Relations between near-field enhancements and Purcell factors in hybrid nanostructures of plasmonic antennas and dielectric cavities.

Strong near-field enhancements (NFEs) of nanophotonic structures are believed to be closely related to high Purcell factors (FP). Here, we theoretically show that the correlation is partially correct; the extinction cross section (σ) response is also critical in determining FP. The divergence between NFE and FP is especially pronounced in plasmonic-dielectric hybrid systems, where the plasmonic antenna supports dipolar plasmon modes and the dielectric cavity hosts Mie-like resonances. The cavity's enhanced-field environment can boost the antenna's NFEs, but the FP is not increased concurrently due to the larger effective σ that is intrinsic to the FP calculations. Interestingly, the peak FP for the coupled system can be predicted by using the NFE and σ responses. Furthermore, the limits for FP of coupled systems are considered; they are determined by the sum of the FP of a redshifted (or modified, if applicable) antenna and an individual cavity. This contrasts starkly with the behavior of NFE which is closely associated with the multiplicative effects of the NFEs provided by the antenna and the dielectric cavity. The differing behaviors of NFE and FP in hybrid cavities have varied impacts on relevant nanophotonic applications such as fluorescence, Raman scattering and enhanced light-matter interactions.

Turning whispering-gallery-mode responses through Fano interferences in coupled all-dielectric block-disk cavities.

Here, we theoretically demonstrate a strategy for efficiently turning whispering-gallery-mode (WGM) responses of a subwavelength dielectric disk through their near-field couplings with common low-order electromagnetic resonances of a dielectric block. Both simulations and an analytical coupled oscillator model show that the couplings are Fano interferences between dark high-quality WGMs and bright modes of the block. The responses of a WGM in the coupled system are highly dependent on the strengths and the relative phases of the block modes, the coupling strength, and the decay rate of the WGM. The WGM responses of coupled systems can exceed that of the individual disk. In addition, such a configuration will also facilitate the excitation of WGMs by a normal incident plane wave in experiments. These results could enable new applications for enhancing light-matter interactions.

Polarization-perceptual anisotropic two-dimensional ReS2 neuro-transistor with reconfigurable neuromorphic vision.

Polarization is a common and unique phenomenon in nature, which reveals more camouflage features of objects. However, current polarization-perceptual devices based on conventional physical architectures face enormous challenges for high-performance computation due to the traditional von Neumann bottleneck. In this work, a novel polarization-perceptual neuro-transistor with reconfigurable anisotropic vision is proposed based on a two-dimensional ReS2 phototransistor. The device exhibits excellent photodetection ability and superior polarization sensitivity due to its direct band gap semiconductor property and strong anisotropic crystal structure, respectively. The fascinating polarization-sensitive neuromorphic behavior, such as polarization memory consolidation and reconfigurable visual imaging, are successfully realized. In particular, the regulated polarization responsivity and dichroic ratio are successfully emulated through our artificial compound eyes. More importantly, two intriguing polarization-perceptual applications for polarized navigation with reconfigurable adaptive learning abilities and three-dimensional visual polarization imaging are also experimentally demonstrated. The proposed device may provide a promising opportunity for future polarization perception systems in intelligent humanoid robots and autonomous vehicles.

Strong couplings between magnetic quantum emitters and subwavelength all-dielectric resonators with whispering gallery modes.

Here we theoretically investigate the coherent interactions between the quantum emitters with magnetic dipole transitions and subwavelength all-dielectric resonators of whispering gallery modes (WGMs). We extend a semi-analytical method which can efficiently calculate the far-field spectrum of a general hybrid system. Then, a subwavelength sphere with refractive index around n = 3.5 is chosen as the dielectric resonator. Due to the high magnetic field enhancements of the WGMs of the sphere, strong couplings between magnetic quantum emitters and subwavelength WGMs can occur, where a clear Rabi splitting appears on the extinction spectrum of the hybrid system. The match between the relaxation times of the WGMs and emitters are important to efficiently achieve a strong enough coupling. The other parameters including the order of a WGM, the radius, the refractive index, the transition dipole moment and excitation intensity are also important factors that can affect the couplings. Our results pave the way for strong interactions between light and magnetic emitters mediated by subwavelength all-dielectric resonators.

