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We investigated hybrid functional transparent conductive electrodes (HFTCEs) composed of indium-tin-oxide (ITO) and silver nanowires (AgNWs) for the enhancement of output efficiency in GaN-based ultraviolet light-emitting diodes (UVLEDs). The HFTCEs demonstrated an optical transmittance of 69.5% at a wavelength of 380 nm and a sheet resistance of 16.4 Ω/sq, while the reference ITO TCE exhibited a transmittance of 76.4% and a sheet resistance of 18.7 Ω/sq. Despite the 8.9% lower optical transmittance, the UVLEDs fabricated with HFTCEs achieved a 25% increase in output efficiency compared to reference UVLEDs. This improvement is attributed to the HFTCE's twofold longer current spreading length under operating forward voltages, and more significantly, the enhanced out-coupling of localized surface plasmon (LSP) resonance with the trapped wave-guided light modes.

Plasmonic excitations decay within femtoseconds, leaving nonthermal (often referred to as "hot") charge carriers behind that can be injected into molecular structures to trigger chemical reactions that are otherwise out of reach─a process known as plasmonic catalysis. In this Letter, we demonstrate that strong coupling between resonator structures and plasmonic nanoparticles can be used to control the spectral overlap between the plasmonic excitation energy and the charge injection energy into nearby molecules. Our atomistic description couples real-time density-functional theory self-consistently to an electromagnetic resonator structure via the radiation-reaction potential. Control over the resonator provides then an additional knob for nonintrusively enhancing plasmonic catalysis, here more than 6-fold, and dynamically reacting to deterioration of the catalyst─a new facet of modern catalysis.

We have demonstrated localized surface plasmon (LSP)-enhanced cathodoluminescence (CL) from an atomic layer deposition (ALD)-grown Al2O3/ZnO/Al2O3 heterostructure to develop a bright nanometer-scale light source for an electron beam excitation-assisted (EXA) optical microscope. Three types of metals, Ag, Al, and Au, were compared, and an 181-fold enhancement of CL emission was achieved with Ag nanoparticles (NPs), with the plasmon resonance wavelength close to the emission wavelength energy of ZnO. The enhanced emission is plausibly attributed to LSP/exciton coupling. However, it is also attributed to an increase in coupling efficiency with penetration depth and also to an increase in light extraction efficiency by grading the refractive indices at the heterostructure., (© The Author(s) 2024. Published by Oxford University Press on behalf of The Japanese Society of Microscopy. All rights reserved. For commercial re-use, please contact reprints@oup.com for reprints and translation rights for reprints. All other permissions can be obtained through our RightsLink service via the Permissions link on the article page on our site–for further information please contact journals.permissions@oup.com.)

Plasmon photocatalysis reactions are thought to occur through vibrationally activated reactants, driven by nonthermal energy transfer from plasmon-induced hot carriers. However, a detailed quantum-state-level understanding and quantification of the activation have been lacking. Using anti-Stokes surface-enhanced Raman scattering (SERS) spectroscopy, we mapped the vibrational population distributions of reactants on plasmon-excited nanostructures. Our results reveal a highly nonthermal distribution with an anomalously enhanced population of multiquantum excited states  ( v ≥ 2). The shape of the distribution and its dependence on local field intensity and excitation wavelength cannot be explained by photothermal heating or vibronic optical transitions of the metal-molecule complex. Instead, it can be modeled by hot electron-molecule energy transfer mediated by the transient negative ions, establishing direct links among nonthermal reactant activation, plasmon-induced hot electrons, and negative ion resonances. Moreover, the presence of multiquantum excited reactants, which are far more reactive than those in the ground state or first excited state, presents opportunities for vibrationally controlling chemical selectivities.

As the driving source, highly efficient silicon-based light emission is urgently needed for the realization of optoelectronic integrated chips. Here, we report that enhanced green electroluminescence (EL) can be obtained from oxygen-doped silicon nitride (SiN x :O) films based on an ordered and tunable Ag nanocavity array with a high density by nanosphere lithography and laser irradiation. Compared with that of a pure SiN x O device, the green electroluminescence (EL) from the SiN x :O/Ag nanocavity array device can be increased by 7.1-fold. Moreover, the external quantum efficiency of the green electroluminescence (EL) is enhanced 3-fold for SiN x :O/Ag nanocavity arrays with diameters of 300 nm. The analysis of absorption spectra and the FDTD calculation reveal that the localized surface plasmon (LSP) resonance of size-controllable Ag nanocavity arrays and SiN x :O films play a key role in the strong green EL. Our discovery demonstrates that SiN x :O films coupled with tunable Ag nanocavity arrays are promising for silicon-based light-emitting diode devices of the AI period in the future.

Ultracompact chiral plasmonic nanostructures with unique chiral light-matter interactions are vital for future photonic technologies. However, previous studies are limited to reporting their steady-state performance, presenting a fundamental obstacle to the development of high-speed optical devices with polarization sensitivity. Here, a comprehensive analysis of ultrafast chiroptical response of chiral gold nano-oligomers using time-resolved polarimetric measurements is provided. Significant differences are observed in terms of the absorption intensity, thus hot electron generation, and hot carrier decay time upon polarized photopumping, which are explained by a phenomenological model of the helicity-resolved optical transitions. Moreover, the chiroptical signal is switchable by reversing the direction of the pump pulse, demonstrating the versatile modulation of polarization selection in a single device. The results offer fundamental insights into the helicity-resolved optical transitions in photoexcited chiral plasmonics and can facilitate the development of high-speed polarization-sensitive flat optics with potential applications in nanophotonics and quantum optics., (© 2023 Wiley-VCH GmbH.)

