Showing papers on "Absorption (electromagnetic radiation) published in 1999"

Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication

Abstract: Two-photon excitation provides a means of activating chemical or physical processes with high spatial resolution in three dimensions and has made possible the development of three-dimensional fluorescence imaging1, optical data storage2,3 and lithographic microfabrication4,5,6. These applications take advantage of the fact that the two-photon absorption probability depends quadratically on intensity, so under tight-focusing conditions, the absorption is confined at the focus to a volume of order λ3 (where λ is the laser wavelength). Any subsequent process, such as fluorescence or a photoinduced chemical reaction, is also localized in this small volume. Although three-dimensional data storage and microfabrication have been illustrated using two-photon-initiated polymerization of resins incorporating conventional ultraviolet-absorbing initiators, such photopolymer systems exhibit low photosensitivity as the initiators have small two-photon absorption cross-sections (δ). Consequently, this approach requires high laser power, and its widespread use remains impractical. Here we report on a class of π;-conjugated compounds that exhibit large δ (as high as 1, 250 × 10−50 cm4 s per photon) and enhanced two-photon sensitivity relative to ultraviolet initiators. Two-photon excitable resins based on these new initiators have been developed and used to demonstrate a scheme for three-dimensional data storage which permits fluorescent and refractive read-out, and the fabrication of three-dimensional micro-optical and micromechanical structures, including photonic-bandgap-type structures7.

Simulation of the Optical Absorption Spectra of Gold Nanorods as a Function of Their Aspect Ratio and the Effect of the Medium Dielectric Constant

Abstract: Gold nanorods with different aspect ratios are prepared in micelles by the electrochemical method and their absorption spectra are modeled by theory. Experimentally, a linear relationship is found between the absorption maximum of the longitudinal plasmon resonance and the mean aspect ratio as determined from TEM. It is shown here that such a linear dependence is also predicted theoretically. However, calculations also show that the absorption maximum of the longitudinal plasmon resonance depends on the medium dielectric constant in a linear fashion for a fixed aspect ratio. Attempts to fit the calculations to the experimental values indicate that the medium dielectric constant has to vary with the aspect ratio in a nonlinear way. Chemically, this suggests that the structure of the micelle capping the gold nanorods is size dependent. Furthermore, comparison with the results obtained for rods of different aspect ratios made by systematic thermal decomposition of the long rods further suggests that the medi...

Calibration and Intercomparison of Filter-Based Measurements of Visible Light Absorption by Aerosols

Abstract: Data on light absorption by atmospheric particles are scarce relative to the need for global characterization. Most of the existing data come from methods that measure the change in light transmission through a filter on which particles are collected. We present a calibration of a recently developed filter-based instrument for continuous measurement of light absorption (model PSAP, Radiance Research, Seattle, WA) that has been incorporated in several measurement programs. This calibration uses a reference absorption determined as the difference between light extinction and light scattering by unaltered (suspended) particles. In addition, we perform the same calibration for two other common filter-based methods: an Integrating Plate and the Hybrid Integrating Plate System. For each method, we assess the responses to both particulate light scattering and particulate light absorption. We find that each of the instruments exhibits a significant response to nonabsorbing aerosols and overestimates absorption at...

A Solar Radiation Parameterization for Atmospheric Studies

Abstract: The solar radiation parameterization (CLIRAD-SW) developed at the Goddard Climate and Radiation Branch for application to atmospheric models are described. It includes the absorption by water vapor, O3, O2, CO2, clouds, and aerosols and the scattering by clouds, aerosols, and gases. Depending upon the nature of absorption, different approaches are applied to different absorbers. In the ultraviolet and visible regions, the spectrum is divided into 8 bands, and single O3 absorption coefficient and Rayleigh scattering coefficient are used for each band. In the infrared, the spectrum is divided into 3 bands, and the k-distribution method is applied for water vapor absorption. The flux reduction due to O2 is derived from a simple function, while the flux reduction due to CO2 is derived from precomputed tables. Cloud single-scattering properties are parameterized, separately for liquid drops and ice, as functions of water amount and effective particle size. A maximum-random approximation is adopted for the overlapping of clouds at different heights. Fluxes are computed using the Delta-Eddington approximation.

