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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Understanding Relationships between Free Volume and Oxygen Absorption in Ionic Liquids

In this report understanding the factors that govern gas absorption in ionic liquids is critical to the development of high-capacity solvents for catalysis, electrochemistry, and gas separations. Here, we report experimental probes of liquid structure that provide insights into how free volume impacts the O 2 absorption properties of ionic liquids. Specifically, we establish that isothermal compressibility - measured rapidly and accurately through small-angle X-ray scattering - reports on the size distribution of transient voids within a representative series of ionic liquids and is correlated with O 2 absorption capacity. Additionally, O 2 absorption capacities are correlated with thermal expansion coefficients, reflecting the beneficial effect of weak intermolecular interactions in ionic liquids on free volume and gas absorption capacity. Molecular dynamics simulations show that the void size distribution - in particular, the probability of forming larger voids within an ionic liquid - has a greater impact on O 2 absorption than the total free volume. These results establish relationships between the ionic liquid structure and gas absorption properties that offer design strategies for ionic liquids with high gas solubilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Dynamic absorption in optical pyrometry of hot spots in plastic-bonded triaminotrinitrobenzene [Optical Pyrometry of Shock-induced Hot Spots in Plastic-bonded Triaminotrinitrobenzene]

Herein we demonstrate a methodology for measuring optical pyrometry in environments which are disadvantageous for typical pyrometery applications by introducing additional fit parameters to account for absorption or emission which convolutes the thermal spectrum. Emission spectra from a plastic-bonded formulation of triaminotrinitrobenzene (TATB) shocked by 2-4 km s -1 impacts with Al flyer plates show significant deviations from graybody behavior. To extract reliable temperatures via optical pyrometry, we fit the spectra to a combination of a graybody and either a Gaussian absorption or emission spectrum. We found that the absorption needed to fit the data corresponds well with the known pressure-dependent absorption of TATB, and that the absorption model gives temperatures and emissivities in line with other explosives. By contrast, emission gives temperatures too low and emissivities that decrease as more material reacts. We conclude the nonthermal part of the spectrum is dominated by the absorption of unreacted TATB, and accurate pyrometry of TATB must use either our graybody plus absorption model or must limit the spectral range of observation to above 650 nm.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Plasmonic absorption-induced haze suppression in random scattering media

Light propagation in random scattering media is a common phenomenon in many scientific and engineering fields. Because of light-matter interaction, part of the light transmitted through a random scattering medium is diffuse and causes haze. Previous approaches to manipulate haze in random media mainly focused on regulating scattering and paid little attention to absorption. In this work, we present a comprehensive analysis of absorption-scattering coupling as well as its impact on haze in random media. We introduce the haze-absorption sensitivity (HAS) spectrum, an intrinsic property of a scattering medium that quantifies the potential of absorption-induced haze suppression. We also investigate the effect of scatterer geometry and concentration on the HAS spectrum. To experimentally demonstrate the effect of absorption in random media, we utilized the plasmonic absorption of silver and gold nanoparticles to reduce haze in a silica nanoparticle aqueous solution as the scattering medium. We showed that 15% (absolute) of haze suppression is possible by carefully choosing the optimal absorber. The experimental results closely matched the theoretical predictions. This work provides new understandings of absorption and scattering coupling in random media. The fundamental mechanisms elucidated in this work can offer new pathways for regulating haze in a variety of random scattering media.

Zhao, Lin (ORCID:000000028865859X)↗
DOE OSTI2022

FLASH pilot survey: detections of associated 21 cm H i absorption in GAMA galaxies at 0.42 < z < 1.00

ABSTRACT We present the results of a search for associated 21 cm H i absorption at redshift 0.42 < z < 1.00 in radio-loud galaxies from three Galaxy And Mass Assembly (GAMA) survey fields. These observations were carried out as part of a pilot survey for the Australian SKA Pathfinder (ASKAP) First Large Absorption Survey in H i (FLASH). From a sample of 326 radio sources with 855.5 MHz peak flux density above 10 mJy, we detected two associated H i absorption systems, in SDSS J090331+010847 at z = 0.522 and SDSS J113622+004852 at z = 0.563. Both galaxies are massive (stellar mass $\gt 10^{11}\, \mathrm{M}_\odot$) and have optical spectra characteristic of luminous red galaxies, though spectral energy distribution fitting implies that SDSS J113622+004852 contains a dust-obscured starburst with star formation rate ∼69 M⊙ yr−1. The H i absorption lines have a high optical depth, with τpk of 1.77 ± 0.16 for SDSS J090331+010847 (the highest value for any z > 0.1 associated system found to date) and 0.14 ± 0.01 for SDSS J113622+004852. In the redshift range probed by our ASKAP observations, the detection rate for associated H i absorption lines (with τpk > 0.1 and at least 3σ significance) is $2.9_{-2.6}^{+9.7}$ per cent. Although the current sample is small, this rate is consistent with a trend seen in other studies for a lower detection rate of associated 21 cm H i absorption systems at higher redshift. We also searched for OH absorption lines at 0.67 < z < 1.34, but no detection was made in the 145 radio sources searched.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Perfect absorption in GaAs metasurfaces near the bandgap edge

