High sensitivity plasmonic index sensor using slablike gold nanoring arrays

We investigate the index sensing characteristics of plasmonic arrays based on square lattice slablike gold nanorings (NRs) with different ring widths. The gold NR arrays exhibit two extinction peaks in the visible and near-infrared corresponding to antibonding and bonding modes. Redshift and blueshift in antibonding and bonding modes when broadening the average ring width are observed. We experimentally demonstrate the sensitivity of bonding mode can be tuned by varying the average ring width. High sensitivity of 691 nm per refractive index unit is obtained for NRs with 199 nm average ring width.     

Nanopin plasmonic resonator array and its optical properties

A one-step electron-beam lithography process for the fabrication of a high-aspect ratio nanopin array is presented. Each nanopin is a metal-capped dielectric pillar upon a ring-shaped metallic disc. Highly tunable optical properties and the electromagnetic interplay between the metallic components were studied by experiment and simulation. The two metallic pieces play asymmetrical roles in their coupling to each other due to their drastic size difference. The structure can lead to ultrasensitive surface-enhanced Raman scattering chemical sensor arrays, etc.     

Chiral metamaterial composed of three-dimensional plasmonic nanostructures

We introduce a top-down fabricated metamaterial composed of three-dimensional, chiral, plasmonic nanostructures for visible and near-infrared wavelengths. Based on a combined spectroscopic and interferometric characterization, the entire complex transmission response in terms of a Jones matrix is disclosed. Particularly, the polarization output state of light after propagation through the nanostructures can be decoded from the measurements for any excitation configuration. We experimentally found a rotation of the polarization azimuth of linearly polarized light exceeding 50° at wavelengths around 1.08 μm. This corresponds to a specific rotation which is significantly larger than that of any linear, passive, and reciprocal medium reported to date.     

Platinum plasmonic nanostructure arrays for massively parallel single-molecule detection based on enhanced fluorescence measurements

We fabricated platinum bowtie nanostructure arrays producing fluorescence enhancement and evaluated their performance using two-photon photoluminescence and single-molecule fluorescence measurements. A comprehensive selection of suitable materials was explored by electromagnetic simulation and Pt was chosen as the plasmonic material for visible light excitation near 500 nm, which is preferable for multicolor dye-labeling applications like DNA sequencing. The observation of bright photoluminescence (λ = 500-600 nm) from each Pt nanostructure, induced by irradiation at 800 nm with a femtosecond laser pulse, clearly indicates that a highly enhanced local field is created near the Pt nanostructure. The attachment of a single dye molecule was attempted between the Pt triangles of each nanostructure by using selective immobilization chemistry. The fluorescence intensities of the single dye molecule localized on the nanostructures were measured. A highly enhanced fluorescence, which was increased by a factor of 30, was observed. The two-photon photoluminescence intensity and fluorescence intensity showed qualitatively consistent gap size dependence. However, the average fluorescence enhancement factor was rather repressed even in the nanostructure with the smallest gap size compared to the large growth of photoluminescence. The variation of the position of the dye molecule attached to the nanostructure may influence the wide distribution of the fluorescence enhancement factor and cause the rather small average value of the fluorescence enhancement factor.     

Background-free three-dimensional selective imaging of anisotropic plasmonic nanoparticles

There is an increasing demand for advanced optical imaging techniques that can detect and resolve nanosize objects at a spatial resolution below the optical diffraction limit,especially in three-dimensional (3D) cellular environments.In this study,using a polarization-activated localization scheme based on the orientation-dependent properties of anisotropic plasmonic metal nanoparticles (MNPs),"photoswitchable" imaging of single gold nanorods (AuNRs) was accomplished not only in two dimensions but also in three dimensions.Moreover,the Rayleigh scattering background arising from the congested subcellular structures was efficiently suppressed.Thus,we obtained the 3D distributions of both the position and the orientation of the AuNRs inside the cells and investigated their internalization kinetics.To our knowledge,this is the first demonstration of the confocal-like 3D imaging of non-fluorescence nanoparticles with a high resolution and almost zero background.This technique is easy to implement and should greatly facilitate MNP studies and applications in biomedicine and biology.     

