Showing papers on "Scattering published in 2006"

Calculated Absorption and Scattering Properties of Gold Nanoparticles of Different Size, Shape, and Composition: Applications in Biological Imaging and Biomedicine

Abstract: The selection of nanoparticles for achieving efficient contrast for biological and cell imaging applications, as well as for photothermal therapeutic applications, is based on the optical properties of the nanoparticles. We use Mie theory and discrete dipole approximation method to calculate absorption and scattering efficiencies and optical resonance wavelengths for three commonly used classes of nanoparticles: gold nanospheres, silica−gold nanoshells, and gold nanorods. The calculated spectra clearly reflect the well-known dependence of nanoparticle optical properties viz. the resonance wavelength, the extinction cross-section, and the ratio of scattering to absorption, on the nanoparticle dimensions. A systematic quantitative study of the various trends is presented. By increasing the size of gold nanospheres from 20 to 80 nm, the magnitude of extinction as well as the relative contribution of scattering to the extinction rapidly increases. Gold nanospheres in the size range commonly employed (∼40 nm)...

Gold and Silver Nanoparticles in Sensing and Imaging: Sensitivity of Plasmon Response to Size, Shape, and Metal Composition

Abstract: Plasmonic metal nanoparticles have great potential for chemical and biological sensor applications, due to their sensitive spectral response to the local environment of the nanoparticle surface and ease of monitoring the light signal due to their strong scattering or absorption. In this work, we investigated the dependence of the sensitivity of the surface plasmon resonance (frequency and bandwidth) response to changes in their surrounding environment and the relative contribution of optical scattering to the total extinction, on the size and shape of nanorods and the type of metal, that is, Au vs Ag. Theoretical consideration on the surface plasmon resonance condition revealed that the spectral sensitivity, defined as the relative shift in resonance wavelength with respect to the refractive index change of surrounding materials, has two controlling factors: first the bulk plasma wavelength, a property dependent on the metal type, and second on the aspect ratio of the nanorods which is a geometrical parameter. It is found that the sensitivity is linearly proportional to both these factors. To quantitatively examine the dependence of the spectral sensitivity on the nanorod metal composition and the aspect ratio, the discrete dipole approximation method was used for the calculation of optical spectra of Ag-Au alloy metal nanorods as a function of Ag concentration. It is observed that the sensitivity does not depend on the type of the metal but depends largely on the aspect ratio of nanorods. The direct dependence of the sensitivity on the aspect ratio becomes more prominent as the size of nanorods becomes larger. However, the use of larger nanoparticles may induce an excessive broadening of the resonance spectrum due to an increase in the contribution of multipolar excitations. This restricts the sensing resolution. The insensitivity of the plasmon response to the metal composition is attributable to the fact that the bulk plasma frequency of the metal, which determines the spectral dispersion of the real dielectric function of metals and the surface plasmon resonance condition, has a similar value for the noble metals. On the other hand, nanorods with higher Ag concentration show a great enhancement in magnitude and sharpness of the plasmon resonance band, which gives better sensing resolution despite similar plasmon response. Furthermore, Ag nanorods have an additional advantage as better scatterers compared with Au nanorods of the same size.

Raman Scattering from High-Frequency Phonons in Supported n-Graphene Layer Films

Abstract: Results of room-temperature Raman scattering studies of ultrathin graphitic films supported on Si (100)/SiO2 substrates are reported. The results are significantly different from those known for graphite. Spectra were collected using 514.5 nm radiation on films containing from n = 1 to 20 graphene layers, as determined by atomic force microscopy. Both the first- and second-order Raman spectra show unique signatures of the number of layers in the film. The nGL film analogue of the Raman G-band in graphite exhibits a Lorentzian line shape whose center frequency shifts linearly relative to graphite as ∼1/n (for n = 1 ωG ≈ 1587 cm-1). Three weak bands, identified with disorder-induced first-order scattering, are observed at ∼1350, 1450, and 1500 cm-1. The ∼1500 cm-1 band is weak but relatively sharp and exhibits an interesting n-dependence. In general, the intensity of these D-bands decreases dramatically with increasing n. Three second-order bands are also observed (∼2450, ∼2700, and 3248 cm-1). They are ana...

