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At least 505 records · Page 28

High temperature measurement of water vapor absorption

An investigation was undertaken to measure the absorption coefficient, at a wavelength of 10.6 microns, for mixtures of water vapor and a diluent gas at high temperature and pressure. The experimental concept was to create the desired conditions of temperature and pressure in a laser absorption wave, similar to that which would be created in a laser propulsion system. A simplified numerical model was developed to predict the characteristics of the absorption wave and to estimate the laser intensity threshold for initiation. A non-intrusive method for temperature measurement utilizing optical laser-beam deflection (OLD) and optical spark breakdown produced by an excimer laser, was thoroughly investigated and found suitable for the non-equilibrium conditions expected in the wave. Experiments were performed to verify the temperature measurement technique, to screen possible materials for surface initiation of the laser absorption wave and to attempt to initiate an absorption wave using the 1.5 kW carbon dioxide laser. The OLD technique was proven for air and for argon, but spark breakdown could not be produced in helium. It was not possible to initiate a laser absorption wave in mixtures of water and helium or water and argon using the 1.5 kW laser, a result which was consistent with the model prediction.

Keefer, Dennis↗

Research on photoelectric properties of n-GaN (0001) surface with point defects via first-principles

In order to reveal the influence of n-type doping and point defects on the electronic and optical properties of GaN (0001) surface, the pristine and defective n-GaN (0001) surface models are established. The formation energy, work function, atomic structure, electronic and optical properties of these surfaces are discussed by first-principles calculations. The results show that the defects have the strong tendency to be close to the surface position, and the N interstitial defect (N{sub i}) and the Ga vacancy (V{sub Ga}) are easily formed. The work function of the surface with V{sub Ga} drops the greatest, and the conductivity of n-type increases. In addition, the absorption coefficient of the surface with various defects is smaller than that of the pristine n-type surface. The appropriate amount of Ga vacancies can increase the probability of electron emission, but it is not conducive to the absorption of photons.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Narrow bandgap semiconducting silicides: Intrinsic infrared detectors on a silicon chip

Polycrystalline thin films of CrSi2, LaSi2, and ReSi2 were grown on silicon substrates. Normal incidence optical transmittance and reflectance measurements were made as a function of wavelength. It was demonstrated that LaSi2 is a metallic conductor, but that CrSi2 and ReSi2 are, in fact, narrow bandgap semiconductors. For CrSi2, the complex index of refraction was determined by computer analysis of the optical data. From the imaginary part, the optical absorption coefficient was determined as a function of photon energy. It was shown that CrSi2 possesses an indirect forbidden energy gap of slightly less than 0.31 eV, and yet it is a very strong absorber of light above the absorption edge. On the other hand, the ReSi2 films exhibit an absorption edge in the vicinity of 0.2 eV. Measurements of the thermal activation energy of resistivity for ReSi2 indicate a bandgap of 0.18 eV. It is concluded that the semiconducting silicides merit further investigation for development as new silicon-compatible infrared detector materials.

Mahan, John E.↗

Temperature dependence of the radiative recombination coefficient in crystalline silicon from spectral photoluminescence

The radiative recombination coefficient B(T) in crystalline silicon is determined for the temperature range 90–363 K, and in particular from 270 to 350 K with an interval of 10 K, where only sparse data are available at present. The band-band absorption coefficient established recently by Nguyen et al. [J. Appl. Phys. 115, 043710 (2014)] via photoluminescence spectrum measurements is employed to compute the values of B(T) at various temperatures. The results agree very well with literature data from Trupke et al. [J. Appl. Phys. 94, 4930 (2003).] We present a polynomial parameterization describing the temperature dependence of the product of B(T) and the square of the intrinsic carrier density. We also find that B(T) saturates at a near constant value at room temperature and above for silicon samples with relatively low free carrier densities.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Quantum mechanical calculation of the collision-induced absorption spectra of N{sub 2}–N{sub 2} with anisotropic interactions

