Sharp Resonance Features Research Articles

Effects of the coupling of dielectric spherical particles on signatures in infrared microspectroscopy

Infrared microspectroscopy is a powerful tool in the analysis of biological samples. However, strong electromagnetic scattering may occur since the wavelength of the incident radiation and the samples may be of comparable size. Based on the Mie theory of single spheres, correction algorithms have been developed to retrieve pure absorbance spectra. Studies of the scattering characteristics of samples of different types, obtained by microspectroscopy, have been performed. However, the detailed, microscopic effects of the coupling of the samples on signatures in spectra, obtained by infrared microspectroscopy, are still not clear. The aim of this paper is to investigate how the coupling of spherical samples influences the spectra. Applying the surface integral equation (SIE) method, we simulate small dielectric spheres, arranged as double-spheres or small arrays of spheres. We find that the coupling of the spheres hardly influences the broad oscillations observed in infrared spectra (the Mie wiggles) unless the radii of the spheres are different or the angle between the direction of the incident radiation and the normal of the plane where the spheres are located is large. Sharp resonance features in the spectra (the Mie ripples) are affected by the coupling of the spheres and this effect depends on the polarization of the incident wave. Experiments are performed to verify our conclusions.

Tuning Collective Plasmon Resonances of Femtosecond Laser-Printed Metasurface.

The optical response of properly excited periodically arranged plasmonic nanostructures is known to demonstrate sharp resonance features associated with high-Q collective modes demanding for various applications in light–matter interaction, filtering and sensing. Meanwhile, practical realization and replication of plasmonic platforms supporting high-Q modes via scalable inexpensive lithography-free approach is still challenging. Here, we justify direct ablation-free irradiation of Si-supported thin Au film by nanojoule-energy femtosecond laser pulses as a single-step and scalable technology for realization of plasmonic metasurfaces supporting collective plasmonic response. Using an adjustable aperture to control and upscale the size of the fabricated nanostructures, nanobumps and nanojets, we demonstrated plasmonic metasurface supporting collective resonances with a moderately high Q-factor (up to 17) and amplitude (up to 45%) within expanded spectral range (1.4–4.5 µm). Vacuum deposition of thin films above the as-fabricated nanostructure arrays was demonstrated to provide fine tuning of the resonance position, also expanding the choice of available materials for realization of plasmonic designs with extended functionality.

Full-color enhanced second harmonic generation using rainbow trapping in ultrathin hyperbolic metamaterials

Metasurfaces have provided a promising approach to enhance the nonlinearity at subwavelength scale, but usually suffer from a narrow bandwidth as imposed by sharp resonant features. Here, we counterintuitively report a broadband, enhanced second-harmonic generation, in nanopatterned hyperbolic metamaterials. The nanopatterning allows the direct access of the mode with large momentum, rendering the rainbow light trapping, i.e. slow light in a broad frequency, and thus enhancing the local field intensity for boosted nonlinear light-matter interactions. For a proof-of-concept demonstration, we fabricated a nanostructured Au/ZnO multilayer, and enhanced second harmonic generation can be observed within the visible wavelength range (400-650 nm). The enhancement factor is over 50 within the wavelength range of 470-650 nm, and a maximum conversion efficiency of 1.13×10−6 is obtained with a pump power of only 8.80 mW. Our results herein offer an effective and robust approach towards the broadband metasurface-based nonlinear devices for various important technologies.

Singular angular magnetoresistance and sharp resonant features in a high-mobility metal with open orbits, ReO3

The oxide ReO3 is one of the most conductive materials known. At 4 Kelvin, its resistivity is 6-10 times lower than that in high-purity gold and the electronic mean free path is 25 microns. It has an open Fermi surface comprised of intersecting cylinders. When an external magnetic field is applied, it exhibits a huge magnetoresistance with a highly singular angular dependence. Tilting the field in the longitudinal plane leads to a sharp decrease in the resistivity whereas tilting in the perpendicular direction sharply increases it. The authors analyze the experimental data using the Shockley-Chambers tube integral, showing that slight tilts lead to the obstruction of closed orbits on the Fermi surface which re-attach to form open orbits. The associated shadowing effect leads to a new way to measure the Fermi wavevector. However, the tube integral approach does not account for very narrow peaks observed at small tilt angles.