Application of spheroid models to account for aerosol particle nonsphericity in remote sensing of desert dust

Abstract: [ 1] The possibility of using shape mixtures of randomly oriented spheroids for modeling desert dust aerosol light scattering is discussed. For reducing calculation time, look-up tables were simulated for quadrature coefficients employed in the numerical integration of spheroid optical properties over size and shape. The calculations were done for 25 bins of the spheroid axis ratio ranging from similar to 0.3 ( flattened spheroids) to similar to 3.0 ( elongated spheroids) and for 41 narrow size bins covering the size parameter range from similar to 0.012 to similar to 625. The look-up tables were arranged into a software package, which allows fast, accurate, and flexible modeling of scattering by randomly oriented spheroids with different size and shape distributions. In order to evaluate spheroid model and explore the possibility of aerosol shape identification, the software tool has been integrated into inversion algorithms for retrieving detailed aerosol properties from laboratory or remote sensing polarimetric measurements of light scattering. The application of this retrieval technique to laboratory measurements by Volten et al. ( 2001) has shown that spheroids can closely reproduce mineral dust light scattering matrices. The spheroid model was utilized for retrievals of aerosol properties from atmospheric radiation measured by AERONET ground-based Sun/sky-radiometers. It is shown that mixtures of spheroids allow rather accurate fitting of measured spectral and angular dependencies of observed intensity and polarization. Moreover, it is shown that for aerosol mixtures with a significant fraction of coarse-mode particles ( radii >= similar to 1 mu m), the nonsphericity of aerosol particles can be detected as part of AERONET retrievals. The retrieval results indicate that nonspherical particles with aspect ratios similar to 1.5 and higher dominate in desert dust plumes, while in the case of background maritime aerosol spherical particles are dominant. Finally, the potential of using AERONET derived spheroid mixtures for modeling the effects of aerosol particle nonsphericity in other remote sensing techniques is discussed. For example, the variability of lidar measurements ( extinction to backscattering ratio and signal depolarization ratio) is illustrated and analyzed. Also, some potentially important differences in the sensitivity of angular light scattering to parameters of nonspherical versus spherical aerosols are revealed and discussed.

Optical properties of star-shaped gold nanoparticles.

Abstract: Here we report the synthesis, structure, and optical properties of ca. 100 nm star-shaped gold nanoparticles. Single particle spectroscopy measurements revealed that these nanoparticles have multiple plasmon resonances resulting in polarization-dependent scattering with multiple spectral peaks, which correspond to the different tips on the star-shaped structure. The plasmon resonances were also found to be extremely sensitive to the local dielectric environment.

Femtosecond diffractive imaging with a soft-X-ray free-electron laser

Abstract: Theory predicts that with an ultrashort and extremely bright coherent X-ray pulse, a single diffraction pattern may be recorded from a large macromolecule, a virus, or a cell before the sample explodes and turns into a plasma. Here we report the first experimental demonstration of this principle using the FLASH soft X-ray free-electron laser. An intense 25 fs, 4 x 10{sup 13} W/cm{sup 2} pulse, containing 10{sup 12} photons at 32 nm wavelength, produced a coherent diffraction pattern from a nano-structured non-periodic object, before destroying it at 60,000 K. A novel X-ray camera assured single photon detection sensitivity by filtering out parasitic scattering and plasma radiation. The reconstructed image, obtained directly from the coherent pattern by phase retrieval through oversampling, shows no measurable damage, and extends to diffraction-limited resolution. A three-dimensional data set may be assembled from such images when copies of a reproducible sample are exposed to the beam one by one.

Improved performance of amorphous silicon solar cells via scattering from surface plasmon polaritons in nearby metallic nanoparticles

Abstract: An engineered enhancement in short-circuit current density and energy conversion efficiency in amorphous silicon p-i-n solar cells is achieved via improved transmission of electromagnetic radiation arising from forward scattering by surface plasmon polariton modes in Au nanoparticles deposited above the amorphous silicon film. For a Au nanoparticle density of ∼3.7×108cm−2, an 8.1% increase in short-circuit current density and an 8.3% increase in energy conversion efficiency are observed. Finite-element electromagnetic simulations confirm the expected increase in transmission of electromagnetic radiation at visible wavelengths, and suggest that substantially larger improvements should be attainable for higher nanoparticle densities.