We present quantum mechanical calculations of the collision-induced absorption spectra of nitrogen molecules, using ab initio dipole moment and potential energy surfaces. Collision-induced spectra are first calculated using the isotropic interaction approximation. Then, we improve upon these results by considering the full anisotropic interaction potential. We also develop the computationally less expensive coupled-states approximation for calculating collision-induced spectra and validate this approximation by comparing the results to numerically exact close-coupling calculations for low energies. Angular localization of the scattering wave functions due to anisotropic interactions affects the line strength at low energies by two orders of magnitude. The effect of anisotropy decreases at higher energy, which validates the isotropic interaction approximation as a high-temperature approximation for calculating collision-induced spectra. Agreement with experimental data is reasonable in the isotropic interaction approximation, and improves when the full anisotropic potential is considered. Calculated absorption coefficients are tabulated for application in atmospheric modeling.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

On the Mechanism of Absorption and Restoration of Radiation Transmission in the Channel of Small-Scale Self-Focusing of a Short Laser Pulse in Neodymium Glass

When diagnosing a small-scale self-focusing (SSSF) channel of a 0.5-ns laser pulse with an intensity of 3–5 GW/cm{sup 2} in neodymium glasses, an absorption jump was detected (with a front of ≈0.5 ns) at wavelengths of 1.06 and 0.66 μm in addition to filament-like damage typical of SSSF, spectral broadening, and laser radiation scattering. The absorption coefficient reached 0.15 cm{sup –1}, and transmission in the medium was restored during 15–35 ns for phosphate glass and 5–10 ns for silicate glass. The physical bases of this effect of the appearance and relaxation of absorption in glasses have not been previously presented. An analysis of the experimental data showed that the absorption jump is due to the fast population of the {sup 4}I{sub 11/2} level of Nd{sup 3+} ions in glasses when nonlinear processes occur in the SSSF channel such as stimulated Raman scattering and broadening of the laser pulse spectrum. The relaxation time of the population at the {sup 4}I{sub 11/2} level and the restoration of transmission in glasses after the termination of the laser pulse are determined by the characteristic sizes of the Nd{sup 3+} ions excitation regions arising in the samples upon interference of the laser and scattered radiation, as well as the thermophysical characteristics of the glasses.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The Influence of Ablation on Radiative Heating for Earth Entry

Using the coupled ablation and radiation capability recently included in the LAURA flowfield solver, this paper investigates the influence of ablation on the shock-layer radiative heating for Earth entry. The extension of the HARA radiation model, which provides the radiation predictions in LAURA, to treat a gas consisting of the elements C, H, O, and N is discussed. It is shown that the absorption coefficient of air is increased with the introduction of the C and H elements. A simplified shock layer model is studied to show the impact of temperature, as well as the abundance of C and H, on the net absorption or emission from an ablation contaminated boundary layer. It is found that the ablation species reduce the radiative flux in the vacuum ultraviolet, through increased absorption, for all temperatures. However, in the infrared region of the spectrum, the ablation species increase the radiative flux, through strong emission, for temperatures above 3,000 K. Thus, depending on the temperature and abundance of ablation species, the contaminated boundary layer may either provide a net increase or decrease in the radiative flux reaching the wall. To assess the validity of the coupled ablation and radiation LAURA analysis, a previously analyzed Mars-return case (15.24 km/s), which contains significant ablation and radiation coupling, is studied. Exceptional agreement with previous viscous shock-layer results is obtained. A 40% decrease in the radiative flux is predicted for ablation rates equal to 20% of the free-stream mass flux. The Apollo 4 peak-heating case (10.24 km/s) is also studied. For ablation rates up to 3.4% of the free-stream mass flux, the radiative heating is reduced by up to 19%, while the convective heating is reduced by up to 87%. Good agreement with the Apollo 4 radiometer data is obtained by considering absorption in the radiometer cavity. For both the Mars return and the Apollo 4 cases, coupled radiation alone is found to reduce the radiative heating by 30 60% and the convective heating by less than 5%.

Johnston, Christopher O.↗

Photoconductivity of ultra-thin Ge(GeSn) layers grown in Si by low-temperature molecular beam epitaxy

Photoconductivity (PC) spectra of Si/Ge(GeSn)/Si structures with the ultra-thin (1.0–2.3 nm) Ge and GeSn alloy layers grown by the low-temperature (T = 100 °C) molecular beam epitaxy are studied. Photoresponse in the range of 1.2–0.4 eV related to light absorption in the buried Ge(GeSn) layer is observed. It is shown that in case of lateral PC, a simple diffusion model can be used to determine the absorption coefficient of this layer α ∼ 10{sup 5 }cm{sup −1}. This value is 100 times larger than that of a single Ge quantum dot layer and is reached significantly above the band gap of most bulk semiconductors. The observed absorption is caused by optical transitions between electron and hole states localized at the interfaces. The anomalous high value of α can be explained by the unusual state of Ge(GeSn) layer with high concentration of dangling bonds, the optical properties of which have been predicted theoretically by Knief and von Niessen (Phys. Rev. B 59, 12940 (1999)).

