Macro-scale transport of the excitation energy along a metal nanotrack: exciton-plasmon energy transfer mechanism
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Igor Khmelinskii↗
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Cytometer on a Chip
A cytometer now under development exploits spatial sorting of sampled cells on a microarray chip followed by use of grating-coupled surface-plasmon-resonance imaging (GCSPRI) to detect the sorted cells. This cytometer on a chip is a prototype of contemplated future miniature cytometers that would be suitable for rapidly identifying pathogens and other cells of interest in both field and laboratory applications and that would be attractive as alternatives to conventional flow cytometers. The basic principle of operation of a conventional flow cytometer requires fluorescent labeling of sampled cells, stringent optical alignment of a laser beam with a narrow orifice, and flow of the cells through the orifice, which is subject to clogging. In contrast, the principle of operation of the present cytometer on a chip does not require fluorescent labeling of cells, stringent optical alignment, or flow through a narrow orifice. The basic principle of operation of the cytometer on a chip also reduces the complexity, mass, and power of the associated laser and detection systems, relative to those needed in conventional flow cytometry. Instead of making cells flow in single file through a narrow flow orifice for sequential interrogation as in conventional flow cytometry, a liquid containing suspended sampled cells is made to flow over the front surface of a microarray chip on which there are many capture spots. Each capture spot is coated with a thin (.50-nm) layer of gold that is, in turn, coated with antibodies that bind to cell-surface molecules characteristic of the cell species of interest. The multiplicity of capture spots makes it possible to perform rapid, massively parallel analysis of a large cell population. The binding of cells to each capture spot gives rise to a minute change in the index of refraction at the surface of the chip. This change in the index of refraction is what is sensed in GCSPRI, as described briefly below. The identities of the various species in a sample of cells is spatially encoded in the chip by the pattern of capture spots. The number of cells of a particular species is determined from the magnitude of the GCSPRI signal from that spot. GCSPRI as used here can be summarized as follows: The cytometer chip is fabricated with a diffraction grating on its front surface. The chip is illuminated with a light emitting diode (LED) from the front. By proper choice of grating parameters and of the wavelength and the angle of incidence of a laser beam, laser light can be made to be coupled into an electromagnetic mode that resonates with surface plasmons and thus couples light into surface plasmons. Coupling of light into a surface plasmon at a given location reduces the amount of incident light reflected from that location. A change in the index of refraction at the surface of a capture spot gives rise to a change in the resonance condition. Depending on the specific design, the change in the index of refraction could manifest itself as a brightening or darkening, a change in the wavelength needed to excite the plasmon at a given angle of incidence, or a change in the angle of incidence needed to excite the plasmon at a given wavelength. Whereas a multiwavelength laser system with multichannel detection would be needed to detect multiple species in conventional flow cytometry, it suffices to use an LED and a single detector channel in the GCSPRI approach: this contributes significantly to reductions in cost, complexity, size, mass, and power. GCSPRI cytometer chips could be made of plastic and could be mass-produced cheaply by use of molding and other methods adopted from the manufacture of digital video disks. These methods are amenable to a high degree of miniaturization: such additional features as fluidic channels, reaction chambers, and fluid-coupling ports could readily be incorporated into the chips, without incurring substantial additional costs.