Screening Effect and Impurity Scattering in Monolayer Graphene

Abstract: The static polarization function is calculated in two-dimensional graphite and used for the calculation of the conductivity limited by charged-impurity scattering. The conductivity increases in proportion to the electron concentration and the mobility remains independent of the Fermi energy, in qualitative agreement with experiments. The screening increases in proportion to temperature at sufficiently high temperatures in contrast to the behavior in conventional two-dimensional systems, leading to the mobility increase proportional to the square of temperature.

Cross Sections for Electron Collisions with Nitrogen Molecules

Abstract: Cross section data have been compiled for electron collisions with nitrogen molecules, based on 104 references. Cross sections are collected and reviewed for: total scattering, elastic scattering, momentum transfer, excitations of rotational, vibrational, and electronic states, dissociation, ionization, and emission of radiation. For each process, the recommended values of the cross section are presented for use. The literature has been surveyed through the end of 2003.

Optical properties of deep glacial ice at the South Pole

Abstract: We have remotely mapped optical scattering and absorption in glacial ice at the South Pole for wavelengths between 313 and 560 nm and depths between 1100 and 2350 m. We used pulsed and continuous light sources embedded with the AMANDA neutrino telescope, an array of more than six hundred photomultiplier tubes buried deep in the ice. At depths greater than 1300 m, both the scattering coefficient and absorptivity follow vertical variations in concentration of dust impurities, which are seen in ice cores from other Antarctic sites and which track climatological changes. The scattering coefficient varies by a factor of seven, and absorptivity (for wavelengths less than ∼450 nm) varies by a factor of three in the depth range between 1300 and 2300 m, where four dust peaks due to stadials in the late Pleistocene have been identified. In our absorption data, we also identify a broad peak due to the Last Glacial Maximum around 1300 m. In the scattering data, this peak is partially masked by scattering on residual air bubbles, whose contribution dominates the scattering coefficient in shallower ice but vanishes at ∼1350 m where all bubbles have converted to nonscattering air hydrates. The wavelength dependence of scattering by dust is described by a power law with exponent -0.90 ± 0.03, independent of depth. The wavelength dependence of absorptivity in the studied wavelength range is described by the sum of two components: a power law due to absorption by dust, with exponent -1.08 ± 0.01 and a normalization proportional to dust concentration that varies with depth; and a rising exponential due to intrinsic ice absorption which dominates at wavelengths greater than ∼500 nm. Copyright 2006 by the American Geophysical Union.

Polyhedral silver nanocrystals with distinct scattering signatures

Abstract: Silver nanoparticles are ideal building blocks for opticalmaterials that seek to manipulate, transport, or amplify light becausethey support surface plasmons with frequencies in the visible and near-IRregime. We demonstrate that polyhedral silvernanocrystals displaycomplex and distinct scattering signatures dictated by shape and size.The ability to engineer specific plasmon modes should have profoundconsequences for surface-enhanced Raman spectroscopy, sub-wavelengthoptics, and plasmonic transport.

Multiple Scattering of Light by Particles: Radiative Transfer and Coherent Backscattering

Abstract: 1. Introduction 2. Maxwell's equations, electromagnetic waves, and Stokes parameters 3. Basic theory of electromagnetic scattering 4. Scattering by a fixed multi-particle group 5. Statistical averaging 6. Scattering by a single random particle 7. Single scattering by a small random particle group 8. Radiative transfer equation 9. Calculations and measurements of single-particle characteristics 10. Radiative transfer in plane-parallel scattering media 11. Macroscopically isotropic and mirror-symmetric scattering media 12. Radiative transfer in plane-parallel, microscopically isotropic and mirror-symmetric scattering media 13. Illustrative applications of radiative transfer theory 14. Coherent backscattering.