Optical nanoantennas possess broad applications in the fields of photodetection, environmental science, biosensing and nonlinear optics, owing to their remarkable ability to enhance and confine the optical field at the nanoscale. In this article, we present a theoretical investigation of surface-enhanced photoluminescence spectroscopy for single molecules confined within novel Au bowtie nanoantenna, covering a wavelength range from the visible to near-infrared spectral regions. We employ the finite element method to quantitatively study the optical enhancement properties of the plasmonic field, quantum yield, Raman scattering and fluorescence. Additionally, we systematically examine the contribution of nonlocal dielectric response in the gap mode to the quantum yield, aiming to gain a better understanding of the fluorescence enhancement mechanism. Our results demonstrate that altering the configuration of the nanoantenna has a significant impact on plasmonic sensitivity. The nonlocal dielectric response plays a crucial role in reducing the quantum yield and corresponding fluorescence intensity when the gap distance is less than 3 nm. However, a substantial excitation field can effectively overcome fluorescence quenching and enhance the fluorescence intensity. By optimizing nanoantenna configuration, the maximum enhancement of surface-enhanced Raman can be turned to 9 and 10 magnitude orders in the visible and near-infrared regions, and 3 and 4 magnitude orders for fluorescence enhancement, respectively. The maximum spatial resolutions of 0.8 nm and 1.5 nm for Raman and fluorescence are also achieved, respectively. Our calculated results not only provide theoretical guidance for the design and application of new nanoantennas, but also contribute to expanding the range of surface-enhanced Raman and fluorescence technology from the visible to the near-infrared region., (© 2024 IOP Publishing Ltd.)

As a promising way to reduce the temperature for conventional thermolysis, plasmon-induced photocatalysis has been utilized for the dehydrogenation of methane. Here we probe the microscopic dynamic mechanism for plasmon-induced methane dissociation over a tetrahedral Ag 20 nanoparticle with molecular orbital insights using time-dependent density functional theory. We ingeniously built the relationship between the chemical bonds and molecular orbitals via Hellmann-Feynman forces. The time- and energy-resolved photocarrier analysis shows that the indirect hot hole transfer from the Ag nanoparticle to methane dominates the photoreaction at low laser intensity, due to the strong hybridization of the Ag nanoparticle and CH 4 orbitals, while indirect and direct charge transfer coexist to facilitate methane dissociation in intense laser fields. Our findings can be used to design novel methane photocatalysts and highlight the broad prospects of the molecular orbital approach for adsorbate-substrate systems.

Surface Plasmonic Resonance (SPR) induced by metallic nanoparticles can be exploited to enhance the response of photodetectors (PD) to a large degree. Since the interface between metallic nanoparticles and semiconductors plays an important role in SPR, the magnitude of the enhancement is highly dependent on the morphology and roughness of the surface where the nanoparticles are distributed. In this work, we used mechanical polishing to produce different surface roughnesses for the ZnO film. Then, we exploited sputtering to fabricate Al nanoparticles on the ZnO film. The size and spacing of the Al nanoparticles were adjusted by sputtering power and time. Finally, we made a comparison among the PD with surface processing only, the Al-nanoparticles-enhanced PD, and the Al-nanoparticles-enhanced PD with surface processing. The results showed that increasing the surface roughness could enhance the photo response due to the augmentation of light scattering. More interestingly, the SPR induced by the Al nanoparticles could be strengthened by increasing the roughness. The responsivity could be enlarged by three orders of magnitude after we introduced surface roughness to boost the SPR. This work revealed the mechanism behind how surface roughness influences SPR enhancement. This provides new means for improving the photo responses of SPR-enhanced photodetectors.

Surface plasmons have robust and strong confinement to the light field which is beneficial for the light-matter interaction. Surface plasmon amplification by stimulated emission of radiation (SPACER) has the potential to be integrated on the semiconductor chip as a compact coherent light source, which can play an important role in further extension of Moore's law. In this study, we demonstrate the localized surface plasmon lasing at room temperature in the communication band using metallic nanoholes as the plasmonic nanocavity and InP nanowires as the gain medium. Optimizing laser performance has been demonstrated by coupling between two metallic nanoholes which adds another degree of freedom for manipulating the lasing properties. Our plasmonic nanolasers exhibit lower power consumption, smaller mode volumes, and higher spontaneous emission coupling factors due to enhanced light-matter interactions, which are very promising in the applications of high-density sensing and photonic integrated circuits.

In this article, we propose a simple method to calculate electrical permittivity and refractive index of surface agents of gold nanoparticles (Au NPs), in which it is possible to find the refractive index of surface agents shell by using the absorption peak of the gold nano-colloid. One of the usual tests for detection of surface agents is colorimetric methods based on the change of color of Au NPs. The color change is mainly due to the shift of localized surface plasmon resonance which is related to electrical interactions of surface agents. Although there are many mathematical models for simulating the absorption spectrum and calculating the plasmonic peak, using them is not simple and possible for everyone due to the need for programming. Here, the necessary simulations have been performed for different values ​​of refractive index of surface agents and particle size, and absorption peaks have been obtained. Using numerical methods, a simple formula is obtained between the wavelength of plasmonic peak, the ratio of hydrodynamic diameter to Feret size of the particles, and the refractive index of the surface agents. This method can help researchers to obtain the refractive index and consequently the type or concentration of surface agents around Au NPs without the need for programming or complex mathematical operations. It can also open new horizons in analyzing colorimetric diagnosis of biological agents such as viral antibodies, antigens, and other biological agents., Competing Interests: Conflict of InterestThe authors declare no competing interests., (© The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature 2023, Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.)

We report on a self-referenced refractive index optical sensor based on Au nanoislands. The device consists of a random distribution of Au nanoislands formed by dewetting on a planar SiO 2 /metal Fabry-Pérot cavity. Experimental and theoretical studies of the reflectance of this configuration reveal that its spectral response results from a combination of two resonances: a localized surface plasmon resonance (LSPR) associated to the Au nanoislands and the lowest-order anti-symmetric resonance of the Fabry-Pérot cavity. When the device is immersed in different fluids, the LSPR contribution provides high sensitivity to refractive index variations of the fluid, whereas those refractive index changes have little impact on the Fabry-Pérot resonance wavelength, allowing its use as a reference signal. The self-referenced sensor exhibits a spectral sensitivity of 212 nm/RIU (RIU: refractive index unit), which is larger than those of similar structures, and an intensity sensitivity of 4.9 RIU -1 . The proposed chip-based architecture and the low cost and simplicity of the Au nanoisland synthesis procedure make the demonstrated sensor a promising self-referenced plasmonic sensor for compact biosensing optical platforms based on reflection mode operation.