Fernandez, Salvador M.↗
Cytometer on a Chip
A cytometer now under development exploits spatial sorting of sampled cells on a microarray chip followed by use of grating-coupled surface-plasmon-resonance imaging (GCSPRI) to detect the sorted cells. This cytometer on a chip is a prototype of contemplated future miniature cytometers that would be suitable for rapidly identifying pathogens and other cells of interest in both field and laboratory applications and that would be attractive as alternatives to conventional flow cytometers. The basic principle of operation of a conventional flow cytometer requires fluorescent labeling of sampled cells, stringent optical alignment of a laser beam with a narrow orifice, and flow of the cells through the orifice, which is subject to clogging. In contrast, the principle of operation of the present cytometer on a chip does not require fluorescent labeling of cells, stringent optical alignment, or flow through a narrow orifice. The basic principle of operation of the cytometer on a chip also reduces the complexity, mass, and power of the associated laser and detection systems, relative to those needed in conventional flow cytometry. Instead of making cells flow in single file through a narrow flow orifice for sequential interrogation as in conventional flow cytometry, a liquid containing suspended sampled cells is made to flow over the front surface of a microarray chip on which there are many capture spots. Each capture spot is coated with a thin (approximately 50-nm) layer of gold that is, in turn, coated with antibodies that bind to cell-surface molecules characteristic of one the cell species of interest. The multiplicity of capture spots makes it possible to perform rapid, massively parallel analysis of a large cell population. The binding of cells to each capture spot gives rise to a minute change in the index of refraction at the surface of the chip. This change in the index of refraction is what is sensed in GCSPRI, as described briefly below. The identities of the various species in a sample of cells is spatially encoded in the chip by the pattern of capture spots. The number of cells of a particular species is determined from the magnitude of the GCSPRI signal from that spot. GCSPRI as used here can be summarized as follows: The cytometer chip is fabricated with a diffraction grating on its front surface. The chip is illuminated with a light emitting diode (LED) from the front. By proper choice of grating parameters and of the wavelength and the angle of incidence of a laser beam, laser light can be made to be coupled into an electromagnetic mode that resonates with surface plasmons and thus couples light into surface plasmons. Coupling of light into a surface plasmon at a given location reduces the amount of incident light reflected from that location. A change in the index of refraction at the surface of a capture spot gives rise to a change in the resonance condition. Depending on the specific design, the change in the index of refraction could manifest itself as a brightening or darkening, a change in the wavelength needed to excite the plasmon at a given angle of incidence, or a change in the angle of incidence needed to excite the plasmon at a given wavelength. Whereas a multiwavelength laser system with multichannel detection would be needed to detect multiple species in conventional flow cytometry, it suffices to use an LED and a single detector channel in the GCSPRI approach: this contributes significantly to reductions in cost, complexity, size, mass, and power. GCSPRI cytometer chips could be made of plastic and could be mass-produced cheaply by use of molding and other methods adopted from the manufacture of digital video disks. These methods are amenable to a high degree of miniaturization: such additional features as fluidic channels, reaction chambers, and fluid-coupling ports could readily be incorporated into the chips, without incurring substantial additional costs.
Fernandez, Salvador M.↗
Inelastic tunnel diodes
Power is extracted from plasmons, photons, or other guided electromagnetic waves at infrared to midultraviolet frequencies by inelastic tunneling in metal-insulator-semiconductor-metal diodes. Inelastic tunneling produces power by absorbing plasmons to pump electrons to higher potential. Specifically, an electron from a semiconductor layer absorbs a plasmon and simultaneously tunnels across an insulator into metal layer which is at higher potential. The diode voltage determines the fraction of energy extracted from the plasmons; any excess is lost to heat.
Anderson, L. M.↗
The theory of ionospheric focused heating
Ionospheric modification by high power radio waves and by chemical releases are combined in a theoretical study of ionospheric focused heating. The release of materials which promote electron-ion recombination creates a hole in the bottomside ionosphere. The ionospheric hole focuses high power radio waves from a ground-based transmitter to give a 20 dB or greater enhancement in power density. The intense radio beam excites atomic oxygen by collisions with accelerated electrons. Airglow from the excited oxygen provides a visible trace of the focused beam. The large increase in the intensity of the radio beam stimulates new wave-plasma interactions. Numerical simulations show that the threshold for the two-plasmon decay instability is exceeded. The interaction of the pump electromagnetic wave with the backward plasmon produces a scattered electromagnetic wave at 3/2 the pump frequency. The scattered wave provides a unique signature of the two-plasmon decay process for ground-based detection.