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Photoaging of phenolic secondary organic aerosol in the aqueous phase: evolution of chemical and optical properties and effects of oxidants

Abstract. While gas-phase reactions are well established to have significant impacts on the mass concentration, chemical composition, and optical properties of secondary organic aerosol (SOA), the aqueous-phase aging of SOA remains poorly understood. In this study, we performed a series of long-duration photochemical aging experiments to investigate the evolution of the composition and light absorption of the aqueous SOA (aqSOA) from guaiacyl acetone (GA), a semivolatile phenolic carbonyl that is common in biomass burning smoke. The aqSOA was produced from reactions of GA with hydroxyl radical (•OH-aqSOA) or a triplet excited state of organic carbon (3C∗-aqSOA) and was then photoaged in water under conditions that simulate sunlight exposure in northern California for up to 48 h. The effects of increasing aqueous-phase •OH or 3C∗ concentration on the photoaging of the aqSOA were also studied. High-resolution aerosol mass spectrometry (HR-AMS) and UV–Vis spectroscopy were utilized to characterize the composition and the light absorptivity of the aqSOA and to track their changes during aging. Compared to •OH-aqSOA, the 3C∗-aqSOA is produced more rapidly and shows less oxidation, a greater abundance of oligomers, and higher light absorption. Prolonged photoaging promotes fragmentation and the formation of more volatile and less light-absorbing products. More than half of the initial aqSOA mass is lost, and substantial photobleaching occurs after 10.5 h of prolonged aging under simulated sunlight illumination for 3C∗-aqSOA and 48 h for •OH-aqSOA. By performing positive matrix factorization (PMF) analysis of the combined HR-AMS and UV–Vis spectral data, we resolved three generations of aqSOA with distinctly different chemical and optical properties. The first-generation aqSOA shows significant oligomer formation and enhanced light absorption at 340–400 nm. The second-generation aqSOA is enriched in functionalized GA species and has the highest mass absorption coefficients in 300–500 nm, while the third-generation aqSOA contains more fragmented products and is the least light absorbing. These results suggest that intermediately aged phenolic aqSOA is more light absorbing than other generations, and that the light absorptivity of phenolic aqSOA results from a competition between brown carbon (BrC) formation and photobleaching, which is dependent on aging time. Although photoaging generally increases the oxidation of aqSOA, a slightly decreased O/C of the •OH-aqSOA is observed after 48 h of prolonged photoaging with additional •OH exposure. This is likely due to greater fragmentation and evaporation of highly oxidized compounds. Increased oxidant concentration accelerates the transformation of aqSOA and promotes the decay of BrC chromophores, leading to faster mass reduction and photobleaching. In addition, compared with •OH, photoaging by 3C∗ produces more low-volatility functionalized products, which counterbalances part of the aqSOA mass loss due to fragmentation and evaporation.

54 ENVIRONMENTAL SCIENCES↗

A search for global and seasonal variation of methane from Nimbus 4 IRIS measurements

The Nimbus 4 infrared interferometer spectrometer (IRIS) measurements in the region around wave number 1304 show absorption due to methane in the earth's atmosphere. From the laboratory measurements of the absorption coefficient and a selected vertical distribution corresponding to 1.13 atm cm of methane, a theoretical model for the transmittance at wave number 1304 is developed. The weighting function deduced from this model shows a maximum around 300 mb. Some weak absorption due to nitrous oxide in the atmosphere has been taken into account. The vertical temperature profile, derived from the 15 micron CO2 band in the IRIS spectrum, together with the methane weighting function have been used in a consistent way to compute the upwelling intensity at wave number 1304. The brightness temperature corresponding to the IRIS observed radiance at wave number 1304 has been compared with the brightness temperature deduced from the calculated upwelling intensity from 80 deg North to 80 deg South and for different periods of the year. This comparison shows that the two brightness temperatures agree with one another to within the accuracy of measurements about 2 K. From this result it was found that global or seasonal variability of methane is less than + or - 0.25 atm cm.