NH- μ LED, namely a micro light-emitting diode structure with nano-holes dug all the way through the active region, is designed to make silver nanoparticles in extremely close contact with the quantum wells for improving the coupling between the localized surface plasmon and the quantum wells (LSP-QWs coupling) and thus enhancing the optical properties of the μ LED. The experimental results show that, thanks to this deep nanohole structure, the LSP-QWs coupling can be realized effectively, which ultimately increases the optical performance of the μ LED. The internal quantum efficiency of the NH- μ LED filled with silver nanoparticles is increased by 12%, and the final optical output power is also enhanced. We have further carried out a comparison study which measures the transient lifetime of two different types of μ LEDs, and the results provide convincing evidence for the existence of the ultra close range LSP-QWs coupling effect., (© 2022 IOP Publishing Ltd.)

Infrared detection technology has been widely applied in many areas. Unlike internal photoemission and the photoelectric mechanism, which are limited by the interface barrier height and material bandgap, the research of the hot carrier effect from nanometer thickness of metal could surpass the capability of silicon-based Schottky devices to detect mid-infrared and even far-infrared. In this work, we investigate the effects of physical characteristics of Cr nanometal surfaces and metal/silicon interfaces on hot carrier optical detection. Based on the results of scanning electron microscopy, atomic force microscopy, and X-ray diffraction analysis, the hot carrier effect and the variation of optical response intensity are found to depend highly on the physical properties of metal surfaces, such as surface coverage, metal thickness, and internal stress. Since the contact layer formed by Cr and Si is the main role of infrared light detection in the experiment, the higher the metal coverage, the higher the optical response. Additionally, a thicker metal surface makes the hot carriers take a longer time to convert into current signals after generation, leading to signal degradation due to the short lifetime of the hot carriers. Furthermore, the film with the best hot carrier effect induced in the Cr/Si structure is able to detect an infrared signal up to 4.2 μm. Additionally, it has a 229 times improvement in the signal-to-noise ratio (SNR) for a single band compared with ones with less favorable conditions.

Using the finite-difference time-domain (FDTD) method, we designed an ultra-thin Ge/GaAs/P3HT:PCBM hybrid solar cell (HSC), which showed good effects of ultra-wideband (300 nm-1200 nm), high absorption, and a short-circuit current density of 44.7 mA/cm 2 . By changing the thickness of the active layer P3HT:PCBM, we analyzed the capture of electron-hole pairs. We also studied the effect of Al 2 O 3 on the absorption performance of the cell. Through adding metal Al nanoparticles (Al-NPs) and then analyzing the figures of absorption and electric field intensity, we found that surface plasma is the main cause of solar cell absorption enhancement, and we explain the mechanism. The results show that the broadband absorption of the solar cell is high, and it plays a great role in capturing sunlight, which will be of great significance in the field of solar cell research.

Harvesting solar energy for water treatments has been considered a promising solution for a global community. The shortage of water is a great challenge for scientists due to the increased demand of the population-however, the low efficiency of absorber materials obstacles in practical applications. In addition, state-of-the-art conventional technologies require optical concentrators and multiple component-based systems, leading to lower efficiency and higher cost. In this review, a low-cost, more reliable, less energy-intensive, and more eco-friendly solar water purification system based on graphene-plasmonic hybrid nanocomposite has been demonstrated. Graphene-plasmonic-based hybrid nanocomposite has been utilized to achieve pure water from wastewater. Such hybrid nanocomposites have the ability to clean polluted water very efficiently due to their excellent properties such as higher surface area, low concentration, and working ability. Furthermore, the development of a solar water purification system has been achieved through optimized hybrid nanocomposites., (Copyright© Bentham Science Publishers; For any queries, please email at epub@benthamscience.net.)

Localized surface plasmon (LSP) coupling with many radiators are investigated. The LSP is generated by excitation of laser or electron beam on the random Ag nano particles (NPs) and arrayed ones embedded in the p-GaN of green LEDs. They couple with the excitons or radiative recombination in the quantum well (QW) and electron beam, which enhance or suppress the luminescence of the radiators. The photoluminescence (PL) intensity of periodic Ag NPs can get as much as 4.5 times higher than that of bare LED. In addition to the periodic structure, the morphology of Ag NPs also affects the localized SP (LSP) resonance intensity and light scattering efficiency. In the finite difference time domain (FDTD) simulation, five x-polarized dipoles are approximated to five quantum wells. Considering the interaction between the five dipoles and their feedback effect on LSP, the enhancement effect of SP dipole coupling with Ag NPs is amplified and the energy dissipation is reduced. The enhancement of cathodoluminescence (CL) was also found in green LEDs with Ag NPs. The three-body model composed of two orthogonal dipoles and an Ag NP is used for 3D FDTD simulation. The LSP-QWs coupling effect is separated from the electron beam (e-beam)-LSP-QW system by linear approximation. Under the excitation of electron beam, the introduction of z-dipole greatly reduces the energy dissipation. In the cross-sectional sample, z-polarized dipoles in QWs show more coupling strength to the dipole and quadrupole modes of LSP. The perturbation theory is used to separate the LSP coupling effects to x-dipole and z-dipole. At last, the resonator and the antenna effects are discussed for LSP coupling at different positions to the Ag NP.

The theoretical research on surface enhanced Raman spectroscopy (SERS) of triangular plate dimer (TPD) is of great significance for the design of experimental substrates. In this paper, the SERS properties of the TPD with Au, Ag, Al and Cu have been theoretical investigated in the ultra-ultraviolet, visible and near-infrared region. The influence of the TPD configuration, including the tip radian, the dimer distance and the aspect ratio on the electric field, Raman enhancement and spatial resolution are studied by the finite element method. The results show that there are dipole resonance band and quadruple dipole resonance band in the surface plasmon resonance band of TPD. The tip radian and dimer distance play the dominant role in the electric field enhancement, and the aspect ratio can be mainly used to tune the peak position of the electric field. The smaller tip radian and dimer distance will produce a stronger localized electric field and a small red shift of the peak position. Adjusting the aspect ratio can tune the position of electric field peak from ultraviolet (UV) to near-infrared without changing the peak value of the electric field significantly, especially for Al TPD. The maximum Raman enhancement factor of Au, Ag and Cu all reach 11 orders of magnitude, and 9 orders of magnitude for Al. The spatial resolution changes linearly with the gap distance, and the maximum spatial distributions of Au, Ag, Al and Cu achieve 0.65 nm, 0.67 nm, 0.69 nm and 0.70 nm with the dimer distance of 1 nm. Our results not only provide a better theoretical guidance for the optimization of TPD substrates in the SERS experiment, but also extend its application scope from ultra-UV to near-infrared range., (© 2021 IOP Publishing Ltd.)

