiation of quantum wells, thereby improving the coupling efficiency of incident electromagnetic waves and free electrons on metal nano-surfaces. In this paper, numerical simulations of visible light bands of 450–700 nm of Ag, Au, and Cu thin films are performed. The local field enhancements of multilayer HMMs with different shapes are compared, and it is found that circle Ag/Si multilayer HMMs have stronger field enhancement effects than other structures. At the same time, Purcell analysis was performed by changing various parameters of multilayer HMMs. It is found that the thickness of the metal/dielectric layer, the distance between the dipole and the HMMs, and the length of the multilayer HMMs change the intensity of the plasmon resonance radiation and have a great impact on the position of the resonance wavelength.

     

Obtain Quadruple Intense Plasmonic Resonances from Multilayered Gold Nanoshells by Silver Coating: Application in Multiplex Sensing

Four intense and separate localized surface plasmon resonance (LSPR) absorption peaks have been obtained in the gold-dielectric–gold–silver multilayer nanoshells. The silver coating on the gold shell results in a new LSPR peak at about 400 nm corresponding to the $ {{\left| {\omega_{+}^{-}} \right\rangle}_{Ag }} $ mode. The intense local electric field concentrated in the silver shell at the wavelength of 400 nm indicates that this new plasmonic band is coming from the symmetric coupling between the antibonding silver shell plasmon mode and the inner sphere plasmon. Increasing the silver shell thickness also leads to the intensity increasing of the $ {{\left| {\omega_{+}^{-}} \right\rangle}_{Au }} $ mode and blue shift of $ \left| {\omega_{-}^{+}} \right\rangle $ and $ \left| {\omega_{-}^{-}} \right\rangle $ modes. Therefore, quadruple intense plasmonic resonances in the visible region could be achieved in gold-dielectric–gold–silver multilayer nanoshells by tuning the geometrical parameters. And the quadruple intense plasmonic resonances in the visible region provide well potential for multiplex biosensing based on LSPR.     

A Computational Exploration of the Color Gamut of Nanoscale Hollow Scalene Ellipsoids of Ag and Au

Hollow, nanoscale, scalene ellipsoids of Ag or Au provide an exceedingly tunable localized surface plasmon resonance. Here, we use numerical simulations to determine the limits of the color space that would be possible from colloidal suspensions of these particles and show that their color gamut will exceed that possible with nanorods, nanoshells, or nanorice. The important parameters are composition, thickness of the shell, and shape of the particle, in that order. The sensitivity of colors to geometry is optimized for an aspect ratio of between 0.3 and 0.5 and was reduced for thinner shells. Shells of Ag will have much wider and more vibrant gamut than those of Au. These findings indicate that hollow scalene ellipsoids could be used as versatile pigments in materials or display systems that exploit plasmon resonance to produce color.     

The Study of Surface Plasmon Resonance in Au-Ag-Au Three-Layered Bimetallic Nanoshell: The Effect of Separate Ag Layer

Localized surface plasmon resonance (LSPR) properties of Au-Ag-Au three-layered nanoshell are investigated theoretically using the quasi-static electricity. Triple-bands LSPRs have been observed in the absorption spectrum. Both the peak wavelength and intensity could be fine tuned by altering the thickness and radius of the separate Ag layer. The properties and physical origin of the LSPR in the Au-Ag-Au three-layered nanoshell is much different from that of Au-dielectric-Au three-layered nanoshell. The corresponding physical mechanism has been illustrated by plotting the local electric field patterns and analyzing the interaction of the surface charges from different metal interfaces. Although the LSPR of Au-Ag-Au three-layered nanoshell is affected by the plasmon hybridization from all metal surfaces, it has been found that the plasmon coupling in different metallic layer takes main effect on the LSPR properties of different absorption peaks. These results indicate that the different type of metallic layers appearing alternately in the multilayered nanoshells could create abundant tunable LSPR modes, which provides potential for multiplex biosensing based on LSPR.     