Semianalytic Moderate‐Resolution Imaging Spectrometer algorithms for chlorophyll a and absorption with bio‐optical domains based on nitrate‐depletion temperatures

Abstract: This paper describes algorithms for retrieval of chlorophyll a concentration and phytoplankton and gelbstoff absorption coefficients for the Moderate-Resolution Imaging Spectrometer (MODIS) or sensors with similar spectral channels. The algorithms are based on a semianalytical, bio-optical model of remote sensing reflectance, Rrs(λ). The Rrs(λ) model has two free variables, the absorption coefficient due to phytoplankton at 675 nm, aϕ(675), and the absorption coefficient due to gelbstoff at 400 nm, ag(400). The Rrs model has several parameters that are fixed or can be specified based on the region and season of the MODIS scene. These control the spectral shapes of the optical constituents of the model. Rrs(λi) values from the MODIS data processing system are placed into the model, the model is inverted, and aϕ(675), ag(400), and chlorophyll a are computed. The algorithm also derives the total absorption coefficients a(λi) and the phytoplankton absorption coefficients aϕ(λi) at the visible MODIS wavelengths. MODIS algorithms are parameterized for three different bio-optical domains: (1) high photoprotective pigment to chlorophyll ratio and low self-shading, which for brevity, we designate as “unpackaged”; (2) low photoprotective pigment to chlorophyll ratio and high self-shading, which we designate as “packaged”; and (3) a transitional or global-average type. These domains can be identified from space by comparing sea-surface temperature to nitrogen-depletion temperatures for each domain. Algorithm errors of more than 45% are reduced to errors of less than 30% with this approach, with the greatest effect occurring at the eastern and polar boundaries of the basins.

Effects of mixing on extinction by carbonaceous particles

Abstract: Reported values for the absorption cross section of particulate carbon per unit mass range from under 4 to over 20 m2/g, and the intermediate value of 10 m2/g is used by many as a standard gram-specific absorption cross section for atmospheric soot. In order to better understand the possible variations in absorption by atmospheric carbon, we reevaluated its optical properties in terms of the material composition and morphology of soot and the electrodynamics of spherules agglomerated into loose (ramiform) aggregates. Primary particles ranging in composition from paracrystalline graphite to low-density air/graphite volume mixtures are considered. The effects on extinction efficiency of aggregation and of internal mixing of carbon with sulfate are considered in detail. We also compare our results with estimates of specific absorption of internally mixed soot that are based on several homogeneous mixing rules (effective medium approximations), On the basis of our modeling of the optical properties of aggregates of graphitic carbon grains, we conclude that 10 m2/g may be over 50% too high in many cases, and we suggest that the mass absorption coefficient for the light-absorbing carbon in diesel soot at a wavelength of 0.550 μm may often be less than 7 m2/g, although variations in optical constants and, especially, the specific gravity of the absorbing material make it difficult to assign a specific numerical value. Adhesion of carbon grains to sulfate droplet surfaces is expected to enhance their absorption by no more than about 30%. Soot randomly positioned within droplets, however, can display averaged absorption enhancement factors of about 2.5–4 for hosts with refractive indices ranging from 1.33–1.53, respectively, and radii ≳0.20 μm. Nonetheless, calculations indicate that for realistic dry particle populations, αa < 10 m2/g for graphitic carbon in the atmosphere unless (1) most of it is encapsulated, and (2) the geometric mean radius of the hosts is larger than about 0.06 μm (which corresponds to a mass median diameter of 0.34 μm). These results suggest the importance of the determination of the physical state of the soot particles and their immediate environment when ascribing characteristic values for their absorption and scattering efficiencies.