Bernhardt, P. A.↗
Metal Nanoparticle Aerogel Composites
We have fabricated sol-gels containing gold and silver nanoparticles. Formation of an aerogel produces a blue shift in the surface plasmon resonance as a result of the decrease in the dielectric constant of the matrix upon supercritical extraction of the solvent. However, as a result of chemical interface damping this blue shift does not obey effective medium theories. Annealing the samples in a reducing atmosphere at 400 C eliminates this discrepancy and results in narrowing and further blue shifting of the plasmon resonance. Metal particle aggregation also results in a deviation from the predictions of effective medium theories, but can be controlled through careful handling and by avoiding the use of alcohol. By applying effective medium theories to the heterogeneous interlayer surrounding each metal particle, we extend the technique of immersion spectroscopy to inhomogeneous materials characterized by spatially dependent dielectric constants, such as aerogels. We demonstrate that the shift in the surface plasmon wavelength provides the average fractional composition of each component (air and silica) in this inhomogeneous layer, i.e. the porosity of the aerogel or equivalently, for these materials, the catalytic dispersion. Additionally, the kinetics suggest that collective particle interactions in coagulated metal clusters are perturbed during silica gelation resulting in a change in the aggregate geometry.
Smith, David D.↗
Nanostructures Exploit Hybrid-Polariton Resonances
Nanostructured devices that exploit the hybrid-polariton resonances arising from coupling among photons, phonons, and plasmons are subjects of research directed toward the development of infrared-spectroscopic sensors for measuring extremely small quantities of molecules of interest. The spectroscopic techniques in question are surface enhanced Raman scattering (SERS) and surface enhanced infrared absorption (SEIRA). An important intermediate goal of this research is to increase the sensitivity achievable by these techniques. The basic idea of the approach being followed in this research is to engineer nanostructured devices and thereby engineer their hybrid-polariton resonances to concentrate infrared radiation incident upon their surfaces in such a manner as to increase the absorption of the radiation for SEIRA and measure the frequency shifts of surface vibrational modes. The underlying hybrid-polariton-resonance concept is best described by reference to experimental devices that have been built and tested to demonstrate the concept. The nanostructure of each such device includes a matrix of silicon carbide particles of approximately 1 micron in diameter that are supported on a potassium bromide (KBr) or poly(tetrafluoroethylene) [PTFE] window. These grains are sputter-coated with gold grains of 40-nm size (see figure). From the perspective of classical electrodynamics, in this nanostructure, that includes a particulate or otherwise rough surface, the electric-field portion of an incident electromagnetic field becomes concentrated on the particles when optical resonance conditions are met. Going beyond the perspective of classical electrodynamics, it can be seen that when the resonance frequencies of surface phonons and surface plasmons overlap, the coupling of the resonances gives rise to an enhanced radiation-absorption or -scattering mechanism. The sizes, shapes, and aggregation of the particles determine the frequencies of the resonances. Hence, the task of designing a nanostructure to exhibit the desired radiation-absorption properties translates, in large part, to selecting particle sizes and shapes to obtain the desired enhanced coupling of energy from photons to plasmons and phonons. To broaden the spectral region(s) of enhanced absorption, one would select a distribution of particle sizes and shapes.
Anderson, Mark↗
Nanostructure Diffraction Gratings for Integrated Spectroscopy and Sensing
The present disclosure pertains to metal or dielectric nanostructures of the subwavelength scale within the grating lines of optical diffraction gratings. The nanostructures have surface plasmon resonances or non-plasmon optical resonances. A linear photodetector array is used to capture the resonance spectra from one of the diffraction orders. The combined nanostructure super-grating and photodetector array eliminates the use of external optical spectrometers for measuring surface plasmon or optical resonance frequency shift caused by the presence of chemical and biological agents. The nanostructure super-gratings can be used for building integrated surface enhanced Raman scattering (SERS) spectrometers. The nanostructures within the diffraction grating lines enhance Raman scattering signal light while the diffraction grating pattern of the nanostructures diffracts Raman scattering light to different directions of propagation according to their wavelengths. Therefore, the nanostructure super-gratings allows for the use of a photodetector array to capture the surface enhanced Raman scattering spectra.
Guo, Junpeng↗
Nanostructure Diffraction Gratings for Integrated Spectroscopy and Sensing
The present disclosure pertains to metal or dielectric nanostructures of the subwavelength scale within the grating lines of optical diffraction gratings. The nanostructures have surface plasmon resonances or non-plasmon optical resonances. A linear photodetector array is used to capture the resonance spectra from one of the diffraction orders. The combined nanostructure super-grating and photodetector array eliminates the use of external optical spectrometers for measuring surface plasmon or optical resonance frequency shift caused by the presence of chemical and biological agents. The nanostructure super-gratings can be used for building integrated surface enhanced Raman scattering (SERS) spectrometers. The nanostructures within the diffraction grating lines enhance Raman scattering signal light while the diffraction grating pattern of the nanostructures diffracts Raman scattering light to different directions of propagation according to their wavelengths. Therefore, the nanostructure super-gratings allows for the use of a photodetector array to capture the surface enhanced Raman scattering spectra.