Magnetic toroidal dipole response in individual all-dielectric nanodisk clusters.

Multipole electromagnetic resonances and their couplings are of crucial importance for both the fundamental understanding of light scattering by high-index all-dielectric nanostructures and lots of nanophotonic applications based on those nanostructures. Here, we show that magnetic dipole modes in a dielectric nanodisk cluster can easily form a magnetic toroidal dipole (MTD) mode. The cluster consists of five silicon nanodisks, where each nanodisk holds a magnetic dipole mode. These magnetic dipole modes can collectively couple with each other and form a MTD mode under suitable excitation. The MTD mode is confirmed by multipole expansion calculations and near field distributions, where two closed loops of magnetic field with opposite directions are seen. The response of the MTD is strong and comparable to that of a common electric dipole or magnetic dipole mode. It is also found that the MTD resonance is accompanied by an electric toroidal quadrupole mode in the cluster. The MTD mode is tunable by varying the geometries. We also fabricated silicon nanoparticle clusters and verified the MTD mode in the experiment. Our results illustrate the controllable excitation of strong high-order electromagnetic modes and these modes may open new opportunities for light manipulation at the nanoscale.

Controlled Synthesis of Au Nanocrystals-Metal Selenide Hybrid Nanostructures toward Plasmon-Enhanced Photoelectrochemical Energy Conversion.

A simple method for the controllable synthesis of Au nanocrystals-metal selenide hybrid nanostructures via amino acid guiding strategy is proposed. The results show that the symmetric overgrowth mode of PbSe shells on Au nanorods can be precisely manipulated by only adjusting the initial concentration of Pb2+. The shape of Au-PbSe hybrids can evolve from dumbbell-like to yolk-shell. Interestingly, the plasmonic absorption enhancement could be tuned by the symmetry of these hybrid nanostructures. This provides an effective pathway for maneuvering plasmon-induced energy transfer in metal-semiconductor hybrids. In addition, the photoactivities of Au-PbSe nanorods sensitized TiO2 electrodes have been further evaluated. Owing to the synergism between effective plasmonic enhancement effect and efficient interfacial charge transfer in these hybrid nanostructures, the Au-PbSe yolk-shell nanorods exhibit an outstanding photocurrent activity. Their photocurrent density is 4.38 times larger than that of Au-PbSe dumbbell-like nanorods under light irradiation at λ > 600 nm. As a versatile method, the proposed strategy can also be employed to synthesize other metal-selenide hybrid nanostructures (such as Au-CdSe, Au-Bi2Se3 and Au-CuSe).

Strategic modulation of energy transfer in Au-TiO2-Pt nanodumbbells: plasmon-enhanced hydrogen evolution reaction.

Owing to the capacity of efficiently harvesting and converting incident energy, localized surface-plasmon resonance of noble metals was introduced into a metal-semiconductor design for promoting hydrogen evolution. In this study, a plasmonic nanodumbbell structure was employed to strategically modulate the energy transfer in the water reduction reaction. A maximum H2 evolution rate of 80 µmol g-1 h-1 was obtained in the Au-TiO2 nanodumbbells, and further improvement was achieved through surface modification with Pt nanoparticles functioning as active sites, leading to ∼4.3 times enhanced photocatalytic activity. Compared with similar nanostructures reported previously, the present superior photoactivity response is ascribed to the injection process of the energetic hot electrons generated from the excitation and decay of the longitudinal surface-plasmon resonance (LSPR) and transverse surface-plasmon resonance (TSPR) in the Au nanorods, which corresponds to the electric field distribution of the finite-difference-time-domain simulation. These intriguing results, originating from the positive synergistic effect of the plasmon and co-catalyst, demonstrated the mechanism of the plasmon-assisted photochemistry and provided a promising strategy for the rational design of novel plasmonic photocatalysts.

Magnetic Plasmon-Enhanced Second-Harmonic Generation on Colloidal Gold Nanocups.