Laser-induced plasma formation in water at nanosecond to femtosecond time scales: calculation of thresholds, absorption coefficients, and energy density

Abstract: The generation of plasmas in water by high-power laser pulses was investigated for pulse durations between 100 ns and 100 fs on the basis of a rate equation for the free electron density. The rate equation was numerically solved to calculate the evolution of the electron density during the laser pulse and to determine the absorption coefficient and energy density of the plasma. For nanosecond laser pulses, the generation of free electrons in distilled water is initiated by multiphoton ionization but then dominated by cascade ionization. For shorter laser pulses, multiphoton ionization gains ever more importance, and collision and recombination losses during breakdown diminish. The corresponding changes in the evolution of the free carrier density explain the reduction of the energy threshold for breakdown and of the plasma energy density observed with decreasing laser pulse duration. By solving the rate equation, we could also explain the complex pulse duration dependence of plasma transmission found in previous experiments. Good quantitative agreement was found between calculated and measured values for the breakdown threshold, plasma absorption coefficient, and plasma energy density.

Energy balance of optical breakdown in water at nanosecond to femtosecond time scales

Abstract: During optical breakdown, the energy delivered to the sample is either transmitted, reflected, scattered, or ab- sorbed. Pathways for the division of the absorbed energy are the evaporation of the focal volume, the plasma radiation, and the mechanical effects such as shock wave emission and cav- itation. The partition of laser energy between these channels during breakdown in water was investigated for four selected laser parameters typical for intraocular microsurgery ( 6-ns pulses of 1 and 10 mJ focused at an angle of 22 ,a nd30-ps pulses of 50 mJ and 1m Jfocused at 14 ,a ll at1064 nm). Scattering and reflection were found to be small compared to transmission and absorption during optical breakdown. The ratio of the shock wave energy and cavitation bubble energy was approximately constant (between 1.5:1 and 2:1). These results allowed us to perform a more comprehensive study of the influence of pulse duration ( 100 fs- 76 ns )a nd focus- ing angle (4- 32) on the energy partition by measuring only the plasma transmission and the cavitation bubble energy. The bubble energy was used as an indicator for the total amount of mechanical energy. We found that the absorption at the breakdown site first decreases strongly with decreasing pulse duration, but increases again for < 3p s. The conversion of the absorbed energy into mechanical energy is 90% with ns pulses at large focusing angles. It decreases both with de- creasing focusing angle and pulse duration (to < 15 %f or fs pulses). The disruptive character of plasma-mediated laser effects is therefore strongly reduced when ultrashort laser pulses are used.

In vivo local determination of tissue optical properties: applications to human brain.

Abstract: Local and superficial near-infrared (NIR) optical-property characterization of turbid biological tissues can be achieved by measurement of spatially resolved diffuse reflectance at small source-detector separations (<1.4 mm). However, in these conditions the inverse problem, i.e., calculation of localized absorption and the reduced scattering coefficients, is necessarily sensitive to the scattering phase function. This effect can be minimized if a new parameter of the phase function gamma, which depends on the first and the second moments of the phase function, is known. If gamma is unknown, an estimation of this parameter can be obtained by the measurement, but the uncertainty of the absorption coefficient is increased. A spatially resolved reflectance probe employing multiple detector fibers (0.3-1.4 mm from the source) is described. Monte Carlo simulations are used to determine gamma, the reduced scattering and absorption coefficients from reflectance data. Probe performance is assessed by measurements on phantoms, the optical properties of which were measured by other techniques [frequency domain photon migration (FDPM) and spatially resolved transmittance]. Our results show that changes in the absorption coefficient, the reduced scattering coefficient, and gamma can be measured to within +/-0.005 mm(-1), +/-0.05 mm(-1), and +/-0.2, respectively. In vivo measurements performed intraoperatively on a human skull and brain are reported for four NIR wavelengths (674, 811, 849, 956 nm) when the spatially resolved probe and FDPM are used. The spatially resolved probe shows optimum measurement sensitivity in the measurement volume immediately beneath the probe (typically 1 mm(3) in tissues), whereas FDPM typically samples larger regions of tissues. Optical-property values for human skull, white matter, scar tissue, optic nerve, and tumors are reported that show distinct absorption and scattering differences between structures and a dependence on the phase-function parameter gamma.