The Effect of Negative Curvature on the Plasmonic Coupling of Concentric Core–Shell Metallic Nanostructures

Negative curvature-dependent localized surface plasmon resonance (LSPR) properties of concentric core–shell metallic nanostructure have been studied using quasistatic approach and plasmon hybridization theory. Whether in single-layered gold nanoshell or double gold nanoshells, the oscillating surface charges always concentrate close to the poles of the metal surface with negative curvature, which results in the anisotropic local electric field distribution and affects both the inter-surface plasmonic coupling and inter-shell plasmonic coupling. Therefore, the change of the radius of the gold surface with negative curvature could modulate the plasmon hybridization and lead to the LSPR shifting. The physical mechanism of the negative curvature-dependent LSPR presents a potential for design and fabrication of nanoscale optical device based on core–shell type metallic nanostructures.     

Frequency-Dependent Polarization Properties of Local Electric Field in Gold–Dielectric Multi-Nanoshells

The polarization properties of the local electric field in the gold–dielectric–gold multilayer nanoshells are investigated by theoretical calculation based on the quasi-static approximation. The calculation results show that the complete polarized incident light does not only stimulate the same directional polarized local electric field. The polarized angle of the local field may changes from 0° to 90° as the wavelength and location are changed. The distributions of local field polarization are different in dielectric layer or gold shell and display different features in different plasmonic hybridization mode. As the incident wavelength is increased, the hot spot of polarizing angle moves monotonously in the middle dielectric shell, whereas moves nonmonotonously in the gold shell and surrounding environment. In the gold shell, the gap between hot spots of polarizing angle may occur at the resonance frequency. However, the hot spots of polarizing angle always occur at the resonance frequencies in the surrounding environment. These interesting results show that the single-molecule detection based on metal nanostructure induced surface-enhanced Raman scattering and surface enhanced fluorescence could be optimized by adjusting the incident light polarization and frequency.     

Location-Dependent Local Field Enhancement Along the Surface of the Metal–Dielectric Core–Shell Nanostructure

A theoretical study based on quasi-static approximation is performed to investigate the location-dependent local field enhancement around the dielectric shell-coated gold nanosphere. Our calculation results show that the local field distribution near a gold nanoparticle can be altered greatly by coating with a dielectric shell. Because of the polarizability of the dielectric shell, increasing azimuth angle along the inner surface leads to the increase of the local field, which is opposite to that of the outer surface. Furthermore, the location-dependent local field enhancement and resonance frequency at both the inner and outer surfaces can also be modulated by varying the shell thickness and shell dielectric constant. These calculation results about the location-dependent local field enhancement show the potential of dielectric-coated metallic nanostructure for single-molecule detection based on surface-enhanced Raman scattering and surface enhanced fluorescence.     

Theoretical Studies of Tunable Localized Surface Plasmon Resonance of Gold-Dielectric Multilayered Nanoshells

Tunable properties of localized surface plasmon resonances (LSPR) of gold-dielectric multilayered nanoshells are studied by quasi-static theory and plasmon hybridization theory. Multilayered nanoshells with the gold core and nanoshell separated by a spacer layer exhibit strong coupling between the core and nanoshell plasmon resonance modes. It is found that the absorption spectra characteristics of LSPR are sensitive to multiple parameters including the surrounding medium refractive index, the dielectric constant of spacer layer, the radius of inner core gold sphere, outer shell layer thickness, and their coupling strength. The results show that LSPR is mainly influenced by the ratio of spacer layer dielectric constant ε ₂ to surrounding medium dielectric constant ε ₄. Absorption spectrum of \(\left |\omega _{-}^{+}\right \rangle \) mode is red-shifted with increasing core radius when ε ₂ > ε ₄. It is surprising to find that LSPR is blue-shifted with increasing core radius when ε ₂ < ε ₄, and no shift when ε ₂ = ε ₄. These interesting contrary shifts of \(\left |\omega _{-}^{+}\right \rangle \) mode with different ratios ε ₂/ε ₄ are well analysed with plasmon hybridization theory and the distributions of induced charges interaction between the inner core and outer shell. In addition, for the sake of clarity, the distributions of electric filed intensity at their plasmon resonance wavelengths are also calculated. This work may provide an alternative approach to analyse property of the core-shell nanoshell particles based on plasmon hybridization theory and the induced charge interaction.     