The magnetic plasmons of three-dimensional nanostructures have unique optical responses and special significance for optical nanoresonators and nanoantennas. In this study, we have successfully synthesized colloidal Au and AuAg nanocups with a well-controlled asymmetric geometry, tunable opening sizes, and normalized depths ( h/ b, where h is depth and b is the height of the templating PbS nanooctahedrons), variable magnetic plasmon resonance, and largely enhanced second-harmonic generation (SHG). The most-efficient SHG of the bare Au nanocups is experimentally observed when the normalized depth h/ b is adjusted to ∼0.78-0.79. We find that the average magnetic field enhancement is maximized at h/ b = ∼0.65 and reveal that the maximal SHG can be attributed to the joint action of the optimized magnetic plasmon resonance and the "lightning-rod effect" of the Au nanocups. Furthermore, we demonstrate for the first time that the AuAg heteronanocups prepared by overgrowth of Ag on the Au nanocups can synergize the magnetic and electric plasmon resonances for nonlinear enhancement. By the tailoring of the dual resonances at the fundamental excitation and second-harmonic wavelengths, the far-field SHG intensity of the AuAg nanocups is enhanced 21.8-fold compared to that of the bare Au nanocups. These findings provide a strategy for the design of nonlinear optical nanoantennas based on magnetic plasmon resonances and can lead to diverse applications ranging from nanophotonics to biological spectroscopy.

Efficient second harmonic generation in gold-silicon core-shell nanostructures.

We theoretically investigate the properties of second-harmonic generation (SHG) in gold-silicon core-shell nanostructures. We first study a concentric structure. This structure exhibits strong electric field enhancement in the silicon shell due to the combined toroidal dipole mode and electric dipole mode. Efficient SHG can be obtained and the SHG signal is about 5 times as strong as that of the individual Si shell. Further calculations show that the contribution from a surface nonlinear susceptibility at the inner surface of the silicon shell dominates the SHG signal of the core-shell structure. The SHG as a function of wavelength is considered and it shows a resonance behavior. The cases of nonconcentric core-shell structures have also been considered. The SHG is further enhanced in this kind of configuration and the SHG signal can reach about 10 times as strong as that of the concentric case. Our results reveal the strong modification of the SHGs in dielectric nanostructures by using the metal-dielectric hybrid configurations, and could find applications in nanoscale nonlinear devices.

Abnormal nonlinear optical properties of hybrid graphene-TiO2 nanostructures.

The nonlinear optical (NLO) properties of graphene-TiO2 nanoparticle (GNP) composite and graphene-TiO2 nanowire composite (GNW) are investigated by spatial self-phase modulation (SSPM) and Z-scan. The SSPM results of the GNP and GNW show that they possess strong self-diffraction effects at 1100 nm and no signal at 700 nm, which is different from all previous reports of other two-dimensional materials. A possible mechanism is that NLO behaviors are dominated by TiO2 at the visible wavelength, while by graphene at a near-infrared wavelength. The Z-scan results of the GNP and GNW show reverse saturable absorption (RSA) at 700 nm, but saturable absorption (SA) at 1100 nm. Our results demonstrate that, by choosing appropriate coupling, we could design two-dimensional materials that have specific NLO properties at particular wavelengths.

Plasmonic nanoantenna-dielectric nanocavity hybrids for ultrahigh local electric field enhancement.

A dielectric nanostructure with a high refractive index can exhibit strong optical resonances with considerable electric field enhancement around the entire structure volume. Here we show theoretically that a dielectric structure with this feature can boost the local electric field of a small plasmonic nanoantenna placed nearby. We construct a hybrid system of a plasmonic nanoantenna and a dielectric nanocavity, where the nanocavity is a concentric disk-ring structure with a lossless material n = 3.3 and the nanoantenna is a gold nanorod dimer. The resonant electric field enhancement at the gap center of the antenna in the hybrid structure reaches more than one order of magnitude higher than that of the individual antenna. The dielectric structure plays two roles in the hybrid system, namely the amplified excitation field and an environment causing the redshift of the antenna resonance. The hybrid configuration is applicable to the cases with various geometries and different materials of the hybrid system. Our results can find applications in enhanced nanoscale light-matter interactions such as surface-enhanced Raman scattering, nonlinear optics, and plasmon-exciton couplings.

Boosting magnetic field enhancement with radiative couplings of magnetic modes in dielectric nanostructures.