The determination of in vivo human tissue optical properties and absolute chromophore concentrations using spatially resolved steady-state diffuse reflectance spectroscopy.

Abstract: A method is described for measuring optical properties and deriving chromophore concentrations from diffuse reflection measurements at the surface of a turbid medium. The method uses a diffusion approximation model for the diffuse reflectance, in combination with models for the absorption and scattering coefficients. An optical fibre-based set-up, capable of measuring nine spectra from 400 to 1050 nm simultaneously, is used to test the method experimentally. Results of the analyses of phantom and in vivo measurements are presented. These demonstrate that in the wavelength range from 600 to 900 nm, tissue scattering can be described as a simple power dependence of the wavelength and that the tissue absorption can be accurately described by the addition of water, oxy- and deoxyhaemoglobin absorption.

Cooperative Enhancement of Two-Photon Absorption in Multi-branched Structures

Abstract: Recent reports of molecular structures with considerably enhanced two-photon absorption cross-section have generated considerable interest in this phenomenon from both fundamental and applications perspectives. In this letter, we report cooperative enhancement of two-photon absorption in multi-branched structures which may lead to new design criteria for development of highly efficient two-photon materials. The multi-branched structures were synthesized using coupling of two and three two-photon active asymmetric donor−acceptor chromophores linked together by a common amine group. The two-photon cross-sections measured both with nanosecond and femtosecond pulses show that the value for the trimer is more than six times larger than that for the monomer, and not just three times larger as expected from the number density increase.

Interpretation of the 685nm peak in water-leaving radiance spectra in terms of fluorescence, absorption and scattering, and its observation by MERIS

Abstract: One of the major design goals of the Medium Resolution Imaging Spectrometer (MERIS) was the capability to use the signal from chlorophyll fluorescence stimulated by ambient sunlight to detect and map phytoplankton. This is considered tobe especially useful in coastal waters, where the determination of chlorophyll from water-leaving radiance spectra using the conventional blue/green ratio method is often complicated by high concentrations of gelbstoff and suspended matter. Based on a variety of studies, three spectral channels centred at 665, 681.25 and 705nm were included in the design of MERIS for retrieving the fluorescence signal. This paper presents observations with highresolution spectrometers which demonstrate the main factors affecting the observed signal in the red part of the spectrum. These factors are absorption by pure water, scattering by suspended particles, absorption and fluorescence of chlorophyll and the influence of submerged macrophyta. The influence of exceptional blooms such as 'red...

Cavity-ringdown spectroscopy : an ultratrace-absorption measurement technique

Abstract: Cavity-ring-down spectroscopy is an emerging method for making high sensitivity absorption measurements with gas-phase samples. This volume covers the history, theory, and numerous applications.

Invariance Violation Extends the Cosmic Ray Horizon

Abstract: We postulate that the energy-momentum relation is modified for very high energy particles to violate Lorentz invariance and the speed of photon is changed from the light velocity c. The violation effect is amplified in a sensitive way to detection through the modified kinematical constraints on the conservation of energy and momentum, in the absorption process of γ-rays colliding against photons of longer wavelengths and converting into an electron-positron pair. For γ-rays of energies higher than 1013 eV, the minimum energy of the soft photons for the reaction and then the absorption mean free path of γ-rays are altered by orders of magnitude from those conventionally estimated. Consideration is similarly applied to high-energy cosmic-ray protons. The consequences may require the standard assumptions on the maximum distance from which very high energy radiation can travel to be revised.