Tailoring LSPR-Based Absorption and Scattering Efficiencies of Semiconductor-Coated Au nanoshells

Absorption and scattering efficiencies of semiconductor-coated Au nanoshell have been studied by the extended Mie theory for their possible solar cell, optical imaging, and photothermal applications, etc. The effect of Au shell layer thickness, core size, and surrounding medium on the absorption and scattering efficiencies at the localized surface plasmon resonance (LSPR) wavelengths has been reported. It has been found that both the absorption and scattering efficiencies get blue-shifted with an increase in Au shell layer thickness from 2 to 10 nm and with an increase in surrounding refractive index whereas the corresponding LSPR peaks shift towards red. It has also been found that the spectra are red-shifted with an increase in the core radius from 20 to 40 nm while keeping the shell thickness same. The effect of shell thickness on the absorption peak position and absorption linewidth has also been studied. Hence, the optical response of both CdSe- and CdTe-coated Au nanoshells can be tuned and controlled from the visible to the near-infrared (NIR) region of the electromagnetic (EM) spectrum. Finally, the CdSe-coated Au nanoshell exhibits high scattering and absorption efficiencies in comparison to the CdTe-coated nanoshell.     

Surface Plasmon as a Probe of Local Field Enhancement

New method of experimental determination of local field enhancement at metal nanoparticles is suggested. It uses surface plasmon as a probe. Alternating-sign shift of surface plasmon resonance in copper nanoparticles incorporated in silica matrix has been observed under irradiation by intense femtosecond laser pulse. The red shift of plasmon observed during the action of pump pulse is interpreted as a result of change of dielectric constant of silica matrix due to optical Kerr effect in electric field of pump pulse enhanced in a vicinity of metal nanoparticles. The field enhancement factor is estimated from the value of the observed red shift of plasmon resonance.     

Metal-Dielectric-Graphene Hybrid Heterostructures with Enhanced Surface Plasmon Resonance Sensitivity Based on Amplitude and Phase Measurements

Metal-dielectric-graphene hybrid heterostructures based on oxides Al₂O₃, HfO₂, and ZrO₂ as well as on complementary metal–oxide–semiconductor compatible dielectric Si₃N₄ covering plasmonic metals Cu and Ag have been fabricated and studied. We show that the characteristics of these heterostructures are important for surface plasmon resonance biosensing (such as minimum reflectivity, sharp phase changes, resonance full width at half minimum and resonance sensitivity to refractive index unit (RIU) changes) can be significantly improved by adding dielectric/graphene layers. We demonstrate maximum plasmon resonance spectral sensitivity of more than 30,000 nm/RIU for Cu/Al₂O₃ (ZrO₂, Si₃N₄), Ag/Si₃N₄ bilayers and Cu/dielectric/graphene three-layers for near-infrared wavelengths. The sensitivities of the fabricated heterostructures were?~?5–8 times higher than those of bare Cu or Ag thin films. We also found that the width of the plasmon resonance reflectivity curves can be reduced by adding dielectric/graphene layers. An unexpected blueshift of the plasmon resonance spectral position was observed after covering noble metals with high-index dielectric/graphene heterostructures. We suggest that the observed blueshift and a large enhancement of surface plasmon resonance sensitivity in metal-dielectric-graphene hybrid heterostructures are produced by stationary surface dipoles which generate a strong electric field concentrated at the very thin top dielectric/graphene layer.