The modified Beer–Lambert law revisited

Abstract: The modified Beer–Lambert law (MBLL) is the basis of continuous-wave near-infrared tissue spectroscopy (cwNIRS). The differential form of MBLL (dMBLL) states that the change in light attenuation is proportional to the changes in the concentrations of tissue chromophores, mainly oxy- and deoxyhaemoglobin. If attenuation changes are measured at two or more wavelengths, concentration changes can be calculated. The dMBLL is based on two assumptions: (1) the absorption of the tissue changes homogeneously, and (2) the scattering loss is constant. It is known that absorption changes are usually inhomogeneous, and therefore dMBLL underestimates the changes in concentrations (partial volume effect) and every calculated value is influenced by the change in the concentration of other chromophores (cross-talk between chromophores). However, the error introduced by the second assumption (cross-talk of scattering changes) has not been assessed previously. An analytically treatable special case (semi-infinite, homogeneous medium, with optical properties of the cerebral cortex) is utilized here to estimate its order of magnitude. We show that the per cent change of the transport scattering coefficient and that of the absorption coefficient have an approximately equal effect on the changes of attenuation, and a 1% increase in scattering increases the estimated concentration changes by about 0.5 µM.

Designing, fabricating, and imaging Raman hot spots

Abstract: We have developed a probe of the electromagnetic mechanism of surface-enhanced Raman scattering via Au nanodisk arrays generated by using on-wire lithography. In this approach, disk thickness and interparticle gap are precisely controlled from 5 nm to many micrometers. Confocal Raman microscopy demonstrates that disk thickness and gap play a crucial role in determining surface-enhanced Raman scattering intensities. Theoretical calculations also demonstrate that these results are consistent with the electromagnetic mechanism, including the surprising result that the largest enhancement does not occur for the smallest gaps.

Inverse Scattering Transform for the Camassa-Holm equation

Abstract: An inverse scattering method is developed for the Camassa–Holm equation. As an illustration of our approach the solutions corresponding to the reflectionless potentials are constructed in terms of the scattering data. The main difference with respect to the standard inverse scattering transform lies in the fact that we have a weighted spectral problem. We therefore have to develop different asymptotic expansions.

Seeded growth of submicron Au colloids with quadrupole plasmon resonance modes.

Abstract: A modified seeded growth process has been used for the controlled synthesis of quasispherical, CTAB-stabilized gold nanoparticles from 12 up to 180 nm with narrow size distributions The UV-visible spectra of the aqueous colloids show distinct bands corresponding to dipole and quadrupole plasmon modes, for diameters above 100 nm, in close agreement with predictions based on Mie theory The assignment of the modes is demonstrated by calculation of near field enhancement maps based on the boundary element method Apart from other applications, since absorption is drastically reduced above 600 nm, while scattering is largely increased, these particles open new possibilities for construction of highly efficient photonic structures

Resonance Raman scattering of rhodamine 6G as calculated using time-dependent density functional theory.

Abstract: In this work, we present the first calculation of the resonance Raman scattering (RRS) spectrum of rhodamine 6G (R6G) which is a prototype molecule in surface-enhanced Raman scattering (SERS). The calculation is done using a recently developed time-dependent density functional theory (TDDFT) method, which uses a short-time approximation to evaluate the Raman scattering cross section. The normal Raman spectrum calculated with this method is in good agreement with experimental results. The calculated RRS spectrum shows qualitative agreement with SERS results at a wavelength that corresponds to excitation of the S(1) state, but there are significant differences with the measured RRS spectrum at wavelengths that correspond to excitation of the vibronic sideband of S(1). Although the agreement with the experiments is not perfect, the results provide insight into the RRS spectrum of R6G at wavelengths close to the absorption maximum where experiments are hindered due to strong fluorescence. The calculated resonance enhancements are found to be on the order of 10(5). This indicates that a surface enhancement factor of about 10(10) would be required in SERS in order to achieve single-molecule detection of R6G.

Observations of Plasmons in Warm Dense Matter

Abstract: We present the first collective x-ray scattering measurements of plasmons in solid-density plasmas. The forward scattering spectra of a laser-produced narrow-band x-ray line from isochorically heated beryllium show that the plasmon frequency is a sensitive measure of the electron density. Dynamic structure calculations that include collisions and detailed balance match the measured plasmon spectrum indicating that this technique will enable new applications to determine the equation of state and compressibility of dense matter.