Perfect optical absorption occurs in a metasurface that supports two degenerate and critically-coupled modes of opposite symmetry. The challenge in designing a perfectly absorbing metasurface for a desired wavelength and material stems from the fact that satisfying these conditions requires multi-dimensional optimization often with parameters affecting optical resonances in non-trivial ways. This problem comes to the fore in semiconductor metasurfaces operating near the bandgap wavelength, where intrinsic material absorption varies significantly. Here we devise and demonstrate a systematic process by which one can achieve perfect absorption in GaAs metasurfaces for a desired wavelength at different levels of intrinsic material absorption, eliminating the need for trial and error in the design process. Using this method, we show that perfect absorption can be achieved not only at wavelengths where GaAs exhibits high absorption, but also at wavelengths near the bandgap edge. In this region, absorption is enhanced by over one order of magnitude compared a layer of unstructured GaAs of the same thickness.

Hale, L. L. (ORCID:0000000176544272)↗
DOE OSTI2019

Space Telescope and Optical Reverberation Mapping Project. VIII. Time Variability of Emission and Absorption in NGC 5548 Based on Modeling the Ultraviolet Spectrum

We model the ultraviolet spectra of the Seyfert 1 galaxy NGC 5548 obtained with the Hubble Space Telescope during the 6 month reverberation mapping campaign in 2014. Our model of the emission from NGC 5548 corrects for overlying absorption and deblends the individual emission lines. Using the modeled spectra, we measure the response to continuum variations for the deblended and absorption-corrected individual broad emission lines, the velocity-dependent profiles of Ly$α$ and C iv, and the narrow and broad intrinsic absorption features. We find that the time lags for the corrected emission lines are comparable to those for the original data. The velocity-binned lag profiles of Ly$α$ and C iv have a double-peaked structure indicative of a truncated Keplerian disk. The narrow absorption lines show a delayed response to continuum variations corresponding to recombination in gas with a density of ~10 5 cm -3 . The high-ionization narrow absorption lines decorrelate from continuum variations during the same period as the broad emission lines. Analyzing the response of these absorption lines during this period shows that the ionizing flux is diminished in strength relative to the far-ultraviolet continuum. The broad absorption lines associated with the X-ray obscurer decrease in strength during this same time interval. The appearance of X-ray obscuration in ~2012 corresponds with an increase in the luminosity of NGC 5548 following an extended low state. We suggest that the obscurer is a disk wind triggered by the brightening of NGC 5548 following the decrease in size of the broad-line region during the preceding low-luminosity state.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Light Absorption by Brown Carbon over the South-East Atlantic Ocean

Biomass burning emissions often contain brown carbon (BrC), which represents a large family of light-absorbing organics that is chemically complex and therefore difficult to estimate their absorption of incoming solar radiation, resulting in large uncertainties in the estimation of the global direct radiative effect of aerosols. Here we investigate the contribution of BrC to the total light absorption of biomass burning aerosols over the South-East Atlantic Ocean with different optical models utilizing a suite of airborne measurements from the ORACLES 2018 campaign by introducing an effective refractive index of black carbon (BC), m eBC = n eBC +ik eBC , that accounts for all possible absorbing components at 660 nm wavelength to facilitate the attribution of absorption at shorter wavelengths. Most values of the imaginary part of the refractive index, k eBC , were larger than those commonly used for BC from biomass burning emissions, suggesting contributions from absorbers beyond BC at 660 nm. The TEM-EDX single particle analysis further suggests that these long-wavelength absorbers might include iron oxides, as iron is found to be present only when large values of k eBC are derived. Using this effective BC refractive index, we find that the contribution of BrC to the total absorption at 470 nm (R BrC,470 ) ranges from ~5–15 %, with the organic aerosol mass absorption coefficient (MAC OA,470 ) at this wavelength ranging from 0.25 ± 0.34 m 2 g -1 to 0.43 ± 0.12 m 2 g -1 . The core-shell model yielded much higher estimates of MAC OA,470 and R BrC,470 than homogeneous mixing models, underscoring the importance of model treatment. Another key finding was that estimates of the BrC contribution at 470 nm from the commonly used AAE (absorption Ångström exponent) attribution method (< 5 %) are much lower than the BrC contribution estimates (R BrC,470 ) using our new methodology that accounts for contributions from both BrC and non-carbonaceous, long-wavelength absorbers, such as magnetite. Thus, it is recommended that application of any optical properties-based attribution method use absorption coefficients at the longest possible wavelength to minimize the influence of BrC at the long wavelength and to account for potential contributions from other absorbing materials.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1973