     

Localized Surface Plasmon Resonance and Refractive Index Sensitivity of Metal–Dielectric–Metal Multilayered Nanostructures

The localized surface plasmon resonances of multilayered nanostructures are studied using finite difference time domain simulations and plasmon hybridization method. Concentric metal–dielectric–metal (MDM) structure with metal core and nanoshell separated by a thin dielectric layer exhibits a strong coupling between the core and nanoshell plasmon resonance modes. The coupled resonance mode wavelengths show dependence on the dielectric layer thickness and composition of core and outer layer metal. The aluminum-based MDM structures show lower plasmon wavelength compared with Ag- and Au-based MDM nanostructures. The calculated refractive index sensitivity (RIS) factor is in the order Ag–Air–Ag>Au–Air–Au>Al–Air–Al for monometallic multilayered nanostructures. Bimetallic multilayered nanostructures support strong and tunable plasmon resonance wavelengths as well as high RIS factor of 510 nm/refractive index unit (RIU) and 470 nm/RIU for Al–Air–Au and Ag-Air-Au, respectively. The MDM structures not only exhibit higher index sensitivity but also cover a wide ultraviolet–near-infrared wavelengths, making these structures very promising for index sensing, biomolecule sensing, and surface-enhanced Raman spectroscopy.     

Tailoring Plasmon Lifetime in Suspended Nanoantenna Arrays for High-Performance Plasmon Sensing

We demonstrate significantly longer plasmon lifetime and stronger electric field enhancement by lifting the nanoantenna arrays above the substrate by dielectric nanopillars. The role of the pillar is to offer a more homogeneous dielectric background allowing stronger diffraction coupling among plasmonic nanoantennas leading to a Fanolike asymmetric lineshape. It is found that the electric fields around the nanoantennas can be greatly enhanced when the Fanolike resonance is excited, and a 4.2 times enhancement is achieved compared with the pure resonance in individual nanoantennas. Furthermore, only a collective surface mode with its electric fields of the same direction as the induced electric moment in the nanoantennas could mediate the excitation of such a Fanolike resonance. More importantly, the sensitivity and the figure of merit (FOM) of this plasmonic structure can reach as high as 900 nm/RIU and 53, respectively. Our study offers a new, simple, and efficient way to design the plasmonic systems with desired electric field enhancement and spectral lineshape for different applications.     

Near- and Far-Field Plasmonic Properties of Different Types of Eccentric Core-Shell Nanodimers

Finite element method (FEM) simulations have been carried out on free-standing and finite dielectric substrate-supported eccentric (i) silica core-gold nanoshell dimers and (ii) gold core-silica nanoshell dimers for understanding their near- and far-field plasmonic properties. In the case of eccentric silica core-gold nanoshell dimers, multiple peaks are observed in the near- and far-field spectra due to the plasmon hybridization. The number of peaks is found to be sensitive to the core offset parameters of the nanoshells forming nanodimer. The wavelength locations of the peaks due to the constructive coupling of the lower order modes found relatively more sensitive to the dielectric substrate. The number of peaks in the near- and far-field spectra found the same presence and absence of the dielectric substrate. The values of full width at half maximum (FWHM) of the peaks observed in the near-field spectra are found larger as compared to those observed in the far-field spectra. In contrast, in the case of eccentric gold core-silica nanoshell dimers, multiple peaks have not been observed. The FWHM of the observed peak is found sensitive to the core offset parameters of the nanoshells, and the number of peaks in the near field- and far-field spectra found not same in the presence and absence of the dielectric substrate. Moreover, the differences in near- and far-field spectra of plasmonically coupled (i) concentric nanoshells, (ii) eccentric nanoshells, and (iii) concentric and eccentric nanoshells also investigated numerically.

     

Subradiant,Superradiant Plasmon Modes and Fano Resonance in a Multilayer Nanocylinder Array Standing on a Thin Metal Film

The optical properties of a novel nanostructure consisting of a hexagonal array of aligned vertically three-layered metal-dielectric-metal nanodisks on a silver film are theoretically studied through the finite-difference time-domain method. The novel nanostructure exhibits three obvious optical transmission bands due to the excitation of subradiant plasmon modes, superradiant plasmon modes, and Fano resonances. Surface plasmon polaritons of the underlying Ag film also play a significant role on these three optical transmission bands via coupling with localized surface plasmons of nanodisk pairs. Moreover, the nanostructure also exhibits a good tunability of optical response by modifying the sizes of cylinders, the thickness of underlying metal film, and the dielectric constant of middle layer. These results demonstrate the nanostructure with great advantages in optical sensors and filters.