Resonance Light Scattering and Its Application in Determining the Size, Shape, and Aggregation Number for Supramolecular Assemblies of Chromophores

Abstract: Resonance light scattering (RLS) on supramolecular assemblies of chromophores is a sensitive and selective method to extract size and shape information, but the interpretation of the data is complicated by the large amount of absorption present. By combining extinction and RLS measurements on the same samples of acidified tetrakis(4-sulfonatophenyl)porphine (H4TPPS), a technique is described whereby the scattering spectrum can be “corrected” for absorption. An additional benefit of this analysis is that the spectrum obtained for these solutions on a spectrophotometer, which is really an extinction spectrum, can be parsed into its absorption and scattering components. The results demonstrate that scattering contributes significantly to the aggregate peak in the extinction spectrum. Knowledge of the absorption and scattering components allows an estimation of the average aggregation number to be made, which for these solutions is on the order of 105−106. In addition, static and dynamic light scattering meas...

Measurements of the thz absorption and dispersion of znte and their relevance to the electro-optic detection of thz radiation

Abstract: Via THz time-domain spectroscopy, we have measured the absorption and index of refraction of single-crystal 〈110〉 ZnTe from 0.3 to 4.5 THz. We find that the absorption is dominated by two lower-frequency phonon lines at 1.6 and 3.7 THz and not by the transverse-optical (TO) -phonon line at 5.3 THz as previously assumed. However, the index of refraction is determined mainly by the TO-phonon line. Using these data, we discuss a frequency-domain picture of electro-optic detection of THz radiation below the TO-phonon resonance and compare with the photoconductive THz receiver over the same frequency range.

Monte Carlo study of diffuse reflectance at source–detector separations close to one transport mean free path

Abstract: The spatially resolved reflectance of turbid media is studied at short source–detector separations (approximately one transport mean free path) with Monte Carlo simulations. For such distances we found that the first and second moments of the phase function play a significant role in the reflectance curve, whereas the effect of higher-order moments is weak. Second-order similarity relations are tested and are found efficient at reducing the number of relevant parameters necessary to predict the reflectance. Indeed, only the four following parameters are necessary: the refractive index, the absorption coefficient, the reduced scattering coefficient, and a phase function parameter γ that depends on the first and second moments of the phase function. For media of known γ, the absorption and reduced scattering coefficients can be determined from the intensity and the slope of the log of the reflectance, measured at a single distance. Other empirical properties of the reflectance are derived from the simulations, using short-distance measurements, which provide clues for determining the scattering and absorption properties. In particular, the slope of the square root of the reflectance does not depend on the absorption coefficient but depends on both the reduced scattering coefficient and the phase function parameter γ.

Thermo-optical effects in Z -scan measurements using high-repetition-rate lasers

Abstract: In this paper the effects on Z-scan measurements of thermo-optical nonlinearities due to cumulative heating of the sample are investigated. A model calculation of the Z-scan signal induced by thermo-optical nonlinearities is presented which takes into account absorption processes involving an arbitrary number of photons as the sources of nonlinearity. It is quantitatively shown how weak linear or nonlinear absorption coefficients can give rise to large signals depending on the repetition rate of the laser and on the experimental conditions. Conversely, very weak nonlinear absorption coefficients can be measured exploiting the effect of cumulative heating when using a long train of laser pulses. The possibility of separating such thermal contributions from fast optical nonlinearities in Z-scan signals is discussed.

