Sensitive label-free biosensors by using gap plasmons in gold nanoslits

The detection sensitivities of gap plasmons in gold nanoslit arrays are studied and compared with surface plasmons on outside surface. The nanoslit arrays were fabricated in a 130 nm-thick gold film with various slit widths. For transverse-magnetic (TM) incident wave, the 600 nm-period nanoslit array shows two distinguishable transmission peaks corresponding to the resonances of gap plasmons and surface plasmons, respectively. The surface sensitivities for both modes were compared by coating thin SiO(2) film and different biomolecules on the nanoslit arrays. Our experimental results verify gap plasmons are more sensitive than conventional surface plasmons. Its detection sensitivity increases with the decrease of slit width. The gap plasmon is one order of magnitude sensitive than the surface plasmon for slit widths smaller than 30 nm. We attribute this high sensitivity to the large overlap between biomolecules and nanometer-sized gap plasmons.     

Plasmon Modes Management

A new plasmonic structure based on bimetallic layer is proposed. We analyze the structure and show that bimetallic film plays a crucial role in the management of surface plasmons. The roll of the buffer is discussed, as well. Up to three surface plasmons can be excited simultaneously in the structure. Two of plasmons can be used for two-plasmon spectroscopy. The third plasmon can be used for controlling the temperature of the structure.     

Curved Gratings as Plasmonic Lenses for Linearly Polarised Light

The ability of curved gratings as sectors of concentric circular gratings to couple linearly polarised light into focused surface plasmons is investigated by theory, simulation, and experiment. The experimental and simulation results show that increasing the sector angle of the curved gratings decreases the width of the lateral distribution of surface plasmons resulting in focusing of surface plasmons, which is analogous to the behaviour of classical optical lenses. We also show that two faced curved gratings, with their groove radius mismatched by half of the plasmon wavelength (asymmetric configuration), can couple linearly polarised light into a single focal spot of concentrated surface plasmons with smaller depth of focus and higher intensity in comparison to single curved gratings. The major advantage of these structures is the coupling of linearly polarised light into focused surface plasmons with access to, and control of, the plasmon focal spot, which facilitate their potential applications in sensing, detection, and nonlinear plasmonics.     

Low Energy Intraband Plasmons and Electron Energy Loss Spectra of Single and Multilayered Graphene

We present a theory for the calculation of the low energy intraband plasmon frequencies and the electron energy loss (EEL) spectra of single layer and multilayer graphene sheets. Our calculation shows that the number of plasmons that can be excited is equal to the number of graphene layers in the sample. One of these is the dominant in-phase plasmon having a square root dependence on the wave number at low wave vectors, whereas the others are out-of-phase plasmons having near linear dependences on the wave number. The EEL spectra of a single layer graphene shows a single peak at the plasmon frequency, which has been observed experimentally. The EEL spectra of all multilayer graphenes have two peaks, one corresponding to the dominant in-phase plasmon and the other due to the out of phase plasmons. We predict that careful measurement of the EEL of multilayer graphene will show both peaks due to the low energy intraband plasmons.

     

Bragg-Scattered Surface Plasmon Microscopy: Theoretical Study

We present a new approach to surface plasmon microscopy with high refractive index sensitivity and spatial resolution that is not limited by the propagation length of surface plasmons. It is based on a nanostructured metallic sensor surface supporting Bragg-scattered surface plasmons. We show that these non-propagating surface plasmon modes are excellently suited for spatially resolved observations of refractive index variations on the sensor surface owing to their highly confined field profile perpendicular to as well as parallel to the metal interface. The presented theoretical study reveals that this approach enables reaching similar refractive index sensitivity as regular surface plasmon resonance (SPR) microscopy and offers the advantage of improved spatial resolution when observing dielectric features with lateral size <10???m for the wavelength around 800?nm and gold as the SPR-active metal. This paper demonstrates the potential of Bragg-scattered surface plasmon microscopy for high-throughput SPR biosensing with high-density microarrays.     