Guo, Junpeng↗
Polarization-Controlled Directional Multiphoton Photoemission from Hot Spots on Single Au Nanoshells
Directional photoemission from single Au nanoshells is demonstrated in the low-intensity, multiphoton regime. Thisdirectionality is shown to be due to the plasmonic excitation of highly photoemissive, nanometer scale surface regions, which are characterized by correlated momentum mapping, scanning electron microscopy (SEM), and laser polarization-dependence studies. Furthermore, the photoelectron flux from a single nanoshell can be systematically rotated by over 90° in momentum space simply by polarization-controlled coupling to different hot spots. Photoelectrondistributions are directly characterized in momentum space via velocity map imaging (VMI) of the two-dimensional transverse (px, py) momentum components for single nanoshells. For the majority of nanoshells studied, the photoemission is directionally orthogonal to the laser polarization, which implicates nanoscale crevice-shaped "hotspots" clearly observed in the correlated SEM/VMI studies, with the near-field plasmonic nature of these crevices clarified further via finite-element simulations. These results rationalize the large photoemission enhancements observed in previous Au nanoshell studies, but more importantly provide a novel experimental access to directionally tunable electron emission from nanoscale sources. The ability to control photoemission/photocurrent angular distributions at the nanoscale with only modest optical fields indicates a new parameter for optimizing nanoplasmonic system performance and suggests new plasmonic applications such as ultrafast, polarization-controlled photoelectric/photovoltaic switches.
Pettine, Jacob↗
Colorimetric and Label-Free Optical Detection of Pb 2+ Ions via Colloidal Gold Nanoparticles
The detection of Lead (Pb) heavy metal in water is crucial in many chemical processes as it is associated with serious health hazard. Here, we report the selective and precise colorimetric detection of Pb 2+ ions in water exploiting the mechanisms of aggregation and self-assembly of Glutathione (GSH) functionalized gold nanoparticles (GNPs). The carboxyl functional groups are available to create coordination complexes with Pb 2+ inducing aggregation amongst the GSH-GNPs in the presence of Pb 2+ due to the chelation of the GSH ligands. The resulting aggregation of amongst the GSHGNPs in the presence of Pb2+ increases the aggregate size depending on available Pb 2+ ions affecting the plasmonic coupling. This causes in a substantial shift in the plasmon wavelength to a longer wavelength side with increasing Pb 2+ concentration, resulting in a red-to-blue colorimetric or visual change, enabling instant determination of lead content in water.
calorimetric detection↗
Photoinduced currents in metal-barrier-metal junctions
The fabrication and application of metal-barrier-metal tunneling junctions for radiative interactions are discussed. Particular attention is given to the photolithographic fabrication of small area devices and the coupling to such devices via surface plasmon waves which play an important role at infrared and optical frequencies. It has been shown that the junction electron tunneling currents can be strongly coupled to surface plasmon junction modes, and spontaneous and stimulated emission of the latter are possible as well as nonlinear interactions. Finally, results demonstrating the photo-excitation of electrons with subsequent tunneling induced by ultraviolet radiation are presented. It is estimated that quantum efficiencies of the order of 5% and higher are possible in the ultraviolet region.
Guedes, M. P.↗
Surface-polaritonlike waves guided by thin, lossy metal films
Surface-plasmon polaritons guided by thin, lossy metallic films bounded by dissimilar dielectric media are investigated. New solutions to the dispersion relation are found, representing waves that are leaky (radiative) in one of the dielectrics. The new waves are interpreted in terms of the coupling of a damped surface plasmon at one interface with continuum modes at the other. Their excitation by end-fire coupling techniques is suggested.