Plasma Absorption Probe for Measuring Electron Density in an Environment Soiled with Processing Plasmas

Abstract: In this paper, we describe a novel and simple technique for measuring electron density using a plasma absorption probe (PAP). PAP enables us to measure the local absolute electron density even when the probe surface is soiled with processing plasmas. The technique relies on the resonant absorption of surface waves (SWs) excited in a "cavity" at the probe head. The PAP consists of a small antenna connected with a coaxial cable and is enclosed in a tube (dielectric constant e) inserted in a plasma (electron plasma frequency ωp). A network analyzer feeds a rf signal to the antenna and displays the frequency dependence of the power absorption. A series of resonant absorptions are observed at frequencies slightly above the SW resonance frequency, ωSW = ωp/(1+e)1/2, which allows us to determine the electron density. The measured electron densities are in good agreement with the data obtained by the plasma oscillation method.

Spectral properties of carbon black

Abstract: The internal structure of carbon black particles considerably influences the optical behavior of the material, apart from the shape and agglomeration state of the primary particles. In this paper the correlation between internal structure and spectral behavior of carbon black is investigated experimentally. The carbon blacks were produced by resistive heating of graphite electrodes and condensation in a cooling gas atmosphere. The internal structure of the primary carbon black particles was investigated by high-resolution transmission electron microscopy, electron energy loss spectroscopy, 13 C NMR spectroscopy, and Raman spectroscopy. The primary particles were found to consist of bent or plane structural subunits. The UV π−π* absorption feature of the produced carbon blacks varies in position between 196 and 265 nm depending on the state of bending of the graphene layers in the subunits of particles and/or the dimensions of the plane graphitic microcrystallites and the incorporation of hydrogen. The different curvature radii of the graphene layers or the sizes of microcrystallites can be summarized by an integral dimension like the ratio of sp2/sp3 hybridized carbon atoms. In the mid-infrared spectral region, the absolute value of the absorption coefficient κ is dominated by a continuous absorption due to free charge carriers which are also influenced by the ratio of sp2/sp3 hybridized carbon in the primary particles. The appearance of prominent bands is related to the existence of functional groups, like C–Hn, CO and/or C–O–C.

Far Infrared Properties of Electro-Optic Crystals Measured by THz Time-Domain Spectroscopy

Abstract: In this article we report an experimental investigation of the far-infrared properties of several nonlinear crystals, LiNbO3, LiTaO3, ZnTe and CdTe Using Terahertz Time-Domain Spectroscopy (THz-TDS) we have measured the complex frequency response, ie both index of refraction and absorption up to 3 THz (100 cm−1) for the electro-optic crystals at room temperature The single Lorentzian oscillator model is used to describe the aquired data Additional resonance features are observed, especially in the II-VI compounds

Electron population analysis by full-potential x-ray absorption simulations

Abstract: We present the first successful attempt at calculating cluster full-potential x-ray absorption near-edge structure (XANES) spectra, based on the finite difference method. By fitting XANES simulations onto experimental spectra we are able to perform electron population analysis. The method is tested in the case of Ti $K$-edge absorption spectrum in ${\mathrm{TiO}}_{2}$, where the amount of charge transfer between Ti and O atoms and of the screening charge on the photoabsorber is obtained taking into account both dipolar and quadrupolar transitions.

Microscale Quantification of the Absorption by Dissolved and Particulate Material in Coastal Waters with an ac-9

Abstract: Measuring coastal and oceanic absorption coefficients of dissolved and particulate matter in the visible domain usually requires a methodology for amplifying the natural signal because conventional spectrophotometers lack the necessary sensitivity. The WET Labs ac-9 is a recently developed in situ absorption and attenuation meter with a precision better than ±0.001 m−1 in the raw signal, which is sufficient to make these measurements in pristine samples. Whereas the superior sensitivity of the ac-9 has been well documented, the accuracy of in situ measurements for bio-optical applications has not been rigorously evaluated. Obtaining accurate results with an ac-9 requires careful attention to calibration procedures because baselines drift as a result of the changing optical properties of several ac-9 components. To correct in situ measurements for instrument drift, a pressurized flow procedure was developed for calibrating an ac-9 with optically clean water. In situ, micro- (cm) to fine- (m) scale...