Effects of defects and surface roughness on high-Q modes in ZnO microspheres

Photoluminescence (PL) spectra of high-Q ZnO microspheres of various degrees of inhomogeneity are studied. Multiple sharp resonance features with distinct patterns associated with whispering gallery modes (WGM) of these microspheres are observed. Relative WGM peak strengths in these PL spectra are found to be closely related to defects and the surface roughness of the microspheres. A theoretical model based on Mie theory and Green’s function method is used to simulate the optical emission spectra of these microspheres. The effects of defects and surface roughness can be characterized by a frequency-dependent external quality factor (Q ex ) with a prefactor. By adjusting the prefactor in Q ex and a parameter describing the contribution of stimulated emission in the PL spectra, we can fit the observed PL spectra well. Through this study, we gain a better understanding of the relation between the diffusive scattering and the lineshapes of spectral features in PL.

Photoionization and photofragmentation of singly charged positive and negative Sc3N@C80 endohedral fullerene ions

Author(s): Muller, A; Martins, M; Kilcoyne, ALD; Phaneuf, RA; Hellhund, J; Borovik, A; Holste, K; Bari, S; Buhr, T; Klumpp, S; Perry-Sassmannshausen, A; Reinwardt, S; Ricz, S; Schubert, K; Schippers, S | Abstract: Photoprocesses of the endohedral fullerene ions Sc3N@C80+ and Sc3N@C80- in the gas phase have been investigated in the photon energy ranges 30-50 eV and 280-420 eV. Single and double ionization as well as single ionization accompanied by the release of a C2 dimer were observed as a function of the photon energy for the positive parent ion and double detachment was measured for the negative parent ion. The emphasis of the experiments was on the specific effects of the encapsulated trimetallic nitride cluster Sc3N on the observed reactions. Clear evidence of photoexcitation near the Sc L edge is obtained with the dominating contributions visible in the one- and two-electron-removal channels. K-vacancy production in the encapsulated central nitrogen atom is seen in the single ionization of Sc3N@C80+ but is much less pronounced in the photoionization-with-fragmentation channel. Comparison of the cross sections near the carbon K edge with the corresponding channels measured previously in the photoionization of Lu3N@C80+ reveal strong similarities. Previously predicted sharp resonance features in the ionization of Sc3N@C80+ ions below the Sc M edge are not confirmed. The experiments are accompanied by quantum-chemistry calculations in the Hartree-Fock approximation and by model calculations employing density functional theory (DFT).

Bound states in the continuum and high-Q resonances supported by a dielectric ridge on a slab waveguide

We investigate the diffraction of guided modes of a dielectric slab waveguide on a simple integrated structure consisting of a single dielectric ridge on the surface of the waveguide. Numerical simulations based on aperiodic rigorous coupled-wave analysis demonstrate the existence of sharp resonant features and bound states in the continuum (BICs) in the reflectance and the transmittance spectra occurring at oblique incidence of a TE-polarized guided mode on the ridge. Using the effective index method, we explain the resonances by the excitation of the cross-polarized modes of the ridge. The formation of the BICs is confirmed using a theoretical model based on the coupled-wave theory. The model suggests that the BICs occur due to coupling of quasi-TE and quasi-TM modes of the structure. Simple analytical expressions for the angle of incidence and the ridge width predicting the location of the BICs are obtained. The existence of high-Q resonances and BICs makes the considered integrated structure promising for filtering, sensing, transformation of optical signals, and enhancing nonlinear light-matter interactions.