Trace detection of krypton using laser-induced fluorescence

Highly sensitive detection of neutral Kr atoms was accomplished by the use of laser-induced fluorescence. In one experiment, Kr at 40 parts per 10(12) in He was detected at a signal-to-noise ratio of 500 by time-resolved fluorescence measurements. The Kr metastable 1s(5) level was populated by cascade after two-photon excitation to the 2p(6) level by the frequency-tripled output of a pulsed single-longitudinalmode dye laser. After a delay, when scattered laser light and cascade resonance fluorescence became negligible, trace quantities of Kr were detected by the use of a pulsed-laser pumping scheme. In a related experiment, (78)Kr/(86)Kr isotope ratios ranging from 1 to 0.1 were measured with a resonant isotopic depletion technique first proposed by Makarov [Sov. J. Quantum Electron. 13, 722 (1983)]. The (86)Kr metastable population was selectively depleted by optical pumping to a higher-lying state that relaxed to the ground state by means of radiative cascade. After the (78)Kr/(86)Kr ratio of metastables had been enriched by a factor of 10, the (78)Kr population was probed by pulsed excitation. Premixed (78)Kr/(86)Kr ratios were measured to within an accuracy of 10%, even for unresolved, Doppler-broadened transitions.     

TNT detection using multiplexed liquid array displacement immunoassays

The presence of trace contamination of soil and groundwater with explosives is an ongoing concern, for which improved methods are required to facilitate their detection and quantification. This is true both for the monitoring of remediation and for site characterization. Immunosensors have been found effective for solution-phase detection of environmental contaminants. Our work utilized the Luminex100 (flow cytometer) to detect TNT in a multiplexed displacement immunoassay format. The Luminex100 can perform a multiplexed assay by discriminating between up to 100 different bead sets. We used this capability to evaluate four different TNT monoclonal antibodies, two recombinant TNT antibodies, and a control antibody simultaneously for the rapid detection of TNT and other nitroaromatics. TNT could be detected at 0.1 ppb and quantified over the range of 1.0 ppb to 10 ppm. In addition, the assay was shown to be effective in various matrixes such as lake water, seawater, and acetone extracts of soil. Seawater required dilution with two parts buffer to avoid loss of microspheres, while the acetone extracts were diluted 100-fold or more to minimize solvent affects.     

Average plasmonic enhancement of molecules-doped Au-NS@SiO2 on fluorescence

The average plasmonic enhancement of Au nanoshell (Au-NS) coated by a molecules-doped silica layer (Au-NS@SiO2) on molecular fluorescence is studied theoretically to estimate the overall performance of a large number of Au-NS@SiO2. Using Mie theory and dyadic Green's functions, analytical solutions of the excitation rate and the apparent quantum yield are obtained to calculate the enhancement factor of Au-NS@SiO2 on the fluorescence of a molecule with a specific orientation and location at a specific excitation wavelength lambda ex and an emission wavelength lambda em. Subsequently, the average enhancement factor (AEF) is calculated by averaging all possible orientations and locations of the molecule. For example, AEF of Au-NS@SiO2 (a3 = 50 nm t2 = 15 nm, t1 = 25 nm) is 4.544 for a NIR fluorescence at lambda ex = 780 nm and lambda em = 820 nm. Our results show that Au-NS is a broadband enhancer for NIR fluorescence; the bandwidth and the peak depend on the core size and the thickness of Au shell.     

Enzyme-free and amplified fluorescence DNA detection using bimolecular beacons

In this work, we propose a simple and enzyme-free strategy for sensitive and selective DNA detection by using two different types of molecular beacons (MBs), MB1 and MB2. In this method, the target DNA binds with and restores the fluorescence of MB1 first. Then, MB2 hybridizes with MB1 and free the target, which is used to trigger another reaction cycle. The cycling use of the target and the employment of bi-MBs amplify the fluorescence intensity for sensitive DNA detection. The detection limit of this method was obtained as 10 pM, which is about 2 orders of magnitude sensitive than the conventional MB-based approaches.     

Infrared microspectroscopy using prism-based spectrographs and focal plane array detection

Several prism-based spectrographs employing a mercury cadmium telluride (MCT) focal plane array detector have been interfaced to an infrared microscope. In the combined system, the area-defining aperture of the microscope also served as the entrance slit to the spectrograph. This investigation considered the fundamental limits of diffraction for both the spectrograph and microscope in order to determine both the spatial and spectral resolution of the system as a whole. Experimental results for spectral resolution, spectral range, and peak-to-peak noise have been presented. Finally, the dynamic capabilities of one spectrograph/microscope combination were investigated.     