A promising route to realize solar-to-chemical energy conversion resorts to water splitting using plasmon photocatalysis. However, the ultrafast carrier dynamics and underlying mechanism in such processes has seldom been investigated, especially when the single-atom catalyst is introduced. Here, from the perspective of quantum dynamics at the atomic length scale and femtosecond time scale, we probe the carrier and structural dynamics of plasmon-assisted water splitting on an Ag-alloyed Pt single-atom catalyst, represented by the Ag 19 Pt nanocluster. The substitution of an Ag atom by the Pt atom at the tip of the tetrahedron Ag 20 enhances the interaction between water and the nanoparticle. The excitation of localized surface plasmons in the Ag 19 Pt cluster strengthens the charge separation and electron transfer upon illumination. These facts cooperatively turn on more than one charge transfer channels and give rise to enhanced charge transfer from the metal nanoparticle to the water molecule, resulting in rapid plasmon-induced water splitting. These results provide atomistic insights and guidelines for the design of efficient single-atom photocatalysts for plasmon-assisted water splitting., Competing Interests: The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2021 Zhang, Chen, Meng, Li and Meng.)

The ability to control the motion of single nanoparticles or molecules is currently one of the major scientific and technological challenges. Despite tremendous progress in the field of plasmonic nanotweezers, controlled nanoscale manipulation of nanoparticles trapped by a plasmonic nanogap antenna has not been reported yet. Here, we demonstrate the controlled orbital rotation of a single fluorescent nanodiamond trapped by a gold trimer nanoantenna irradiated by a rotating linearly polarized light or circularly polarized light. Remarkably, the rotation direction is opposite to the light's polarization rotation. We numerically show that this inversion comes from sequential excitation of individual nanotriangles in the reverse order when the linear polarization is rotated, whereas using a circular polarization, light-nanoparticle angular momentum transfer occurs via the generation of a Poynting vector vortex of reversed handedness. This work provides a new path for the control of light-matter angular momentum transfer using plasmonic nanogap antennas.

Water splitting is an essential process for converting light energy into easily storable energy in the form of hydrogen. As environmentally preferable catalysts, Cu-based materials have attracted attention as water-splitting catalysts. To enhance the efficiency of water splitting, a reaction process should be developed. Single-molecule junctions (SMJs) are attractive structures for developing these reactions because the molecule electronic state is significantly modulated, and characteristic electromagnetic effects can be expected. Here, water splitting is induced at Cu-based SMJ and the produced hydrogen is characterized at a single-molecule scale by employing electron transport measurements. After visible light irradiation, the conductance states originate from Cu/hydrogen molecule/Cu junctions, while before irradiation, only Cu/water molecule/Cu junctions were observed. The vibration spectra obtained from inelastic electron tunneling spectroscopy combined with the first-principles calculations reveal that the water molecule trapped between the Cu electrodes is decomposed and that hydrogen is produced. Time-dependent and wavelength-dependent measurements show that localized-surface plasmon decomposes the water molecule in the vicinity of the junction. These findings indicate the potential ability of Cu-based materials for photocatalysis., (© 2021 Wiley-VCH GmbH.)

The role of silver localized surface plasmons (LSPs) on the luminescence of a Si(111)-(7 × 7) surface has been investigated by scanning tunneling microscopy (STM) with a silver tip at 77 K. On a bare Si(111)-(7 × 7) surface, a characteristic peak at 1.85 eV dominates the STM-induced luminescence spectrum, although the luminescence intensity is extremely weak. Once Ag atoms are deposited onto the Si surface to form islands with a few atomic layers, it is found that the intensity of the characteristic peak from the Si surface underneath the Ag islands is significantly enhanced by about one order. In addition to the luminescence from the Si surface, light emission originating from the irradiation decay of the Ag plasmons is also detected. Such great enhancement of the luminescence from the Si surface is attributed to the strong coupling between the surface states of the Si and the LSPs of the Ag islands., (© 2021 IOP Publishing Ltd.)

Localized surface plasmon resonance (LSPR) excitation on the photochromic reaction of a diarylethene derivative (DE) was studied by surface enhanced Raman scattering (SERS). UV and visible light irradiations transform reversibly DE between open-form (OF) and closed-form (CF) isomers, respectively. A mixture of PMMA and DE (either OF or CF isomer) was spin-coated onto gold nanorods (GNRs) arrays, designed by electron beam lithography, with two localized surface plasmon resonances (LSPR) at distinct wavelengths, due to their anisotropy. The photochromic reaction rates from CF to OF isomers, under LSPR excitation, were monitored from SERS spectral changes under different polarizations, on the same GNR substrate to compare the effect of LSPR field strength. It appears that the photoisomerization rate was faster when LSPR was excited with the polarization parallel to the GNR long axis. The present results highlight a potential genuine mechanism, from near field LSPR excitation, involved in the photochromic enhancement of diarylethene photochromes., (© 2020 Wiley-VCH GmbH.)

Long-range interaction in regular metallic nanostructure arrays can provide the possibility to manipulate their optical properties, governed by the excitation of localized surface plasmon (LSP) resonances. When assembling the nanoparticles in an array, interactions between nanoparticles can result in a strong electromagnetic coupling for specific grating constants. Such a grating effect leads to narrow LSP peaks due to the emergence of new radiative orders in the plane of the substrate, and thus, an important improvement of the intensity of the local electric field. In this work, we report on the optical study of LSP modes supported by square arrays of gold nanodiscs deposited on an indium tin oxyde (ITO) coated glass substrate, and its impact on the surface enhanced Raman scattering (SERS) of a molecular adsorbate, the mercapto benzoic acid (4-MBA). We estimated the Raman gain of these molecules, by varying the grating constant and the refractive index of the surrounding medium of the superstrate, from an asymmetric medium (air) to a symmetric one (oil). We show that the Raman gain can be improved with one order of magnitude in a symmetric medium compared to SERS experiments in air, by considering the appropriate grating constant. Our experimental results are supported by FDTD calculations, and confirm the importance of the grating effect in the design of SERS substrates.