Prabhakara, C.↗

Collisional Broadening of CO{sub 2} Transition Lines 10{sup 0}0–00{sup 0}1 by Inert Gas Atoms at 300–700 K

Using a tunable CO{sub 2} laser, unsaturated absorption coefficients in pure CO{sub 2} and binary CO{sub 2} gas mixtures with inert gases He, Ar, Kr, and Xe in a 1 : 2 ratio at 100 Torr were measured at the central frequencies of the R(8), R(22), P(8), P(22), and P(32) CO{sub 2} spectral lines of the 10{sup 0}0-00{sup 0}1 transition at 300–700 K. The coefficients of the collisional broadening of the CO{sub 2} spectral lines by He, Ar, Kr, and Xe are determined. The obtained temperature dependences of the collisional broadening coefficients are approximated by power functions with two different degrees.

74 ATOMIC AND MOLECULAR PHYSICS↗

Near-infrared free carrier absorption in heavily doped silicon

Free carrier absorption in heavily doped silicon can have a significant impact on devices operating in the infrared. In the near infrared, the free carrier absorption process can compete with band to band absorption processes, thereby reducing the number of available photons to optoelectronic devices such as solar cells. In this work, we fabricate 18 heavily doped regions by phosphorus and boron diffusion into planar polished silicon wafers; the simple sample structure facilitates accurate and precise measurement of the free carrier absorptance. We measure and model reflectance and transmittance dispersion to arrive at a parameterisation for the free carrier absorption coefficient that applies in the wavelength range between 1000 and 1500 nm, and the range of dopant densities between ∼10{sup 18} and 3 × 10{sup 20} cm{sup −3}. Our measurements indicate that previously published parameterisations underestimate the free carrier absorptance in phosphorus diffusions. On the other hand, published parameterisations are generally consistent with our measurements and model for boron diffusions. Our new model is the first to be assigned uncertainty and is well-suited to routine device analysis.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

In situ phytoplankton absorption, fluorescence emission, and particulate backscattering spectra determined from reflectance

An inverse model was developed to extract the absortion and scattering (elastic and inelastic) properties of oceanic constituents from surface spectral reflectance measurements. In particular, phytoplankton spectral absorption coefficients, solar-stimulated chlorophyll a fluorescence spectra, and particle backscattering spectra were modeled. The model was tested on 35 reflectance spectra obtained from irradiance measurements in optically diverse ocean waters (0.07 to 25.35 mg/cu m range in surface chlorophyll a concentrations). The universality of the model was demonstrated by the accurate estimation of the spectral phytoplankton absorption coefficents over a range of 3 orders of magnitude (rho = 0.94 at 500 nm). Under most oceanic conditions (chlorophyll a less than 3 mg/cu m) the percent difference between measured and modeled phytoplankton absorption coefficents was less than 35%. Spectral variations in measured phytoplankton absorption spectra were well predicted by the inverse model. Modeled volume fluorescence was weakly correlated with measured chl a; fluorescence quantum yield varied from 0.008 to 0.09 as a function of environment and incident irradiance. Modeled particle backscattering coefficients were linearly related to total particle cross section over a twentyfold range in backscattering coefficents (rho = 0.996, n = 12).

Roesler, Collin S.↗

Non-gray gas radiation effect on mixed convection in lid driven square cavity

A numerical study is performed to investigate the effect of non-gray radiation on mixed convection in a vertical two sided lid driven square cavity filled with air-H{sub 2}O-CO{sub 2} gas mixture. The vertical moving walls of the enclosure are maintained at two different but uniform temperatures. The horizontal walls are thermally insulated and considered as adiabatic walls. The governing differential equations are solved by a finite-volume method and the SIMPLE algorithm was adopted to solve the pressure–velocity coupling. The radiative transfer equation (RTE) is solved by the discrete ordinates method (DOM). The spectral line weighted sum of gray gases model (SLW) is used to account for non-gray radiation properties. Simulations are performed in configurations where thermal and shear forces induce cooperating buoyancy forces. Streamlines, isotherms, and Nusselt number are analyzed for three different values of Richardson’s number (from 0.1 to 10) and by considering three different medium (transparent medium, gray medium using the Planck mean absorption coefficient, and non-gray medium assumption).