Plasmonics in Biology and Plasmon-Controlled Fluorescence

Fluorescence technology is fully entrenched in all aspects of biological research. To a significant extent, future advances in biology and medicine depend on the advances in the capabilities of fluorescence measurements. As examples, the sensitivity of many clinical assays is limited by sample autofluorescence, single-molecule detection is limited by the brightness and photostability of the fluorophores, and the spatial resolution of cellular imaging is limited to about one-half of the wavelength of the incident light. We believe a combination of fluorescence, plasmonics, and nanofabrication can fundamentally change and increase the capabilities of fluorescence technology. Surface plasmons are collective oscillations of free electrons in metallic surfaces and particles. Surface plasmons, without fluorescence, are already in use to a limited extent in biological research. These applications include the use of surface plasmon resonance to measure bioaffinity reactions and the use of metal colloids as light-scattering probes. However, the uses of surface plasmons in biology are not limited to their optical absorption or extinction. We now know that fluorophores in the excited state can create plasmons that radiate into the far field and that fluorophores in the ground state can interact with and be excited by surface plasmons. These reciprocal interactions suggest that the novel optical absorption and scattering properties of metallic nanostructures can be used to control the decay rates, location, and direction of fluorophore emission. We refer to these phenomena as plasmon-controlled fluorescence (PCF). We predict that PCF will result in a new generation of probes and devices. These likely possibilities include ultrabright single-particle probes that do not photobleach, probes for selective multiphoton excitation with decreased light intensities, and distance measurements in biomolecular assemblies in the range from 10 to 200 nm. Additionally, PCF is likely to allow design of structures that enhance emission at specific wavelengths and the creation of new devices that control and transport the energy from excited fluorophores in the form of plasmons, and then convert the plasmons back to light. Finally, it appears possible that the use of PCF will allow construction of wide-field optical microscopy with subwavelength spatial resolution down to 25 nm.     

Single-Particle Spectroscopy of Supported Silver Clusters on Silicon: Substrate Effects on Localized Surface Plasmons

The presence of a surrounding medium strongly affects the spectral properties of localized surface plasmons at metallic nanoparticles. Vice versa, plasmonic resonances have large impact on the electric polarization in a surrounding or supporting material. For applications, e.g., in light-converting devices, the coupling of localized surface plasmons with polarizations in semiconducting substrates is of particular importance. Using photoemission electron microscopy with tunable laser excitation, we perform single-particle spectroscopy of silver nanoclusters directly grown on Si(100). Two distinct localized surface plasmon modes are observed as resonances in the two-photon photoemission signals from individual silver clusters. The strengths of these resonances strongly depend on the polarization of the exciting electric field, which allows us to assign them to plasmon modes with polarizations parallel and perpendicular, respectively, to the supporting silicon substrate. Our mode assignment is supported by simulations which provide insight into the mutual interaction of charge oscillations at the particle surface with electric polarizations at the silver/silicon interface.

     

Surface plasmon resonance imaging on a microchip for detection of DNA-modified gold nanoparticles deposited onto the surface in a non-cross-linking configuration

We report theoretical predictions and experimental observations of the reduced detection volume with the use of surface-plasmon-coupled emission (SPCE). The effective fluorescence volume (detection volume) in SPCE experiments depends on two near-field factors: the depth of evanescent wave excitation and a distance-dependent coupling of excited fluorophores to the surface plasmons. With direct excitation of the sample (reverse Kretschmann excitation) the detection volume is restricted only by the distance-dependent coupling of the excitation to the surface plasmons. However, with the excitation through the glass prism at surface plasmon resonance angle (Kretschmann configuration), the detection volume is a product of evanescent wave penetration depth and distance-dependent coupling. In addition, the detection volume is further reduced by a metal quenching of excited fluorophores at a close proximity (below 10nm). The height of the detected volume size is 40-70nm, depending on the orientation of the excited dipoles. We show that, by using the Kretschmann configuration in a microscope with a high-numerical-aperture objective (1.45) together with confocal detection, the detection volume can be reduced to 1-2attoL. The strong dependence of the coupling to the surface plasmons on the orientation of excited dipoles can be used to study the small conformational changes of macromolecules.     

Quantum Theory of Surface Plasmon Polaritons: Planar and Spherical Geometries

A quantum theory of retarded surface plasmons on a metal–vacuum interface is formulated, by analogy with the well-known and widely exploited theory of exciton-polaritons. The Hamiltonian for mutually interacting instantaneous surface plasmons and transverse electromagnetic modes is diagonalized with recourse to a Hopfield–Bogoljubov transformation, in order to obtain a new family of modes, to be identified with retarded plasmons. The interaction with nearby dipolar emitters is treated with a full quantum formalism based on a general definition of modal effective volumes. The illustrative cases of a planar surface and of a spherical nanoparticle are considered in detail. In the ideal situation of absence of dissipation, as an effect of the conservation of in-plane wavevector, retarded plasmons on a planar surface represent true stationary states (which are usually called surface plasmon polaritons), whereas retarded plasmons in a spherical nanoparticle, characterized by frequencies that overlap with the transverse electromagnetic continuum, become resonances with a finite radiative broadening. The theory presented constitutes a suitable full quantum framework for the study of nonperturbative and nonlinear effects in plasmonic nanosystems.     