Fine structure in the optical-absorption edge of silicon.

Investigation of the dependence of the photocurrent generated in silicon p-n junctions on the energy of the incident photons to obtain details concerning the fine structure in the indirect optical-absorption edge of silicon. It is found that at room temperature there are three prominent thresholds in the absorption tail. The first, which is not too well defined, occurs at 0.91 eV, the second at 0.99 eV, and the third at 1.026 eV. The dependence of the absorption coefficient on the photon energy following the latter two thresholds is found to differ from that found by Mcfarlane et al. (1958). The threshold energies and temperature dependence of the absorption coefficient suggest that two- and three-phonon processes give rise to the absorption tail. In the transverse-optical phonon-absorption region more structure is found in the absorption coefficient than is accounted for by the theory.

Anagnostopoulos, C.↗
NASA NTRS1978

The line-locking hypothesis, absorption by intervening galaxies, and the z = 1.95 peak in redshifts

The controversy over whether the absorption spectrum in QSOs is intrinsic or extrinsic is approached with attention to the peak of redshifts at z = 1.95. Also considered are the line-locking and the intervening galaxy hypotheses. The line locking hypothesis is based on observations that certain ratios found in absorption line QSOs are preferred, and leads inevitably to the conclusion that the absorption line systems are intrinsic. The intervening galaxy hypothesis is based on absorption redshifts resulting from given absorption cross-sections of galactic clusters and the intergalactic medium, and would lead to the theoretical conclusion that most QSOs show strong absorption, a conclusion which is not supported by empirical data. The 1.95 peak, on the other hand, is most probably an intrinsic property of QSOs. The peak is enhanced by redshift, and it is noted that both an emission and an absorption redshift peak are seen at 1.95.

Burbidge, G.↗
NASA NTRS1980

Absorption-line spectra of quasi-stellar objects - Physical properties of absorbing gas

The optical absorption lines of quasars are examined, and implications of the lines for the physical properties of the absorbing gas are discussed. Consideration is given to the characteristics of broad absorption lines observed in such quasars as PHL 5200 and Q 1246-057 and of the more prevalent extremely narrow lines, with discussion of the presumed physical conditions in the absorbing gas and the distribution of absorption-line redshifts with respect to emission-line redshifts. It is pointed out that absorption features become more prevalent in quasar spectra with emission redshifts greater than 2.3, and results of studies of column densities and abundances and of the presence of absorption in radio compact quasars are indicated. Research programs currently under way are then described, including a search for the distribution of absorption lines in a fixed wavelength range less than the Lyman alpha emission wavelength, study of low absorption-redshift systems, a study of individual objects such as the quasar pair 1548+114a and b, and various theoretical investigations.

Burbidge, E. M.↗
NASA NTRS1985

Ultraviolet interstellar absorption toward stars in the Small Magellanic Cloud. IV - Highly ionized gas associated with the Small Magellanic Cloud

High-dispersion International Ultraviolet Explorer satellite spectra of seven stars in the Small Magellanic Cloud (SMC) are examined to study the properties of interstellar C IV and Si IV absorption in the SMC. Absorption by C IV or Si IV or both is found near 160 km/s for all the stars. The velocity and the relative C IV and Si IV strengths suggest UV-photoionized nebular gas as the origin of this absorption. In addition, the stars show absorption by C IV and, sometimes, Si IV in the velocity range 100-130 km/s. This velocity is 30-60 km/s more negative than that expected for normal nebular gas, and the relative C IV and Si IV strengths indicate an ionization source other than stellar UV photoionization by normal Population I stars. Possible global origins are considered for this absorption, including a hot phase of the SMC interstellar medium and a circum-SMC distribution of highly ionized gas. The only detection of interstellar N V toward a SMC star is for HD 5980. The line is broad, possibly complex, and spans the velocity range of the nebular absorption and the 100-130 km/s absorption.