We prepared MoS 2 monolayers on Au nanodot (ND) and nanohole (NH) arrays. Both these sample arrays exhibited enhanced photoluminescence intensity compared with that of a bare SiO 2 /Si substrate. The reflectance spectra of MoS 2 /ND and MoS 2 /NH had clear features originating from excitation of localized surface plasmon and propagating surface plasmon polaritons. Notably, the surface photovoltages (SPV) of these hybrid plasmonic nanostructures had opposite polarities, indicating negative and positive charging at MoS 2 /ND and MoS 2 /NH, respectively. Surface potential maps, obtained by Kelvin probe force microscopy, suggested that the potential gradient led to a distinct spatial distribution of photo-generated charges in these two samples under illumination. Furthermore, the local density of photo-generated excitons, as predicted from optical simulations, explained the SPV spectra of MoS 2 /ND and MoS 2 /NH. We show that the geometric configuration of the plasmonic nanostructures modified the polarity of photo-generated excess charges in MoS 2 . These findings point to a useful means of optimizing optoelectronic characteristics and improving the performance of MoS 2 -based plasmonic devices.

Metal nanoparticles are attractive for plasmon-enhanced generation of hot carriers, which may be harnessed in photochemical reactions. In this work, we analyze the coherent femtosecond dynamics of photon absorption, plasmon formation, and subsequent hot-carrier generation through plasmon dephasing using first-principles simulations. We predict the energetic and spatial hot-carrier distributions in small metal nanoparticles and show that the distribution of hot electrons is very sensitive to the local structure. Our results show that surface sites exhibit enhanced hot-electron generation in comparison to the bulk of the nanoparticle. Although the details of the distribution depend on particle size and shape, as a general trend, lower-coordinated surface sites such as corners, edges, and {100} facets exhibit a higher proportion of hot electrons than higher-coordinated surface sites such as {111} facets or the core sites. The present results thereby demonstrate how hot carriers could be tailored by careful design of atomic-scale structures in nanoscale systems.

Broadband metamaterial absorbers (MAs) are critical for applications of photonic and optoelectronic devices. Despite long-standing efforts on broadband MAs, it has been challenging to achieve ultrabroadband absorption with high absorptivity and omnidirectional characteristics within a comparatively simple and low-cost architecture. Here we design, fabricate, and characterize a novel compact Cr-based MA to achieve ultrabroadband absorption in the visible to near-infrared wavelength region. The Cr-based MA consists of Cr nanorods and Cr substrate sandwiched by three pairs of SiO 2 /Cr stacks. Both simulated and experimental results show that an average absorption over 93.7% can be achieved in the range of 400-1000 nm. Specifically, the ultrabroadband features result from the co-excitations of localized surface plasmon (LSP) and propagating surface plasmon (PSP) and their synergistic absorption effects, where absorption in the shorter and longer wavelengths are mainly contributed bythe LSP and PSP modes, respectively. The Cr-based MA is very robust to variations of the geometrical parameters, and angle-and polarization-insensitive absorption can be operated well over a large range of anglesunder both transverse magnetic(TM)- and transverse electric (TE)-polarized light illumination.

Ag nanoparticles (NPs) are filled in a photonic crystal (PhC) hole array on green light emitting diodes (LEDs). The localized surface plasmon (LSP)-quantum well (QW) coupling effect is studied by measuring the cathodoluminescence (CL) spectra impinging at the specific spots on the Ag NPs. Twenty-six percent and fifty-two percent enhancements of the CL intensities are obtained at the center and edge of the Ag NP, respectively, compared to the result that the electron-beam (e-beam) excites the QW directly. To illustrate the coupling process of the three-body system of e-beam-LSP-QW, a perturbation theory combining a three-dimensional (3D) finite difference time domain (FDTD) simulation is put forward. The effects of the polarization orientation of the dipole and the field symmetry of the LSP on the LSP-QW coupling are also discussed.

Absorption enhancement based on interaction between the localized surface plasmon (LSP) and molecular exciton is one of the most important phenomena for the development of high-performance solar devices. In this study, hybrids of plasmonic metal nanoparticles and dye molecules have been developed, which exhibit enhanced absorption at precisely tuned wavelengths in a visible region. The hybrids consist of a porphyrin derivative, which has four absorption peaks (Q-bands) in a range of 500-700 nm, and triangular silver nanoprisms (AgPRs), which are developed by us to exhibit precisely tuned LSP resonance wavelengths. Absorption enhancement over the whole Q-band range is induced by the combined use of three kinds of AgPRs of different aspect ratios. Furthermore, the quantitative evaluation of absorption enhancement based on the LSP-based fluorescence enhancement phenomenon has demonstrated that efficient absorption enhancement can be effected at multiple wavelengths.

The excitation of localized surface plasmon resonances (LSPRs) in metal nanostructures enables subwavelength photon localization and large electric field enhancement, which can be advantageously used to strongly enhance light-matter interactions at the nanoscale. For this purpose, efficient methods for deterministically handling and arranging nanomaterials at the exact position of the localized electric field are required. In this Letter, we propose a novel method based on a hydrothermal synthesis reaction to locally and selectively synthesize zinc oxide in a plasmonic nanoantenna. We first make evident the role of LSPR for achieving efficient heating of gold nanostructures. Then, by selectively addressing one of the LSPRs of a gold antenna, we demonstrate that localized zinc oxide formation at the targeted location of the antenna can be achieved due to the nanoscale confinement of the heat production.

A new colorimetric method that can be used to rapidly detect toxic ricin is demonstrated. Lactosylated cysteine-functionalized gold nanoparticles (Au@LACY NPs) were prepared by a one-pot reaction and employed as optical probes for determination of ricin B chain. It is found that the Au@LACY NPs undergo aggregation in the presence of ricin B chain. This leads to surface plasmon coupling effects of the particles and a color change from red to blue, with absorption maxima at 519 and 670 nm, respectively. The feasibility of using the current approach for quantitative analysis of ricin B chain is also demonstrated. The calibration plot is generated by plotting the ratio of the absorbance at the wavelength of 634 to 518 nm versus the concentration of the ricin B chain. The spectrophotometric method has a ~29 pM (~ 0.91 ng·mL -1 ) detection limit, and the sample with the concentration of ~ 400 pM (~ 13 ng·mL -1 ) can be detected visually. Graphical abstractSchematic representation of using lactosylated cysteine capped gold nanoparticles (Au@LACY NPs) as colorimetric probes for the ricin B chain through surface plasmon coupling effects. Sample solution turns from red to blue in the presence of ricin B chain.