Efficient Extraction of Fluorescence Emission Utilizing Multiple Surface Plasmon Modes from Gold Wire Gratings

We demonstrate directional enhanced fluorescence emission from fluorophores located above gold wire gratings. In contrast to previous studies on corrugated films, efficient coupling was recorded for multiple plasmon modes associated with both the active and substrate side of the wires. This difference is likely due to the subtle differences in how light interacts with corrugated films versus metal films with periodic subwavelength slots. For corrugated films, coupling between modes on opposite sides of the grating are out of phase, and therefore plasmon modes on the opposite side of the grating are only weakly excited. For wire gratings, transmission and reflection features have been modeled well with a dynamical diffraction model that includes surface plasmons, which allows for efficient coupling to surface plasmon modes on both sides of the grating. We also compared the two mechanisms for fluorescent enhancement, namely the intense electromagnetic field associated with surface plasmons and excited fluorophores radiating via surface plasmon modes. We found the latter mechanism clearly dominant.     

Fabrication of Silver-Silicon Gratings for Surface Plasmon Excitation Using Nanosecond Laser Interference Lithography

Plasmonics - We introduce a new two-step method to fabricate silver-silicon gratings that can excite surface plasmons efficiently. The grating structure was firstly created on a flat silicon...     

Ring Gap Resonance Modes on Disk/Film Coupling System Caused by Strong Plasmon Interaction

Ring modes with large wave vectors cannot be easily excited on a single disk by the plane wave illumination with the polarization parallel to the disk interface. In this work, we show that special antisymmetric ring gap modes on the surface of the disk in close proximity to the metallic thin film can be excited in the visible light region of the electromagnetic spectrum. In the presence of the film, the strong plasmon interaction between disk and film causes ring gap modes to have lower energies and be more easily excited. We apply the plasmon hybridization method to illustrate the ring gap modes arising from the interaction between the localized disk plasmons and the continuum surface plasmons. The calculated hybridization data show good agreement with the results of finite element simulations. The excitation of ring gap modes provides further insight into the strong coupling of plasmons and the design of novel nanostructures.

     

Four-dimensional microED of conformational dynamics in protein microcrystals on the femto-to-microsecond timescales

As structural determination of protein complexes approaches atomic resolution, there is an increasing focus on conformational dynamics. Here we conceptualize the combination of two techniques which have become established in recent years: microcrystal electron diffraction and ultrafast electron microscopy. We show that the extremely low dose of pulsed photoemission still enables microED due to the strength of the electron bunching from diffraction of the protein crystals. Indeed, ultrafast electron diffraction experiments on protein crystals have already been demonstrated to be effective in measuring intermolecular forces in protein microcrystals. We discuss difficulties that may arise in the acquisition and processing of data and the overall feasibility of the experiment, paying specific attention to dose and signal-to-noise ratio. In doing so, we outline a detailed workflow that may be effective in minimizing the dose on the specimen. A series of model systems that would be good candidates for initial experiments is provided.     

Controllable Coupling of Localized and Propagating Surface Plasmons to Tamm Plasmons

We theoretically investigate the coupling between Tamm plasmons and localized surface plasmons (LSPs) as well as propagating surface plasmons (PSPs) in a multilayer structure consisting of a metallic nanowire array and a spatially separated metal–dielectric Bragg reflector (DBR). A clear anticrossing behavior of the resonances is observed in the dispersion diagram resulting from the coupling, which is well explained by the coupled oscillator model. The coupling also creates new hybrid LSP or PSP modes with narrow bandwidths and unique spectral features. Upon the excitation of these hybrid modes, the local fields underneath the nanowires for the hybrid LSPs or near the lower metal layer surface for the hybrid PSPs are both enhanced greatly as compared with those achieved in the structure without DBR, which has potential applications in nonlinear optics and surface-enhanced spectroscopies.     