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

UV-Vis Spectroscopy as a Tool for Safeguards; Instrumentation installation and fundamental data collection

Two spectrophotometric process monitors, one optimized for high concentration (approximately 10 g/L) and one for trace levels (approximately 10 ppm),were developed at Argonne and installed at the SRS H-Canyon facility for field testing. These systems were built of Commercial-Off-The-Shelf components utilizing a custom, facility-specific hardware interface. The systems directly provide a qualitative measurement of process chemistry (i.e. valence state). With appropriate calibrations the systems could provide quantitative data. Laboratory tests were performed to determine the spectrophotometric molar absorptivity coefficients for relevant actinide and transition metals of interest.

36 MATERIALS SCIENCE↗

Detection of volcanic eruptions from space by their sulfur dioxide clouds

The capabilities of the total ozone mapping spectrometer (TOMS) on the Nimbus 7 satellite for tracking volcano plumes are assessed. TOMS was installed on the sun-synchronous polar orbiting satellite to measure spatial variations in the global total ozone field. Radiance absorption coefficients of the atmosphere for four near-UV wavelengths from 312.5-380.0 are measured. Data from the El Chichon eruption in March-April 1982 revealed that SO2 was an absorbing species at 312.5 and 317.5 nm. The near-UV absorption level differences between SO2 and O3 permit discriminating the atmospheric densities of each species. An examination of the data base generated by TOMS since 1978 showed the perceptible tracks of all known major eruptions in the 1978-1982 time period. A constellation of three of the polar orbiting TOMS would be sufficient to provide near-real time alerts of plumes to warn aircraft of the hazards.

Krueger, A. J.↗

Radio observations of the planets - The importance of laboratory measurements

Laboratory data on the line broadening parameters of H2S gas under Uranian/Neptunian conditions, on the far wings of the H2S and NH3 line profiles, and on the dielectric properties of CH4-, NH3-, H2S-, and NH4SH-ice are needed to constrain elemental abundances and understand the dynamics and cloud physics in the atmospheres of the giant planets. Measurements of the absorption coefficient of gaseous H2SO4 at millimeter wavelengths are needed in order to obtain a better understanding of Venus' atmosphere. To determine wind velocity fields in Venus' and Mars' atmospheres, accurate measurements of the center frequencies of the CO lines are necessary. The absorption and scattering properties of lunar soils and/or terrestrial rock powders at frequencies from approximately 1 to 200 GHz, determined in laboratory experiments, would provide a valuable addition to existing data at 450 MHz, 35 GHz, and far infrared frequencies. These data would be used to analyze the microwave spectra of planetary surfaces. Such studies may be helpful in distinguishing the effects of radiative transfer from those of nonlinear heat conduction and internal heat sources.

De Pater, Imke↗

Structure and optical properties of ZnO with silver nanoparticles

Textured nanocrystalline ZnO thin films are synthesized by ion beam assisted deposition. According to X-ray diffraction data, the crystallite size is ∼25 nm. Thin (∼15 nm) ZnO layers containing Ag nanoparticles are formed in a thin surface region of the films by the implantation of Ag ions with an energy of 30 keV and a dose in the range (0.25–1) × 10{sup 17} ion/cm{sup 2}. The structure and optical properties of the layers are studied. Histograms of the size distribution of Ag nanoparticles are obtained. The average size of the Ag nanoparticles varies from 0.5 to 1.5–2 nm depending on the Ag-ion implantation dose. The optical transmittance of the samples in the visible and ultraviolet regions increases, as the implantation dose is increased. The spectra of the absorption coefficient of the implanted films are calculated in the context of the (absorbing film)/(transparent substrate) model. It is found that the main changes in the optical-density spectra occur in the region of ∼380 nm, in which the major contribution to absorption is made by Ag nanoparticles smaller than 0.75 nm in diameter. In this spectral region, absorption gradually decreases, as the Ag-ion irradiation dose is increased. This is attributed to an increase in the average size of the Ag nanoparticles. It is established that the broad surface-plasmon-resonance absorption bands typical of nanocomposite ZnO films with Ag nanoparticles synthesized by ion implantation are defined by the fact that the size of the nanoparticles formed does not exceed 1.5–2 nm.

36 MATERIALS SCIENCE↗