In this study, we propose a liquid-phase-deposited silver nanoparticle embedded ZnO (LPD-Ag NP/ZnO) thin film at room temperature to improve the light extraction efficiency (LEE) for InGaN/GaN light-emitting diodes (LEDs). The treatment solution for the deposition of the LPD-Ag/NP ZnO thin film comprised a ZnO-powder-saturated HCl and a silver nitrate (AgNO₃) aqueous solution. The enhanced LEE of an InGaN/GaN LED with the LPD-Ag NP/ZnO window layer can be attributed to the surface texture and localized surface plasmon (LSP) coupling effect. The surface texture of the LPD-Ag/NP ZnO window layer relies on the AgNO₃ concentration, which decides the root-mean-square (RMS) roughness of the thin film. The LSP resonance or extinction wavelength also depends on the concentration of AgNO₃, which determines the Ag NP size and content of Ag atoms in the LPD-Ag NP/ZnO thin film. The AgNO₃ concentration for the optimal LEE of an InGaN/GaN LED with an LPD-Ag NP/ZnO window layer occurs at 0.05 M, which demonstrates an increased light output intensity that is approximately 1.52 times that of a conventional InGaN/GaN LED under a 20-mA driving current., Competing Interests: The authors declare no conflict of interest.

The metal/graphene interface has been one of the most important research topics with regard to charge screening, charge transfer, contact resistance, and solar cells. Chemical bond formation of metal and graphene can be deduced from the defect induced D-band and its second-order mode, 2D band, measured by Raman spectroscopy, as a simple and nondestructive method. However, a phonon mode located at ∼1350 cm -1 , which is normally known as the defect-induced D-band, is intriguing for graphene deposited with noble metals (Ag, Au, and Cu). We observe anomalous K-point phonons in nonreactive noble metal/graphene heterostructures. The intensity ratio of the midfrequency mode at ∼1350 cm -1 over G-band (∼1590 cm -1 ) exhibits nonlinear but resonant behavior with the excitation laser wavelength, and more importantly, the phonon frequency-laser energy dispersion is ∼10-17 cm -1 eV -1 , which is much less than the conventional range. These phonon modes of graphene at nonzero phonon wave vector (q ≠ 0) around K points are activated by localized surface plasmon resonance and not by the defects due to chemical bond formation of metal/graphene. This hypothesis is supported by density functional theory (DFT) calculations for noble metals and Cr along with the measured contact resistances.

In order to enhance the refractive index sensing performance of simple particle arrays, a structure, consisting of Au/SiO 2 triangle arrays layers and reflection Au substrate, with increasing size and lengthening tips of triangles, is studied. The triangle arrays are modeled after an experimentally realizable "imprint" of microsphere lithography. Numerical calculation was carried out to study its optical properties and spectral sensitivity. The calculation results show that a large local enhancement of electric field (61 times) and simultaneously high absorption is due to combination of the resonance absorption of Au triangle disks, plasmonic couplings between the Au triangle disks and the Au film, and the high-density packing of triangle disks. The absorption peaks were not detuned when the gap between neighboring tips of the triangles varied from 10 to 50 nm. When the thickness of SiO 2 layer increased from 10 to 50 nm, the absorption peak shifted to longer wavelengths and the amplitude rises quickly signaling the dominance of the gap mode resonance between the two Au layers. As the thickness of the top Au layer varies from 10 to 50 nm, the absorption peak is also red shifted and the peak amplitude increases. The full width at half maximum of the peaks for high absorption (> 90%) is about 5 nm. When fixing the gap, the thicknesses of Au/SiO 2 triangle layer, and increasing the surrounding refractive index from 1.33 to 1.36, the absorption peaks shifted quickly, with a refractive index sensitivity and figure of merit as high as 660 nm per refractive index unit and 132, respectively. Such arrays can be easily fabricated by using microsphere array as projection masks and find application in refractive index monitoring of liquid and identification of gas and liquid phases.

Three kinds of typical structures, hemi-/spherical nanoparticles/nanoparticle dimers on the substrate and spherical nanoparticles/nanoparticle dimers half-buried into the substrate, are used for FDTD simulation to theoretically discuss the influence of the substrate to the localized surface plasmon (LSP) coupling when the metal nanoparticles/nanoparticle dimers are locating near a substrate. Simulated results show that the dependencies between the LSP coupling wavelength and the refractive index of the substrate for different structures are not the same, which can be attributed to the different polarization field distributions of LSPs. When light is incident from different directions, the LSP coupling strength are not the same as well and the ratios of the scattering peak intensities depend on the position of the metal nanoparticles or nanoparticle dimers. These phenomenon can be explained by the difference of the local driving electric field intensities which is modulated by the interface between the air and the substrate.

The ability to manipulate light-matter interaction in semiconducting nanostructures is fascinating for implementing functionalities in advanced optoelectronic devices. Here, we report the tailoring of radiative emissions in a ZnTe/ZnTe:O/ZnO core-shell single nanowire coupled with a one-dimensional aluminum bowtie antenna array. The plasmonic antenna enables changes in the excitation and emission processes, leading to an obvious enhancement of near band edge emission (2.2 eV) and subgap excitonic emission (1.7 eV) bound to intermediate band states in a ZnTe/ZnTe:O/ZnO core-shell nanowire as well as surface-enhanced Raman scattering at room temperature. The increase of emission decay rate in the nanowire/antenna system, probed by time-resolved photoluminescence spectroscopy, yields an observable enhancement of quantum efficiency induced by local surface plasmon resonance. Electromagnetic simulations agree well with the experimental observations, revealing a combined effect of enhanced electric near-field intensity and the improvement of quantum efficiency in the ZnTe/ZnTe:O/ZnO nanowire/antenna system. The capability of tailoring light-matter interaction in low-efficient emitters may provide an alternative platform for designing advanced optoelectronic and sensing devices with precisely controlled response.