High-Q resonances supported by a single dielectric ridge on the surface of a slab waveguide

Diffraction of slab waveguide modes on a dielectric ridge located on the waveguide surface is studied. Calculations, based on aperiodic rigorous coupled-wave analysis, demonstrate the existence of sharp resonant features in the reflectance and the transmittance spectra occurring at oblique incidence of TE-polarized waveguide mode on the ridge. Angular widths of the resonant peaks and dips vary from units to less than a thousandth of a degree. Using the effective index method, we explain the resonances by the excitation of cross-polarized modes of the ridge. The existence of high-Q resonances makes this structure promising for filtering, sensing and all-optical signal processing.

A New Method for Quantifying SWCNT Dispersion Quality from Absorption Spectra

Individualization of single-walled carbon nanotubes (SWCNTs) in aqueous surfactant dispersions can vary greatly. We will present a new method for quantitatively assessing dispersion quality based on simple absorption spectra. In this method, the visible and short-wave infrared portions of a sample’s absorption spectrum are modeled as a superposition of two components. One component (labeled “S”) has sharp resonant features and is associated with the subpopulation of SWCNTs that are suspended as individuals or very small aggregates; the other (labeled “B”) has broad absorption features and is associated with stably dispersed materials such as carbonaceous impurities, imperfect nanotubes, and larger aggregates. Using absorption spectra from samples in various stages of purification by centrifugation or magnetic processing, we apply the method of multivariate curve resolution to extract the S and B component spectra and determine their relative contributions in samples of interest. The ratio of S to B content then provides a simple index of dispersion quality. We illustrate this new characterization method with measurements on both shear-dispersed and tip-sonicated SWCNT samples purified by three different processes: centrifugation, ultracentrifugation, and magnetic purification. We determine the dispersion efficiency of each sample preparation and find results that correlate well with those of established analytical techniques. In addition, we have further characterized the effects of these purification processes on the SWCNT length distribution (using the diffusion-based LAND method) and on SWCNT emissive properties (through variance spectroscopy). We believe that our new absorption-based method provides a practical tool for quickly assessing the dispersion quality of SWCNT samples.

Resonance Raman signature of intertube excitons in compositionally-defined carbon nanotube bundles

Electronic interactions in low-dimensional nanomaterial heterostructures can lead to novel optical responses arising from exciton delocalization over the constituent materials. Similar phenomena have been suggested to arise between closely interacting semiconducting carbon nanotubes of identical structure. Such behavior in carbon nanotubes has potential to generate new exciton physics, impact exciton transport mechanisms in nanotube networks, and place nanotubes as one-dimensional models for such behaviors in systems of higher dimensionality. Here we use resonance Raman spectroscopy to probe intertube interactions in (6,5) chirality-enriched bundles. Raman excitation profiles for the radial breathing mode and G-mode display a previously unobserved sharp resonance feature. We show the feature is evidence for creation of intertube excitons and is identified as a Fano resonance arising from the interaction between intratube and intertube excitons. The universality of the model suggests that similar Raman excitation profile features may be observed for interlayer exciton resonances in 2D multilayered systems.

Dark plasmonic modes in diatomic gratings for plasmoelectronics

AbstractOwing to the unique ability of nanostructured metals to confine and enhance light waves along metal‐dielectric interfaces, plasmonics has enabled unprecedented flexibility in manipulating light at the deep‐subwavelength scale. With regard to the spectral behavior of plasmonic resonances, the spectral location of a resonance can be tailored with relative ease while the control over the spectral linewidth represents a more daunting task. In this paper, we present sharp resonance features by introducing dark plasmonic modes in diatomic gratings. The induced asymmetry in the metallic structure facilitates the generation of a dark mode with significantly suppressed radiative loss leading to an ultra‐sharp spectral feature ∼5 nm wide. We further use this metallic structure as an optoelectronic platform for the transduction of light waves to electrical signals via a plasmoelectric effect. The light concentrating ability of dark plasmonic modes, in conjunction with the ultra‐sharp resonance feature at a relatively low loss offers a novel route to enhanced light‐matter interactions with high spectral sensitivity for diverse applications. image