Fitzpatrick, E. L.↗
NASA NTRS1990

Deconvolution of mineral absorption bands - An improved approach

Although visible and near IR reflectance spectra contain absorption bands that are characteristic of the composition and structure of the absorbing species, deconvolving a complex spectrum is nontrivial. An improved approach to spectral deconvolution is presented that accurately represents absorption bands as discrete mathematical distributions and resolves composite absorption features into individual absorption bands. The frequently used Gaussian model of absorption bands is shown to be inappropriate for the Fe(2+) electronic transition absorptions in pyroxene spectra. A modified Gaussian model is derived using a power law relationship of energy to average bond length. The modified Gaussian model is shown to provide an objective and consistent tool for deconvolving individual absorption bands in the more complex orthopyroxene, clinopyroxene, pyroxene mixtures, and olivine spectra.

Sunshine, Jessica M.↗
NASA NTRS1990

Radio line and continuum observations of quasar-galaxy pairs and the origin of low reshift quasar absorption line systems

There are a number of known quasars for which our line of sight to the high redshift quasar passes within a few Holmberg radii of a low redshift galaxy. In a few of these cases, spectra of the quasar reveal absorption by gas associated with the low redshift galaxy. A number of these pairs imply absorption by gas which lies well outside the optical disk of the associated galaxy, leading to models of galaxies with 'halos' or 'disks' of gas extending to large radii. The authors present observations of 4 such pairs. In three of the four cases, they find that the associated galaxy is highly disturbed, typically due to a gravitational interaction with a companion galaxy, while in the fourth case the absorption can be explained by clouds in the optical disk of the associated galaxy. They are led to an alternative hypothesis concerning the origin of the low redshift absorption line systems: the absorption is by gas clouds which have been gravitationally stripped from the associated galaxy. These galaxies are rapidly evolving, and should not be used as examples of absorption by clouds in halos of field spirals. The authors conclude by considering the role extended gas in interacting systems plays in the origin of higher redshift quasar absorption line systems.

Carilli, C. L.↗
NASA NTRS1992

Detection of Ca II absorption in the QSO 0958 + 559 due to a Heiles shell in NGC 3079

Optical observations of the QSO 0958 + 559 and the nearby, edge-on spiral galaxy NGC 3079 are presented. Spectra of the QSO show Ca II absorption lines due to extended gas in NGC 3079; the Na absorption lines due to NGC 3079 are not detected. An unrelated higher redshift absorption system at 1.1327 is also present in the QSO spectrum. The QSO sightline shines directly through a Heiles shell. The coincidence in position coupled with the agreement between the Ca II absorption and shell emission velocities demonstrates that the QSO absorption system is due to gas in this shell. This system is discussed in comparison with the six other low-redshift QSO-galaxy pair absorption systems, and the influence of Heiles shells on the interpretation of higher redshift QSO absorption systems is addressed.

Womble, Donna S.↗
NASA NTRS1993

Theoretical calculations on the electron absorption spectra of selected Polycyclic Aromatic Hydrocarbons (PAH) and derivatives

As a theoretical component of the joint effort with the laboratory of Dr. Lou Allamandola to search for potential candidates for interstellar organic carbon compound that are responsible for the visible diffuse interstellar absorption bands (DIB's), quantum mechanical calculations were performed on the electron absorption spectra of selected polycyclic aromatic hydrocarbons (PAH) and derivatives. In the completed project, 15 different species of naphthalene, its hydrogen abstraction and addition derivatives, and corresponding cations and anions were studied. Using semiempirical quantum mechanical method INDO/S, the ground electronic state of each species was evaluated with restricted Hartree-Fock scheme and limited configuration interaction. The lowest energy spin state for each species was used for electron absorption calculations. Results indicate that these calculations are accurate enough to reproduce the spectra of naphthalene cation and anion observed in neon matrix. The spectral pattern of the hydrogen abstraction and addition derivatives predicted based on these results indicate that the electron configuration of the pi orbitals of these species is the dominant determinant. A combined list of 19 absorptions calculated from 4500 A to 10,400 A were compiled and suggested as potential candidates that are relevant for the DIB's absorptions. Continued studies on pyrene and derivatives revealed the ground state symmetries and multiplicities of its neutral, anionic, and cationic species. Spectral calculations show that the cation (B(sub 3g)-2) and the anion (A(sub u)-2) are more likely to have low energy absorptions in the regions between 10 kK and 20 kK, similar to naphthalene. These absorptions, together with those to be determined from the hydrogen abstraction and addition derivatives of pyrene, can be used to provide additional candidates and suggest experimental work in the search for interstellar compounds that are responsible for DIB's.