Intervalley Scattering, Long-Range Disorder, and Effective Time-Reversal Symmetry Breaking in Graphene

Abstract: We discuss the effect of certain types of static disorder, like that induced by curvature or topological defects, on the quantum correction to the conductivity in graphene. We find that when the intervalley scattering time is long or comparable to ?o these defects can induce an effective time-reversal symmetry breaking of the Hamiltonian associated to each one of the two valleys in graphene. The phenomenon suppresses the magnitude of the quantum correction to the conductivity and may result in the complete absence of a low-field magnetoresistance, as recently found experimentally. Our work shows that a quantitative description of weak localization in graphene must include the analysis of new regimes, not present in conventional two-dimensional electron gases.

Absorption and scattering microscopy of single metal nanoparticles

Abstract: Several recently developed detection techniques opened studies of individual metal nanoparticles (1-100 nm in diameter) in the optical far field. Eliminating averaging over the broad size and shape distributions produced by even the best of current synthesis methods, these studies hold great promise for gaining a deeper insight into many of the properties of metal nanoparticles, notably electronic and vibrational relaxation. All methods are based on detection of a scattered wave emitted either by the particle itself, or by its close environment. Direct absorption and interference techniques rely on the particle's scattering and have similar limits in signal-to-noise ratio. The photothermal method uses a photo-induced change in the refractive index of the environment as an additional step to scatter a wave with a different wavelength. This leads to a considerable improvement in signal-to-background ratio, and thus to a much higher sensitivity. We briefly discuss and compare these various techniques, review the new results they generated so far, and conclude on their great potential for nanoscience and for single-molecule labelling in biological assays and live cells.

On the fundamental imaging-depth limit in two-photon microscopy

Abstract: We have analyzed how the maximal imaging depth of two-photon microscopy in scattering samples depends on properties of the sample and the imaging system. We find that the imaging depth increases with increasing numerical aperture and staining inhomogeneity and with decreasing excitation-pulse duration and scattering anisotropy factor, but is ultimately limited by near-surface fluorescence with slight improvements possible using special detection strategies.

Heterodyne coherent anti-Stokes Raman scattering (CARS) imaging.

Abstract: We have achieved rapid nonlinear vibrational imaging free of nonresonant background with heterodyne coherent anti-Stokes Raman scattering (CARS) interferometric microscopy. This technique completely separates the real and imaginary responses of nonlinear susceptibility chi(3) and yields a signal that is linear in the concentration of vibrational modes. We show that heterodyne CARS microscopy permits the detection of weak vibrational resonances that are otherwise overshadowed by the strong interference of the nonresonant background.

Contributions from radiation damping and surface scattering to the linewidth of the longitudinal plasmon band of gold nanorods: a single particle study

Abstract: The scattering spectra of single gold nanorods with aspect ratios between 2 and 4 have been examined by dark field microscopy. The results show that the longitudinal plasmon resonance (electron oscillation along the long axis of the rod) broadens as the width of the rods decreases from 14 to 8 nm. This is attributed to electron surface scattering. Analysis of the data using γ = γbulk + AνF/Leff, where Leff is the effective path length of the electrons and νF is the Fermi velocity, allows us to determine a value for the surface scattering parameter of A = 0.3. Larger rods with widths of 19 and 30 nm were also examined. These samples also show spectral broadening, which is attributed to radiation damping. The relative strengths of the surface scattering and radiation damping effects are in excellent agreement with recent work on spherical gold nanoparticles by Sonnichsen et al., Phys. Rev. Lett., 2002, 88, 077402; and by Berciaud et al., Nano Lett., 2005, 5, 515.