Dielectric nanostructures can readily support considerable magnetic field enhancements that offer great potential applications in field enhanced spectroscopies. However, the magnetic fields of dielectric structures are usually distributed within the entire volume, which brings challenge to the further increment of the magnetic field enhancement. Here, we theoretically demonstrate that the magnetic field enhancement in dielectric nanostructures can be boosted through the radiative couplings of magnetic modes. Our concentric structure consists of a hollow disk and a ring. The disk has a magnetic dipole mode. The ring has two magnetic dipole modes that are out of phase. Strong radiative interactions between the modes on the disk and the ring can occur, which result in a net constructive coupling effect. For a lossless material with n = 3.3, a sharp peak can be obtained on the scattering spectrum of the coupled system due to the radiative interactions. The corresponding resonant magnetic field enhancement at the disk center reaches 96 times. This enhancement is about 7 times higher than that of an individual disk. The structure with a lossy material Si is also considered, where radiative couplings and boosted magnetic field can also be obtained. Our research reveals the strong radiative mode couplings in dielectric structures and is important for furthering our understanding on the light-matter interactions at the nanoscale.

Magnetic Fano resonance-induced second-harmonic generation enhancement in plasmonic metamolecule rings.

The "artificial magnetic" resonance in plasmonic metamolecules extends the potential application of magnetic resonance from terahertz to optical frequency bypassing the problem of magnetic response saturation by replacing the conduction current with the ring displacement current. So far, the magnetic Fano resonance-induced nonlinearity enhancement in plasmonic metamolecule rings has not been reported. Here, we use the magnetic Fano resonance to enhance second-harmonic generation (SHG) in plasmonic metamolecule rings. In the spectra of the plasmonic metamolecule, an obvious Fano dip appears in the scattering cross section, while the dip does not appear in the absorption cross section. It indicates that at the Fano dip the radiative losses are suppressed, while the optical absorption efficiency is at a high level. The largely enhanced SHG signal is observed as the excitation wavelength is adjusted at the magnetic Fano dip of the plasmonic metamolecule rings with stable and tunable magnetic responses. We also compare the magnetic Fano dip with the electric case to show its advantages in enhancing the fundamental and second harmonic responses. Our research provides a new thought for enhancing optical nonlinear processes by magnetic modes.

Role of material loss and mode volume of plasmonic nanocavities for strong plasmon-exciton interactions.

We investigate the role of material loss and mode volume of plasmonic nanostructures on strong plasmon-exciton coupling. We find that the field enhancement, and therefore loss, is not important for the magnitude of the Rabi splitting as such, but instead it is determined by the mode volume. Nevertheless, for reaching true strong coupling condition, that is, coupling greater than any dissipation, it is important to compromise losses. We also show that using such popular geometries as a dimer of two spheres or bow-tie nanoantennas, does not allow compressing the mode volume much in comparison to a single nanoparticle case, except for very narrow gaps, but rather it allows for efficient extraction of the mode out of the metal thus making it more accessible for excitons to interact with. Even more efficient mode extraction is achieved when high refractive index dielectric is placed in the gap. Our findings may find practical use for quantum plasmonics applications.

Gold Nanorod Rotary Motors Driven by Resonant Light Scattering.

Efficient and robust artificial nanomotors could provide a variety of exciting possibilities for applications in physics, biology and chemistry, including nanoelectromechanical systems, biochemical sensing, and drug delivery. However, the application of current man-made nanomotors is limited by their sophisticated fabrication techniques, low mechanical output power and severe environmental requirements, making their performance far below that of natural biomotors. Here we show that single-crystal gold nanorods can be rotated extremely fast in aqueous solutions through optical torques dominated by plasmonic resonant scattering of circularly polarized laser light with power as low as a few mW. The nanorods are trapped in 2D against a glass surface, and their rotational dynamics is highly dependent on their surface plasmon resonance properties. They can be kept continuously rotating for hours with limited photothermal side effects and they can be applied for detection of molecular binding with high sensitivity. Because of their biocompatibility, mechanical and thermal stability, and record rotation speeds reaching up to 42 kHz (2.5 million revolutions per minute), these rotary nanomotors could advance technologies to meet a wide range of future nanomechanical and biomedical needs in fields such as nanorobotics, nanosurgery, DNA manipulation and nano/microfluidic flow control.

Ultimate Limit of Light Extinction by Nanophotonic Structures.