We analyzed the coupling behavior between the localized surface plasmon (LSP) and quantum wells (QWs) using cathodoluminescence (CL) in a green light-emitting diodes (LED) with Ag nanoparticles (NPs) filled in photonic crystal (PhC) holes. Photoluminescence (PL) suppression and CL enhancement were obtained for the same green LED sample with the Ag NP array. Time-resolved PL (TRPL) results indicate strong coupling between the LSP and the QWs. Three-dimensional (3D) finite difference time domain (FDTD) simulation was performed using a three-body model consisting of two orthogonal dipoles and a single Ag NP. The LSP–QWs coupling effect was separated from the electron-beam (e-beam)–LSP–QW system by linear approximation. The energy dissipation was significantly reduced by the z-dipole introduction under the e-beam excitation. In this paper, the coupling mechanism is discussed and a novel emission structure is proposed.

We investigated the influence of metal coating on the optical characteristics of Si nanopillar (NP) arrays with and without thin metal layers coated on the sample surface. The reflection dips of the metal-coated arrays were much broader and more pronounced than those of the bare arrays. The coated metal layers consisted of two parts-the metal disks on the Si NP top and the holey metal backreflectors on the Si substrate. The Mie-like geometrical resonance in the NPs, the localized surface plasmons in the metal disks, and the propagation of surface plasmon polariton along the backreflector/substrate interface could contribute to the reflection spectra. Finite-difference time-domain simulation results showed that the interplay of the plasmonic effects and the geometric resonance gave rise to significantly enhanced light confinement and consequent local absorption in the metal-Si hybrid nanostructures.

Surface-enhanced resonance Raman scattering (SERRS) of rhodamine 6G was measured on confeito-like Au nanoparticles (CAuNPs). The large CAuNPs (100 nm in diameter) in aqueous dispersion systems showed stronger enhancing effect (analytical enhancement factor: over 10⁵) of SERRS than the small CAuNPs (50 nm in diameter), while the spherical Au nanoparticles (20 nm in diameter) displayed rather weak intensities. Especially, minor bands in 1400-1600 cm -1 were uniquely enhanced by the resonance effect of CAuNPs. The enhancement factors revealed a concentration dependence of the enhancing effect at low concentration of rhodamine 6G. This dependency was due to a large capacity of hot-spots on CAuNPs, which were formed without agglomeration. The surface-enhancing behaviour in the film systems was similar to that in the dispersions, although the large CAuNPs had lower enhancing effect in the films, and the small CAuNPs and the spherical Au nanoparticles were more effective in their films. These results suggest that the CAuNPs have an advantage in ultrasensitive devices both in dispersions and films, compared to the agglomerate of spherical Au nanoparticles., Competing Interests: The authors declare no conflict of interest.

A label-free technique for the detection of triacylglycerides by a localized surface plasmon resonance (LSPR)-based biosensor is demonstrated. An LSPR-based fiber-optic sensor probe is fabricated by immobilizing lipase enzyme on silver nanoparticles (Ag-NPs) coated on an unclad segment of a plastic clad optical fiber. The size and shape of nanoparticles were characterized by high-resolution transmission electron microscopy and UV-visible spectroscopy. The peak absorbance wavelength changes with concentration of triacylglycerides surrounding the sensor probe, and sensitivity is estimated from shift in the peak absorbance wavelength as a function of concentration. The fabricated sensor was characterized for the concentration of triacylglyceride solution in the range 0 to 7 mM. The sensor shows the best sensitivity at a temperature of 37°C and pH 7.4 of the triacylglycerides emulsion with a response time of 40 s. A sensitivity of 28.5  nm/mM of triacylglyceride solution is obtained with a limit of detection of 0.016 mM in the entire range of triacylglycerides. This compact biosensor shows good selectivity, stability, and reproducibility in the entire physiological range of triacylglycerides and is well-suited to real-time online monitoring and remote sensing., ((2017) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE).)

Localized surface plasmon (LSP) has been widely applied for the enhancement of fluorescence emission for biosensing owing to its potential for strong field enhancement. However, due to its small penetration depth, LSP offers limited fluorescence enhancement over a whole sensor chip and, therefore, insufficient sensitivity for the detection of biomolecules, especially large molecules. We demonstrate the simultaneous excitation of LSP and propagating surface plasmon (PSP) on an Au nanohole array under Kretschmann configuration for the detection of prostate-specific antigen with a sandwich immunoassay. The proposed method combines the advantages of high field enhancement by LSP and large surface area probed by PSP field. The simulated results indicated that a maximum enhancement of electric field intensity up to 1,600 times can be achieved under the simultaneous excitation of LSP and PSP modes. The sandwich assay of PSA carried out on gold nanohole array substrate showed a limit of detection of 140 fM supporting coexcitation of LSP and PSP modes. The limit of detection was approximately sevenfold lower than that when only LSP was resonantly excited on the same substrate. The results of this study demonstrate high fluorescence enhancement through the coexcitation of LSP and PSP modes and pave a way for its implementation as a highly sensitive bioassay., Competing Interests: Disclosure The authors report no conflicts of interest in this work.

We developed a localized surface plasmon-induced visible light-responsive photoelectrochemical (PEC) biosensor using a titanium dioxide (TiO 2 ) photoelectrode loaded with gold nanoislands (AuNIs) for in situ real-time measurement of biotin-streptavidin association. As a proof of concept, self-assembled thiol-terminated biotin molecules bound on a AuNIs/TiO 2 photoelectrode were successfully utilized to explore the photocurrent response to streptavidin-modified gold nanoparticle (STA-AuNP) solutions. This plasmon-induced PEC biosensor is simple and easy to miniaturize. Additionally, the PEC biosensor achieves highly sensitive measurements under only visible light irradiation and prevents the UV-induced damage of samples. Furthermore, a novel approach has been proposed to realize the real-time monitoring of biotin-STA binding affinities and kinetics by analyzing the PEC sensing characteristics. This PEC biosensor and novel analysis method could provide a new approach for the specific electrical detection and real-time kinetic measurements for clinical diagnostics and drug development., (Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.)

We demonstrate the fabrication and characterization of localized surface plasmon (LSP)-enhanced n-ZnO quantum dot (QD)/MgO/p-GaN heterojunction light-emitting diodes (LEDs) by embedding Ag nanoparticles (Ag-NPs) into the ZnO/MgO interface. The maximum enhancement ration of the Ag-NP-decorated LEDs in electroluminescence (EL) is 4.3-fold by optimizing MgO electron-blocking layer thickness. The EL origination was investigated qualitatively in terms of photoluminescence (PL) results. Through analysis of the energy band structure of device and carrier transport mechanisms, it suggests that the EL enhancement is attributed to the increased rate of spontaneous emission and improved internal quantum efficiency induced by exciton-LSP coupling.