Lyman α radiative transfer in a multiphase medium

Abstract: Hydrogen Lyman a (Lya) is our primary emission-line window into high-redshift galaxies. Despite an extensive literature, Lya radiative transfer in the most realistic case of a dusty, multiphase medium has received surprisingly little detailed theoretical attention. We investigate Lya resonant scattering through an ensemble of dusty, moving, optically thick gas clumps. We treat each clump as a scattering particle and use Monte Carlo simulations of surface scattering to quantify continuum and Lya surface scattering angles, absorption probabilities, and frequency redistribution, as a function of the gas dust content. This atomistic approach speeds up the simulations by many orders of magnitude, making possible calculations which are otherwise intractable. Our fitting formulae can be readily adapted for fast radiative transfer in numerical simulations. With these surface scattering results, we develop an analytic framework for estimating escape fractions and line widths as a function of gas geometry, motion, and dust content. Our simple analytic model shows good agreement with full Monte Carlo simulations. We show that the key geometric parameter is the average number of surface scatters for escape in the absence of absorption, N 0 , and we provide fitting formulae for several geometries of astrophysical interest. We consider the following two interesting applications. (i) Equivalent widths (EWs). Lya can preferentially escape from a dusty multiphase interstellar medium if most of the dust lies in cold neutral clouds, which Lya photons cannot penetrate. This might explain the anomalously high EWs sometimes seen in high-redshift/submillimetre sources. (ii) Multiphase galactic outflows. We show the characteristic profile is asymmetric with a broad red tail, and relate the profile features to the outflow speed and gas geometry. Many future applications are envisaged.

Determination of optical properties of human blood in the spectral range 250 to 1100 nm using Monte Carlo simulations with hematocrit-dependent effective scattering phase functions.

Abstract: The absorption coefficient mu(a), scattering coefficient mu(s), and anisotropy factor g of diluted and undiluted human blood (hematocrit 0.84 and 42.1%) are determined under flow conditions in the wavelength range 250 to 1100 nm, covering the absorption bands of hemoglobin. These values are obtained by high precision integrating sphere measurements in combination with an optimized inverse Monte Carlo simulation (IMCS). With a new algorithm, appropriate effective phase functions could be evaluated for both blood concentrations using the IMCS. The best results are obtained using the Reynolds-McCormick phase function with the variation factor alpha = 1.2 for hematocrit 0.84%, and alpha = 1.7 for hematocrit 42.1%. The obtained data are compared with the parameters given by the Mie theory. The use of IMCS in combination with selected appropriate effective phase functions make it possible to take into account the nonspherical shape of erythrocytes, the phenomenon of coupled absorption and scattering, and multiple scattering and interference phenomena. It is therefore possible for the first time to obtain reasonable results for the optical behavior of human blood, even at high hematocrit and in high hemoglobin absorption areas. Moreover, the limitations of the Mie theory describing the optical properties of blood can be shown.

Wouthuysen-Field coupling strength and application to high-redshift 21-cm radiation

Abstract: The first ultraviolet sources in the universe are expected to have coupled the H I spin temperature to the gas kinetic temperature via scattering in the Lyα resonance (the 'Wouthuysen-Field effect'). By establishing an Hi spin temperature different from the temperature of the cosmic microwave background, the Wouthuysen-Field effect should allow observations of H I during the reionization epoch in the redshifted 21-cm hyperfine line. This paper investigates four mechanisms that can affect the strength of the Wouthuysen-Field effect that were not previously considered. (1) Photons redshifting into the Hi Lyman resonances may excite an H atom and result in a radiative cascade terminating in two-photon 2s 1/2 → 1s 1/2 emission, rather than always degrading to Lyα as usually assumed. (2) The fine structure of the Lyα resonance alters the photon frequency distribution and leads to a suppression of the scattering rate. (3) The spin-flip scatterings change the frequency of the photon and cause the photon spectrum to relax not to the kinetic temperature of the gas but to a temperature between the kinetic and spin temperatures, effectively reducing the strength of the Wouthuysen-Field coupling. (4) Near line centre, a photon can change its frequency by several times the line width in a single scattering event, thus potentially invalidating the usual calculation of the Lyα spectral distortion based on the diffusion approximation. It is shown that (1) suppresses the Wouthuysen-Field coupling strength by a factor of up to ∼2, while (2) and (3) are important only at low kinetic temperatures. Effect (4) has a ≤3 per cent effect for kinetic temperatures T k ≥ 2 K. In particular, if the pre-reionization intergalactic medium was efficiently heated by X-rays, only effect (1) is important. Fitting formulae for the Wouthuysen-Field coupling strength are provided for the range of T k ≥ 2 K and Gunn-Peterson optical depth 10 5 < TOP < 10 7 so that all of these effects can be easily incorporated into 21-cm codes.