Enhancement of optical processes in coupled plasmonic nanocavities [Invited

We present detailed experimental and numerical investigations of resonances in deep nanogroove gratings in metallic substrates. These plasmonic nanocavity gratings feature enhanced fields within the grooves that enable a large enhancement of linear and nonlinear optical processes. This enhancement relies on both localized and propagating surface plasmons on the nanopatterned surface. We show that the efficiency of optical processes such as Raman scattering and four-wave mixing is dramatically enhanced by plasmonic nanocavity gratings.     

Fabrication of discrete array of metallodielectric nanoshells and their surface plasmonic properties

In this paper we describe the fabrication of two-dimensionally periodic non-close-packed nanoshell arrays, consisting of a spherical polystyrene core coated with a thin gold shell, as well as their surface plasmonic properties. The principle of this procedure relies on stepwise integration of spin-coat-assisted colloidal self-assembly of the single layer of close-packed polystyrene nanoparticle, atmospheric pressure plasma-induced isotropic etching, and deposition of gold thin film by thermal evaporation. The plasma process converted the close-packed nanoparticle array into non-close-packed arrangement without changing their original spherical shape and periodicity. Both experimental and theoretical studies revealed that the densely packed nanoshell array with a 160 nm inner core diameter and a 20 nm thick shell strongly scattered and absorbed near infrared light, due to the interaction between primitive plasmon modes associated with the surface of the nanoparticle. Furthermore, the resultant nanoshell array was utilized for near infrared light responsible localized surface plasmon resonance based sensor. The bulk refractive index sensitivity was 220 nm RIU^− 1.     

通过模态滤波实现阵列式传感器系统的故障诊断

基于结构振动响应特性利用改进的模态滤波方法对阵列式传感器系统进行故障诊断。在梁结构表面均匀布置一组加速度计,利用模态振型对该系统的输出信号进行重构,将重构信号与实际信号之间的曲率误差作为敏感参数,对系统中的模拟故障传感器进行检测与识别,并加以实验验证。数值计算和实验结果表明:改进的模态滤波方法不仅可以直接有效地对传感器系统进行实时故障监测,而且该方法与外界激励力位置无关,具有良好的工程应用前景。     

Palladium bridged gold nanocylinder dimer: plasmonic properties and hydrogen sensitivity

Plasmonic nanodimers facilitate electromagnetic hotspots at their gap junction. By loading these gap junctions with nanomaterials, the plasmonic properties of nanodimer can be varied. In this study, we bridged the gap junction of gold (Au) nanocylinder dimer with palladium (Pd), and numerically evaluated the plasmonic properties of the designed nanostructure. We simulated the far-field extinction spectra of Pd bridged Au nanocylinder dimer, and identified the dipole and quadrupole plasmon modes at 839 and 578 nm, respectively. By varying the geometrical parameters of the Pd bridge, we revealed the ability to tune the dipolar plasmon resonance of the bridged dimer. Further, we exploited the hydrogen sensitivity of Pd bridge to harness the bridged-Au dimer as nanoplasmonic hydrogen sensor. Such nano-optical detection platforms have minimal spatial footprint and can be further harnessed for chip-based plasmonic sensing.     

Element-specific detection in capillary electrophoresis using X-ray fluorescence spectroscopy