Stegeman, G. I.↗
Coupling of radiation into thin film modes by means of localized plasma resonances
The interaction between the surface plasmon mode that propagates at a metal dielectric interface and the localized plasma resonances (LPR) is investigated experimentally in Ag-island films. A stair-stepped sample geometry comprising a glass substrate, a continuous 50-nm Ag film, an LiF spacer film of thickness d = 5-60 nm, and an Ag-island film of mass thickness 3 nm is used in near-normal-reflectivity and plasmon-propagation-constant (k) determinations. The results are presented graphically and discussed. The overall shape of the reflectivity curves is found to be characteristic of Ag films, but with a dip at about 400 nm (corresponding to the absorption resonance of the island film) which is most pronounced with d = 25 nm. It is inferred that the island resonances are strongly coupled to a continuous-film dissipative mechanism at this d value. This inference is supported by the fact that the variation in k, correctd for LiF effects and plotted as a function of d, is greatest at around d = 25 nm. The implications of this finding for broad-band coupling into a thin-film mode, LPR enhancement of waveguide nonlinear effects, and new surface-enhanced-Raman-scattering geometries are indicated.
Holland, W. R.↗
Solar energy converter using surface plasma waves
Sunlight is dispersed over a diffraction grating formed on the surface of a conducting film on a substrate. The angular dispersion controls the effective grating period so that a matching spectrum of surface plasmons is excited for parallel processing on the conducting film. The resulting surface plasmons carry energy to an array of inelastic tunnel diodes. This solar energy converter does not require different materials for each frequency band, and sunlight is directly converted to electricity in an efficient manner by extracting more energy from the more energetic photons.
Anderson, L. M.↗
Diffusion of Si in thin CoSi2 layers
Evidence of silicon diffusion in 100-A CoSi2 layers grown by room-temperature codeposition and annealing on Si(111) substrates was from Auger peak height ratios, which were interpreted in terms of a Si overlayer. It was found that this layer could be removed by chemical etching and reformed by subsequent annealing. By measuring the intensity of the plasmon energy loss peak associated with the CoL23 VV Auger peak, the effective thickness of the Si overlayer was measured as a function of annealing temperature, by calibrating the plasmon loss data against known overlayer thicknesses on unannealed samples. Similar results were found for samples grown both with and without the addition of a 10-A Si cap to prevent pinhole formation in the CoSi2; moreover, Si diffusion was also observed at temperatures well below the point where pinhole formation is first found, suggesting that Si diffusion does not depend on the presence of observable pinholes.
Schowengerdt, F. D.↗
Surface characterization of hydrogen charged and uncharged alpha-2 and gamma titanium aluminide alloys using AES and REELS
The surfaces of selected uncharged and hydrogen charged alpha-2 and gamma titanium aluminide alloys with Nb additions were characterized by Auger electron (AES) and reflected electron energy loss (REELS) spectroscopy. The alloy surfaces were cleaned before analysis at room temperature by ion sputtering. The low energy (500 eV) ion sputtering process preferentially sputtered the surface concentration. The surface concentrations were determined by comparing AES data from the alloys with corresponding data from elemental references. No differences were observed in the Ti or Nb Auger spectra for the uncharged and hydrogen charged alloys, even though the alpha-2 alloy had 33.4 atomic percent dissolved hydrogen. Also, no differences were observed in the AES spectra when hydrogen was adsorbed from the gas phase. Bulk plasmon energy shifts were observed in all alloys. The energy shifts were induced either by dissolved hydrogen (alpha-2 alloy) or hydrogen adsorbed from the gas phase (alpha-2 and gamma alloys). The adsorption induced plasmon energy shifts were greatest for the gamma alloy and cp-Ti metal.
Shanabarger, M. R.↗
Method of forming silicon structures with selectable optical characteristics
Silicon and metal are coevaporated onto a silicon substrate in a molecular beam epitaxy system with a larger than stoichiometric amount of silicon so as to epitaxially grow particles of metal silicide embedded in a matrix of single crystal epitaxially grown silicon. The particles interact with incident photons by resonant optical absorption at the surface plasmon resonance frequency. Controlling the substrate temperature and deposition rate and time allows the aspect ratio of the particles to be tailored to desired wavelength photons and polarizations. The plasmon energy may decay as excited charge carriers or phonons, either of which can be monitored to indicate the amount of incident radiation at the selected frequency and polarization.
Fathauer, Robert W.↗