Phonon assisted resonant tunneling and its phonons control

We observe a series of sharp resonant features in the tunnelling differential conductance of InAs quantum dots. We found that dissipative quantum tunnelling has a strong influence on the operation of nano-devices. Because of such tunnelling the current-voltage characteristics of tunnel contact created between atomic force microscope tip and a surface of InAs/GaAs quantum dots display many interesting peaks. We found that the number, position, and heights of these peaks are associated with the phonon modes involved. To describe the found effect we use a quasi-classical approximation. There the tunnelling current is related to a creation of a dilute instanton-anti-instanton gas. Our experimental data are well described with exactly solvable model where one charged particle is weakly interacting with two promoting phonon modes associated with external medium. We conclude that the characteristics of the tunnel nanoelectronic devices can thus be controlled by a proper choice of phonons existing in materials, which are involved.

Phonon-Assisted Resonant Tunneling of Electrons in Graphene-Boron Nitride Transistors.

We observe a series of sharp resonant features in the differential conductance of graphene-hexagonal boron nitride-graphene tunnel transistors over a wide range of bias voltages between 10 and 200mV. We attribute them to electron tunneling assisted by the emission of phonons of well-defined energy. The bias voltages at which they occur are insensitive to the applied gate voltage and hence independent of the carrier densities in the graphene electrodes, so plasmonic effects can be ruled out. The phonon energies corresponding to the resonances are compared with the lattice dispersion curves of graphene-boron nitride heterostructures and are close to peaks in the single phonon density of states.

The Fano Resonance in Symmetry Broken Terahertz Metamaterials

The spectral characteristic of a Fano resonance is a distinct and unique asymmetric line shape. It arises from the destructive interference between a bright continuum mode and a discrete dark mode. Metamaterials and plasmonics have facilitated the observation of Fano resonances in the realm of classical electrodynamics and have spurred intense interest to study and to exploit their peculiarities due their low loss and very sharp resonant features. Here, we survey the excitation of Fano resonance at terahertz frequencies by using asymmetric metamaterial structures. In particular, we discuss the high Q of Fano resonances, their sensitivity to the asymmetry parameter and potential applications. We believe that the manipulation of terahertz radiation by exploiting Fano resonances in terahertz metamaterials could usher in next-generation terahertz photonic devices for delay, storage, filtering, sensing, and nonlinear applications.

Photoemission band mapping with a tunable femtosecond source using nonequilibrium absorption resonances

The authors show that the tunability of a femtosecond optical parametric amplifier combined with its high-repetition rate and short pulses provide a powerful tool for an alternate approach to conventional nonresonant band mapping by two-photon photoemission (2PPE). The authors demonstrate this 2PPE mapping via use of two model systems, i.e., the pair of sp surface and image states on flat Cu(111) and vicinal Cu(775) surfaces, over a photon energy range of 3.9–4.6 eV by making use of direct resonant band-to-band electronic transitions. Since the experimental excitation of the Cu image state from the surface state is comparable in time to the electron-electron equilibration time, the authors measure sharp resonant features in the electron energy distributions. In this approach, the authors track these resonant electronic transitions using 2PPE by varying the photon energy so as to achieve resonant excitation at each value of photoelectron emission angle over a large wavelength range on both types of surfaces. In addition, the authors explore the range of photon energies and optical intensities which may be used for this approach. The repetition rate of this laser was sufficient to yield a good signal-to-noise ratio while maintaining pump pulse intensities at levels that were low enough to prevent significant photon-induced space-charge broadening and electron-kinetic-energy shifting, even for photon energies close to the work function of the sample.