X-ray fluorescence spectroscopy is demonstrated here as a novel, element-specific detector for capillary electrophoresis. Monochromatic 10 keV X-rays from a synchrotron light source are used to excite core electrons, causing emission of characteristic Kalpha X-ray fluorescence (XRF) lines. Using this technique, XRF energies provide elemental identification, while XRF intensities can be used to quantitate the metal composition of each eluent. An X-ray transparent polymer coupling is used to create a window for the on-line, X-ray detection. This coupling contributes no measurable extra-column variance, and electrophoretic mobilities for the metal complexes used as model solutes are highly reproducible. The combination of XRF detection with capillary electrophoresis (CE-XRF) creates the first on-line detection system that is element-specific, nondestructive, and directly applicable to a broad range of applications including nonelectroactive species. CE-XRF is successfully demonstrated here for high binding-constant complexes of Fe(III), Co(II), Cu(II), and Zn(II). Within a single injection, electropherograms are obtained for each element of interest, with the element identity obtained directly from the emission energy. In contrast with ICPMS, this detection technique is directly on-line and does not require volatilization of the eluent. As a result, element-specific detection is not limited by the sample or the buffer volatility or atomization efficiency. Simultaneous XRF and UV absorbance detection can be used to provide an on-line determination of metal/chelate ratios. Although XRF detection limits are presently only in the 0.1 mM (0.5 ng) range, both collection geometry and incident intensity have yet to be optimized. Further optimization is expected to enhance this detection limit by another 2-3 orders of magnitude. As a result, the advent of XRF detection combined with the separating power of CE presents new possibilities for on-line, element-specific analysis.     

Adjustable plasmonic resonances of a gold nanotube array with a non-coaxial core

The plasmonic resonant properties of a gold nanotube array with a non-coaxial core were investigated using the finite-difference time-domain (FDTD) method. There exist two large photonic band gaps in the transmission spectra for large core offset. It is observed that the plasmonic behaviors can also be tuned by the inter-tube spacing, the size and the thickness of the nanotube with a non-coaxial core in the metallic array structure. Based on the field distribution, we deduce that the lower energy peaks of the spectra are characterized by dipole resonances, while the higher energy peaks are characterized by multipolar resonances.     

Giant and uniform fluorescence enhancement over large areas using plasmonic nanodots in 3D resonant cavity nanoantenna by nanoimprinting

Using a new nanoplasmonic architecture and an optimized spacer, we observed the following: (a) the average fluorescence of an infrared dye (indocyanine green) is enhanced by?2970 fold uniformly (variation < 11%) over a large sample area and over a wide range of dye concentrations (380 to 380?000?molecule?μm(-2)), laser excitation powers and laser beam sizes; and (b) for a single molecule placed at a 'hot spot', the fluorescence enhancement is 4.5?×?10(6) fold. The giant and uniform enhancements (orders of magnitude higher than before), plus easy and inexpensive large area fabrication (?>?4″ wafers), should open up wide applications.     

Flow-through vs flow-over: analysis of transport and binding in nanohole array plasmonic biosensors

We quantify the efficacy of flow-through nanohole sensing, as compared to the established flow-over format, through scaling analysis and numerical simulation. Nanohole arrays represent a growing niche within surface plasmon resonance-based sensing methods, and employing the nanoholes as nanochannels can enhance transport and analytical response. The additional benefit offered by flow-through operation is, however, a complex function of operating parameters and application-specific binding chemistry. Compared here are flow-over sensors and flow-through nanohole array sensors with equivalent sensing area, where the nanohole array sensing area is taken as the inner-walls of the nanoholes. The footprints of the sensors are similar (e.g., a square 20 μm wide flow-over sensor has an equivalent sensing area as a square 30 μm wide array of 300 nm diameter nanoholes with 450 nm periodicity in a 100 nm thick gold film). Considering transport alone, an analysis here shows that given equivalent sensing area and flow rate the flow-through nanohole format enables greatly increased flux of analytes to the sensing surface (e.g., 40-fold for the case of Q = 10 nL/min). Including both transport and binding kinetics, a computational model, validated by experimental data, provides guidelines for performance as a function of binding time constant, analyte diffusivity, and running parameters. For common binding kinetics and analytes, flow-through nanohole arrays offer ～10-fold improvement in response time, with a maximum of 20-fold improvement for small biomolecules with rapid kinetics.     

Electric field tuning of plasmonic response of nanodot array in liquid crystal matrix

In this work we demonstrate the feasibility of electric-field tuning of the plasmonic spectrum of a novel gold nanodot array in a liquid crystal matrix. As opposed to previously reported microscopically observed near-field spectral tuning of individual gold nanoparticles, this system exhibits macroscopic far-field spectral tuning. The nanodot-liquid crystal matrix also displays strong anisotropic absorption characteristics, which can be effectively described as a collective ensemble within a composite matrix in the lateral dimension and a group of noninteracting individual particles in the normal direction. The effective medium model and the Mie theory are employed to describe the experimental results.