     

Effective Coupling of Incident Light Through an Air Region into an S-Shape Plasmonic Ag Nanowire Waveguide with Relatively Long Propagation Length

Coupling of incident light through an air region into an S-shape silver (Ag) plasmonic nanowire waveguide (SSAPNW) is a highly difficult challenge of light guiding on the surface of metal nanowire. In this paper, we numerically analyze the coupling effect of an SSAPNW which is covered by a dielectric medium using a finite element method. The coupling effect can be modulated by adjusting the Ag nanowire diameter and the covering dielectric medium width and wavelength of incident light, and the propagation length of surface plasmon (SP) coupling can be maximized. Simulation results reveal that the field confinement can be significantly improved and the majority of the electric field can be carried on the surface of a bending Ag nanowire. The effect of electric field transport along an SSAPNW due to SP coupling and Fabry-Perot resonance is investigated for different dimensions and lengths. Accordingly, long propagation lengths of about 41.5 μm for 10?×?SSAPNW at an incident wavelength of 810 nm and longer propagation length can be achieved if more sections of an SSAPNW are used. Simulation results offer an efficient method for optimizing SP coupling into bending metal nanowire waveguides and promote the realization of highly integrated plasmonic devices.     

Optical Absorption Modeling of Plasmonic Organic Solar Cells Embedding Silica-Coated Silver Nanospheres

We numerically study plasmonic solar cells in which a square periodic array of core–shell Ag@SiO₂ nanospheres (NSs) are placed on top of the indium tin oxide (ITO) layer using a 3D finite-difference time-domain (FDTD) method. We investigate the influence of various parameters such as the periodicity of the array, the Ag core diameter, the active layer thickness, the shell thickness, and the refractive index of the shell materials on the optical performance of the organic solar cells (OSC). Our results show that the optimal periodicity of the array of NSs is dependent on the size of Ag core NSs in order to maximize optical absorption in the active layer. A very thin active layer (<70 nm) and an ultrathin (<5 nm) SiO₂ shell are needed in order to obtain the highest optical absorption enhancement. Strong electric field localization is observed around the plasmonic core–shell nanoparticles as a result of localized surface plasmon resonance (LSPR) excited by Ag NSs with and without silica shell. Embedding 50 nm Ag NSs with 1-nm-thick SiO₂ shell thickness on top of ITO leads to an enhanced intrinsic optical absorption in a 40-nm-thick poly(3-hexylthiophene):phenyl-C₆₁-butyric acid methyl ester (P3HT:PCBM) active layer by 24.7% relative to that without the NSs. The use of 1-nm-thick ZnO shell instead of SiO₂ leads to an enhanced intrinsic absorption in a 40-nm-thick P3HT:PCBM active layer by 27%.

     

The Effect of Bumpy Structure on Optical Properties of Bimetallic Nanoshells

In this paper, a sensitive bumpy bimetallic nanoshell for detection of thyroid cancer market (Thyroglobulin, Tg) and bovine serum albumin (BSA) proteins is reported. The physical origin of plasmonic properties of bimetal nanoshells is described by plasmon hybridization theory which indicates three intense and clearly separated plasmon modes. The electric field intensity enhancement of the bumpy bimetal nanoshell increases by ~559 %, at the surface of the bump in comparison with a smooth shell. The presence of bumpy structure on the nanoshell surface provides a high enhancement of the resulting Raman signal through an electromagnetic field of the order of 10⁷ which leads to an increase in sensitivity detection of Tg and BSA proteins. In addition, a refractive index (RI) sensitivity of 332.54 nm/RIU is achieved for this bumpy bimetallic nanoshell.