Metallic Adhesion Layer Induced Plasmon Damping and Molecular Linker as a Nondamping Alternative

Drastic chemical interface plasmon damping is induced by the ultrathin (∼2 nm) titanium (Ti) adhesion layer; alternatively, molecular adhesion is implemented for lithographic fabrication of plasmonic nanostructures without significant distortion of the plasmonic characteristics. As determined from the homogeneous linewidth of the resonance scattering spectrum of individual gold nanorods, an ultrathin Ti layer reduces the plasmon dephasing time significantly, and it reduces the plasmon scattering amplitude drastically. The increased damping rate and decreased plasmon amplitude are due to the dissipative dielectric function of Ti and the chemical interface plasmon damping where the conduction electrons are transferred across the metal-metal interface. In addition, a pronounced red shift due to the Ti adhesion layer, more than predicted using electromagnetic simulation, suggests the prevalence of interfacial reactions. By extending the experiment to conductively coupled ring-rod nanostructures, it is shown that a sharp Fano-like resonance feature is smeared out due to the Ti layer. Alternatively, vapor deposition of (3-mercaptopropyl)trimethoxysilane on gently cleaned and activated lithographic patterns functionalizes the glass surface sufficiently to link the gold nanostructures to the surface by sulfur-gold chemical bonds without observable plasmon damping effects.

Recombination of Au20+ at low electron–ion collision energies

The rate coefficient for the recombination of Au20+ with free electrons was measured in the electron–ion collision energy range of 0–10 eV by employing the electron–ion merged-beams technique at the heavy-ion storage ring TSR of the Max-Planck-Institute for Nuclear Physics in Heidelberg, Germany. In contrast to earlier measurements with more highly charged Au25+ (Hoffknecht et al 1998 J. Phys. B: At. Mol. Opt. Phys.31 2415), sharp dielectric recombination resonance features are observed.

Active Terahertz Nanoantennas Based on VO2 Phase Transition

Unusual performances of metamaterials such as negative index of refraction, memory effect, and cloaking originate from the resonance features of the metallic composite atom(1-6). Indeed, control of metamaterial properties by changing dielectric environments of thin films below the metallic resonators has been demonstrated(7-11). However, the dynamic control ranges are still limited to less than a factor of 10,(7-11) with the applicable bandwidth defined by the sharp resonance features. Here, we present ultra-broad-band metamaterial thin film with colossal dynamic control range, fulfilling present day research demands. Hybridized with thin VO(2) (vanadium dioxide) (12-18) films, nanoresonator supercell arrays designed for one decade of spectral width in terahertz frequency region show an unprecedented extinction ratio of over 10000 when the underlying thin film experiences a phase transition. Our nanoresonator approach realizes the full potential of the thin film technology for long wavelength applications.

Dependence of guided resonances on the structural parameters of terahertz photonic crystal slabs

Using terahertz spectroscopy, we measure the normal-incidence transmission coefficient of photonic crystals consisting of a periodic lattice of air holes in a silicon slab. Sharp resonant features are observed in the transmission spectra due to coupling of the leaky photonic crystal modes, called guided resonances, to the continuum of free-space modes. The resonances show considerable sensitivity to the structural parameters of the slab, including the slab thickness. By varying each crystal parameter systematically, we study the dependence of the resonances on the geometry of the photonic crystal slabs. Even small changes in a parameter such as the slab thickness, for example, can lead to dramatic changes in the optical spectrum. We also compare the transmission spectrum of a photonic crystal slab with a hexagonal lattice to that of a slab with a square lattice. In most cases, the experimental results match very well with numerical simulations based on the finite element method.

Nanoscale porous silicon waveguide for label-free DNA sensing

Porous silicon (PSi) is an excellent material for biosensing due to its large surface area and its capability for molecular size selectivity. In this work, we report the experimental demonstration of a label-free nanoscale PSi resonant waveguide biosensor. The PSi waveguide consists of pores with an average diameter of 20nm. DNA is attached inside the pores using standard amino-silane and glutaraldehyde chemistry. Molecular binding in the PSi is detected optically based on a shift of the waveguide resonance angle. The magnitude of the resonance shift is directly related to the quantity of biomolecules attached to the pore walls. The PSi waveguide sensor can selectively discriminate between complementary and non-complementary DNA. The advantages of the PSi waveguide biosensor include strong field confinement and a sharp resonance feature, which allow for high sensitivity measurements with a low detection limit. Simulations indicate that the sensor has a detection limit of 50nM DNA concentration or equivalently, 5pg/mm2.