As the use of biosensors for early in-vitro diagnosis of malignant diseases has expanded, issues associated with ultra-sensitivity and wide dynamic range have become paramount. In this study, we designed a sub-zeptomolar sensor for detecting the alpha-feto protein (AFP) that utilizes localized surface plasmon resonance (LSPR) assisted by bio-catalytic reaction and a self-controlled detection scheme. A gold nanodot array (GNA), serving as a plasmonic material, was fabricated using an improved UV nanoimprint lithography (NIL) method that employs a sacrificial layer. In the new approach, LSPR observation is highly stable because it employs a back reflection mode, which avoids passing the signal through the sample solution. An enzyme-precipitation reaction was conducted on the AFP antigen-antibody complex on the surface of the gold nanodot (nano-ELISA) using a procedure that was described previously. To extend the AFP detection limit below femtomolar concentrations, a scheme involving self-controlled detection was employed to lower the limit. In this method, the sample including the target simultaneously plays the role of both sample and negative control. Using this scheme, AFP can be detected at concentrations as low as 14 aM (0.7 zeptomole in 50μL serum) and with the wide dynamic range of 10fgmL(-1)-10ngmL(-1). Importantly, the new method provides a platform for studying and monitoring interactions between biochemically active substances that are present in very low concentrations. Finally, the general strategy used to design the detection method can be easily adapted to the ultra-sensitive detection of other biomarkers and pathogens., (Copyright © 2016 Elsevier B.V. All rights reserved.)

Plasmonic surfaces are mainly used for their optical intensity concentration properties that allow for enhancement of physical interaction like in nonlinear optics, optical sensors, or tweezers. Phase response in plasmonic resonances can also play a major role, especially in a periodic assembly of plasmonic resonators like metasurfaces. Here we show that localized surface plasmons collectively excited by a guided mode in a metallic nanostructure periodic chain present nonmonotonous phase variation along the 1D metasurface, resulting from both selective Bloch mode coupling and dipolar coupling. As shown by near-field measurements, the phase profile of the highly concentrated optical field is carved out in the vicinity of the metallic metasurface, paving the way to unusual local optical functions.

Strong coupling between semiconductor excitons and localized surface plasmons (LSPs) giving rise to hybridized plexciton states in which energy is coherently and reversibly exchanged between the components is vital, especially in the area of quantum information processing from fundamental and practical points of view. Here, in photoluminescence spectra, rather than from common extinction or reflection measurements, we report on the direct observation of Rabi splitting of approximately 160 meV as an indication of strong coupling between excited states of CdSe/ZnS quantum dots (QDs) and LSP modes of silver nanoshells under nonresonant nanosecond pulsed laser excitation at room temperature. The strong coupling manifests itself as an anticrossing-like behavior of the two newly formed polaritons when tuning the silver nanoshell plasmon energies across the exciton line of the QDs. Further analysis substantiates the essentiality of high pump energy and collective strong coupling of many QDs with the radiative dipole mode of the metallic nanoparticles for the realization of strong coupling. Our finding opens up interesting directions for the investigation of strong coupling between LSPs and excitons from the perspective of radiative recombination under easily accessible experimental conditions.

Exciton-plasmon coupling in hybrids of a monolayer transition metal dichalcogenide and Ag nanoparticles is investigated in the weak and strong coupling regimes. In the weak coupling regime, both absorption enhancement and the Purcell effect collectively modify the photoluminescence properties of the semiconductor. In the strong coupling regime, electromagnetically induced transparency dips are displayed, evidencing coherent energy exchange between excitons and plasmons., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

It is known (yet often ignored) from quantum mechanical or energetic considerations, that the threshold gain of the quasi-static spaser depends only on the dielectric functions of the metal and the gain material. Here, we derive this result from the purely classical electromagnetic scattering framework. This is of great importance, because electrodynamic modelling is far simpler than quantum mechanical one. The influence of the material dispersion and spaser geometry are clearly separated; the latter influences the threshold gain only indirectly, defining the resonant wavelength. We show that the threshold gain has a minimum as a function of wavelength. A variation of nanoparticle shape, composition, or spasing mode may shift the plasmonic resonance to this optimal wavelength, but it cannot overcome the material-imposed minimal gain. Furthermore, retardation is included straightforwardly into our framework; and the global spectral gain minimum persists beyond the quasi-static limit. We illustrate this with two examples of widely used geometries: Silver spheroids and spherical shells embedded in and filled with gain materials.

The generation of ammonia from atmospheric nitrogen and water using sunlight is a preferable approach to obtaining ammonia as an energy carrier and potentially represents a new paradigm for achieving a low-carbon and sustainable-energy society. Herein, we report the selective conversion of dinitrogen into ammonia through plasmon-induced charge separation by using a strontium titanate (SrTiO3) photoelectrode loaded with gold nanoparticles (Au-NPs) and a zirconium/zirconium oxide (Zr/ZrOx ) thin film. We observed the simultaneous stoichiometric production of ammonia and oxygen from nitrogen and water under visible-light irradiation., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Localized surface plasmon (LSP)-enhanced ultraviolet LEDs have been constructed via spin-coating Ag nanoparticles onto ZnO/SiO2 core/shell nanorod array/p-GaN heterostructures. Different from the previous reports where the dielectric spacer-layer thickness was determined only through photoluminescence (PL) characterization, the SiO2 shell thickness in this work is also optimized by actual electroluminescence (EL) measurements to maximize the enhancement. It is interesting to find that the enhancement ratios derived from PL and EL measurements demonstrate different thickness dependences on SiO2 shell: an optimal 3.5-fold PL enhancement was obtained at the SiO2 thickness of 16 nm, while an "abnormal" 7-fold EL enhancement was achieved at the thickness of 12 nm. Time-resolved spectroscopy studies, as well as theoretical estimations and numerical simulations, reveal that the higher-ratio EL enhancement stems from joint contributions, both internal-quantum-efficiency improvement induced by exciton-LSP coupling and light-extraction-efficiency improvement aroused by photon-LSP coupling.