Nanophotonic structures make it possible to precisely engineer the optical response at deep subwavelength scales. However, a fundamental understanding of the general performance limits remains a challenge. Here we use extensive electrodynamics simulations to demonstrate that the so-called f-sum rule sets a strict upper bound to the light extinction by nanostructures regardless their internal interactions and retardation effects. In particular, we show that the f-sum rule applies to arbitrarily complex plasmonic metal structures that exhibit an extraordinary spectral sensitivity to size, shape, near-field coupling effects, and incident polarization. The results may be used for benchmarking light scattering and absorption efficiencies, thus imposing fundamental limits on solar light harvesting, biomedical photonics, and optical communications.

Plasmon Enhanced Internal Photoemission in Antenna-Spacer-Mirror Based Au/TiO2 Nanostructures.

Emission of photoexcited hot electrons from plasmonic metal nanostructures to semiconductors is key to a number of proposed nanophotonics technologies for solar harvesting, water splitting, photocatalysis, and a variety of optical sensing and photodetector applications. Favorable materials and catalytic properties make systems based on gold and TiO2 particularly interesting, but the internal photoemission efficiency for visible light is low because of the wide bandgap of the semiconductor. We investigated the incident photon-to-electron conversion efficiency of thin TiO2 films decorated with Au nanodisk antennas in an electrochemical circuit and found that incorporation of a Au mirror beneath the semiconductor amplified the photoresponse for light with wavelength λ = 500-950 nm by a factor 2-10 compared to identical structures lacking the mirror component. Classical electrodynamics simulations showed that the enhancement effect is caused by a favorable interplay between localized surface plasmon excitations and cavity modes that together amplify the light absorption in the Au/TiO2 interface. The experimentally determined internal quantum efficiency for hot electron transfer decreases monotonically with wavelength, similar to the probability for interband excitations with energy higher than the Schottky barrier obtained from a density functional theory band structure simulation of a thin Au/TiO2 slab.

Dimer-on-mirror SERS substrates with attogram sensitivity fabricated by colloidal lithography.

Nanoplasmonic substrates with optimized field-enhancement properties are a key component in the continued development of surface-enhanced Raman scattering (SERS) molecular analysis but are challenging to produce inexpensively in large scale. We used a facile and cost-effective bottom-up technique, colloidal hole-mask lithography, to produce macroscopic dimer-on-mirror gold nanostructures. The optimized structures exhibit excellent SERS performance, as exemplified by detection of 2.5 and 50 attograms of BPE, a common SERS probe, using Raman microscopy and a simple handheld device, respectively. The corresponding Raman enhancement factor is of the order 10(11), which compares favourably to previously reported record performance values.

Manipulating nonlinear emission and cooperative effect of CdSe/ZnS quantum dots by coupling to a silver nanorod complex cavity.

Colloidal semiconductor quantum dots have three-dimensional confined excitons with large optical oscillator strength and gain. The surface plasmons of metallic nanostructures offer an efficient tool to enhance exciton-exciton coupling and excitation energy transfer at appropriate geometric arrangement. Here, we report plasmon-mediated cooperative emissions of approximately one monolayer of ensemble CdSe/ZnS quantum dots coupled with silver nanorod complex cavities at room temperature. Power-dependent spectral shifting, narrowing, modulation, and amplification are demonstrated by adjusting longitudinal surface plasmon resonance of silver nanorods, reflectivity and phase shift of silver nanostructured film, and mode spacing of the complex cavity. The underlying physical mechanism of the nonlinear excitation energy transfer and nonlinear emissions are further investigated and discussed by using time-resolved photoluminescence and finite-difference time-domain numerical simulations. Our results suggest effective strategies to design active plasmonic complex cavities for cooperative emission nanodevices based on semiconductor quantum dots.

Plasmonic Fano resonances in metallic nanorod complexes.

Plasmonic Fano resonances (FRs) in nanostructures have been extensively studied in recent years. Nanorod-based complexes for FRs have also attracted much attention. The basic optical properties and fabrication technology of different kinds of plasmonic nanorods have been greatly developed over the last several years. The mutipole plasmon resonances and their flexible adjustment ranges on nanorods make them promising for FR modifications and structure diversity. In this paper, we review some recently studied plasmonic nanorod based nanostructures for FRs, including single nanorods, dimers, mutipole rods and nanorod-nanoparticle hybrids. The corresponding applications of the FRs are also briefly discussed.