Diversity of dermal denticle structure in sharks: Skin surface roughness and three‐dimensional morphology

Shark skin is covered with numerous placoid scales or dermal denticles. While previous research has used scanning electron microscopy and histology to demonstrate that denticles vary both around the body of a shark and among species, no previous study has quantified three‐dimensional (3D) denticle structure and surface roughness to provide a quantitative analysis of skin surface texture. We quantified differences in denticle shape and size on the skin of three individual smooth dogfish sharks (Mustelus canis) using micro‐CT scanning, gel‐based surface profilometry, and histology. On each smooth dogfish, we imaged between 8 and 20 distinct areas on the body and fins, and obtained further comparative skin surface data from leopard, Atlantic sharpnose, shortfin mako, spiny dogfish, gulper, angel, and white sharks. We generated 3D images of individual denticles and measured denticle volume, surface area, and crown angle from the micro‐CT scans. Surface profilometry was used to quantify metrology variables such as roughness, skew, kurtosis, and the height and spacing of surface features. These measurements confirmed that denticles on different body areas of smooth dogfish varied widely in size, shape, and spacing. Denticles near the snout are smooth, paver‐like, and large relative to denticles on the body. Body denticles on smooth dogfish generally have between one and three distinct ridges, a diamond‐like surface shape, and a dorsoventral gradient in spacing and roughness. Ridges were spaced on average 56 µm apart, and had a mean height of 6.5 µm, comparable to denticles from shortfin mako sharks, and with narrower spacing and lower heights than other species measured. We observed considerable variation in denticle structure among regions on the pectoral, dorsal, and caudal fins, including a leading‐to‐trailing edge gradient in roughness for each region. Surface roughness in smooth dogfish varied around the body from 3 to 42 microns.     

Tunnel Light Through a Continuous Optically Thick Metal Film Utilizing Higher Order Magnetic Plasmon Resonance

In this letter, we investigate the extraordinary optical transmission behavior of a flat continuous metal film sandwiched by magnetic plasmonic structures. A new mechanism by utilizing higher order magnetic plasmon resonance is proposed to enhance the transmission. Numerical simulation results show that 80 % electromagnetic energy can be transmitted through the middle 50-nm-thick continuous gold film in near-infrared regime. The excitation of the second-order magnetic plasmons and the propagating surface plasmons, as well as the interaction between them accounts for such a high transmission. The interaction of magnetic plasmons and surface plasmons leads to new hybrid modes, and the coupled oscillator model is introduced to analyze this hybridization. This work extends the application range of higher order magnetic plasmons and may have potential in transparent electrode and electromagnetic energy transfer applications.     

Negative and Positive Impact of Roughness and Loss on Subwavelength Imaging for Superlens Structures

We study on the negative and positive effect of surface roughness and loss coefficient on subwavelength imaging of the superlens structure. It has been found that even though surface roughness enables more transmission of high spatial frequency components, the random interferential noise between neighborhood images becomes more severe with increasing distortion. We show that additional loss is able to restrain the interferential noise caused by random roughness while preserving the imaging integrity. The results with practical parameters prove that the mean contrast and uniformity are improved by adding adequate loss on rough surface. Moreover, other two situations are further studied: (a) a single superlens with roughness on different interfaces and (b) a multilayered alternated metal–dielectric superlens with roughness on each surface. We found that the roughness on the imaging surface (metal–photoresist interface) plays a major role in determining the superlens imaging. The multilayer superlens is able to enhance the subwavelength imaging with fractionalized thinner films. But with the further fractionizing layers, the multilayer becomes more vulnerable to the roughness due to the multiple mixing and distorting. We still prove that additional loss is able to improve the performance in both situations.     

Localized Surface Plasmon Enhanced Organic Light-Emitting Diodes

Current work demonstrates enhanced efficiencies in organic light-emitting diodes by using the localized surface plasmons originated from Au nanoclusters deposited using thermal evaporation technique. The effect of localized surface plasmons on organic emitter was studied using UV–vis absorption spectra, steady state and time-resolved photoluminescence spectra. These studies have revealed that the optical properties like absorption, emission have been greatly modified by the localized surface plasmon. These effects were found to be dependent on the distance between the emitter and Au layer. Further, efficiencies of the OLEDs were also found to be dependent on this distance.     

Multiple Surface Plasmon Resonances in Compound Structure with Metallic Nanoparticle and Nanohole Arrays

The optical properties of a compound structure with metallic nanoparticle and nanohole arrays are numerically investigated by the means of finite-difference time domain method. We report on the observation of multi-valleys in the reflection spectra due to the excitation of surface plasmon (SP) resonant modes of the compound structure. Simulation results show that multiple SP resonances consist of surface plasmon polaritons on the gold film, localized surface plasmons on the nanoparticles, and coupling mode between them. These findings are important for applications utilizing multiple surface plasmon resonances.