Du, Ping↗
NASA NTRS1993

Clear evidence for the presence of O VI absorption in QSO metal systems

We have detected O VI 1031.93 A, 1037.62 A doublet absorption in a composite QSO spectrum formed from a large number of intervening C IV absorption systems. The detections constitute the first firm evidence for the presence of O VI in intervening QSO metal absorption systems. The equivalent width of the detected O VI absorption implies an O VI column density N(O VI) not less than 2.8 x 10 exp 14/sq cm. This value, together with the nondetection of the N V 1238.82 A, 1242.80 A doublet absorption, suggests that N(O VI)/N(N V) not less than 4.4. For collisionally ionized gas with a solar O to N abundance ratio in thermal equilibrium the above ratio requires a temperature T not less than 2.5 x 10 exp 5 K. It is found that C IV systems which show low-ionization species and those which do not both have associated O VI absorption, suggesting that O VI is probably present in all C IV systems. We also find that C IV systems which show low-ionization species on average have stronger high-ionization absorption lines than those which do not. A simple interpretation was given to explain this trend.

Lu, Limin↗
NASA NTRS1993

Damped Lyman-alpha absorption by disk galaxies with large redshifts. IV - More intermediate-resolution spectroscopy

Intermediate-resolution spectra of six QSOs exhibiting seven Ly-alpha absorption troughs that are candidates for damped Ly-alpha absorption lines are presented. The metal content of the confirmed damped systems is investigated by examining the metal-line velocity profiles, and by performing curve-of-growth analyses for four of the six confirmed damped systems. The low-ionization lines associated with the z(metals) = 2.0399 damped system toward Q0458-020 have velocity widths up to 10 times wider than the width of the 21-cm absorption feature found at the same redshift. Since the 21-cm absorption arises in a low velocity dispersion layer of H I that extends more than 8/h kpc transverse to the line of sight, the H I absorption cannot arise from the same clouds responsible for the bulk of the metal-line absorption. This is strong evidence for a two-component model consisting of high column density 'quiescent' gas which gives rise to damped Ly-alpha and 21-cm absorption, and low column density 'turbulent' gas which dominates equivalent widths of saturated metal lines.

Wolfe, Arthur M.↗
NASA NTRS1994

A model predicting the evolution of ice particle size spectra and radiative properties of cirrus clouds. Part 2: Dependence of absorption and extinction on ice crystal morphology

This study builds upon the microphysical modeling described in Part 1 by deriving formulations for the extinction and absorption coefficients in terms of the size distribution parameters predicted from the micro-physical model. The optical depth and single scatter albedo of a cirrus cloud can then be determined, which, along with the asymmetry parameter, are the input parameters needed by cloud radiation models. Through the use of anomalous diffraction theory, analytical expressions were developed describing the absorption and extinction coefficients and the single scatter albedo as functions of size distribution parameters, ice crystal shapes (or habits), wavelength, and refractive index. The extinction coefficient was formulated in terms of the projected area of the size distribution, while the absorption coefficient was formulated in terms of both the projected area and mass of the size distribution. These properties were formulated as explicit functions of ice crystal geometry and were not based on an 'effective radius.' Based on simulations of the second cirrus case study described in Part 1, absorption coefficients predicted in the near infrared for hexagonal columns and rosettes were up to 47% and 71% lower, respectively, than absorption coefficients predicted by using equivalent area spheres. This resulted in single scatter albedos in the near-infrared that were considerably greater than those predicted by the equivalent area sphere method. Reflectances in this region should therefore be underestimated using the equivalent area sphere approach. Cloud optical depth was found to depend on ice crystal habit. When the simulated cirrus cloud contained only bullet rosettes, the optical depth was 142% greater than when the cloud contained only hexagonal columns. This increase produced a doubling in cloud albedo. In the near-infrared (IR), the single scatter albedo also exhibited a significant dependence on ice crystal habit. More research is needed on the geometrical properties of ice crystals before the influence of ice crystal shape on cirrus radiative properties can be adequately understood. This study provides a way of coupling the radiative properties of absorption, extinction, and single scatter albedo to the microphysical properties of cirrus clouds. The dependence of extinction and absorption on ice crystal shape was not just due to geometrical differences between crystal types, but was also due to the effect these differences had on the evolution of ice particle size spectra. The ice particle growth model in Part 1 and the radiative properties treated here are based on analytical formulations, and thus represent a computationally efficient means of modeling the microphysical and radiative properties of cirrus clouds.

Mitchell, David L.↗