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At least 145 records · Page 8

Spectroscopic signatures and oxidation characteristics of nanosecond laser-induced cerium plasmas

Improving technologies related to the wide area environmental sampling of nuclear materials supports the nuclear nonproliferation mission of preventing the proliferation of nuclear weapons by monitoring nuclear weapons tests and detecting undeclared nuclear fuel cycle activities. Standoff, laser-based detection techniques such as laser-induced breakdown spectroscopy have the potential to offer robust, field-deployable methods that provide rapid element-specific and phase identifiable measurements over a wide range of materials. This work aims to elucidate the effects of atmospheric conditions and oxidation reactions on the highly complex and transient spectroscopic signatures of laser-induced plutonium surrogate plasmas. Time-resolved spectra of nanosecond laser ablation cerium plasmas were measured using laser-induced breakdown spectroscopy in a range of atmospheres containing low to high concentrations of oxygen. Here, the growth of strong CeO molecular emission bands was observed in the visible spectrum, where it was shown that the persistence of CeO is reduced from around 60 μs to 50 μs in oxygen rich atmospheric environments. To further investigate the growth and depletion of CeO in the laser-produced plasma, ratios of CeO-to-Ce emission were generated using integrated intensities corresponding to the Q-branch of the CeO D 1 -X 1 transitions and numerous strong atomic Ce peaks. It was determined that the fastest rate of formation of CeO in argon occurred for moderate oxygen mass fractions between 0.10 and 0.15 while the ratios were reduced at higher oxygen mass fractions (i.e., Y O 2 = 0.20) due to competing oxidation reactions and lower plasma temperatures.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

A new measurement of the flux of the light cosmic-ray nuclei at high energies

A new cosmic-ray detector utilizing a ring-imaging Cerenkov counter to determine the energy of light cosmic-ray nuclei was flown on high-altitude balloon from Fort Sumner, NM, in 1991 September. We describe the design and performance of this instrument and discuss the data analysis procedures. The measurement provides a new determination of the absolute flux and differential energy spectrum of the primary cosmic-ray species helium between 40 and 320 GeV/nucleon. The experiment also yields the spectra of carbon and oxygen and some information on the intensities of the secondary nuclei Li, Be, and B. A comparison between our results and previous measurements of heavier nuclei (Z greater than or equal to 4) from HEAO 3 and Spacelab 2 indicates good consistency between these measurements. The data set is compared with the results of a leaky box propagation model. We find good agreement with this model if the abundance of helium relative to oxygen at the source is taken to be 25 +/- 6 and if the source spectrum is given by a power law in energy proportional to E(exp -2.15).

Buckley, J.↗

Ultrafast laser filament-induced fluorescence for detecting uranium stress in Chlamydomonas reinhardtii

Abstract Plants and other photosynthetic organisms have been suggested as potential pervasive biosensors for nuclear nonproliferation monitoring. We demonstrate that ultrafast laser filament-induced fluorescence of chlorophyll in the green alga Chlamydomonas reinhardtii is a promising method for remote, in-field detection of stress from exposure to nuclear materials. This method holds an advantage over broad-area surveillance, such as solar-induced fluorescence monitoring, when targeting excitation of a specific plant would improve the detectability, for example when local biota density is low. After exposing C. reinhardtii to uranium, we find that the concentration of chlorophyll a, chlorophyll fluorescence lifetime, and carotenoid content increase. The increased fluorescence lifetime signifies a decrease in non-photochemical quenching. The simultaneous increase in carotenoid content implies oxidative stress, further confirmed by the production of radical oxygen species evidence in the steady-state absorption spectrum. This is potentially a unique signature of uranium, as previous work finds that heavy metal stress generally increases non-photochemical quenching. We identify the temporal profile of the chlorophyll fluorescence to be a distinguishing feature between uranium-exposed and unexposed algae. Discrimination of uranium-exposed samples is possible at a distance of $$\sim $$ ∼ 35 m with a single laser shot and a modest collection system, as determined through a combination of experiment and simulation of distance-scaled uncertainty in discriminating the temporal profiles. Illustrating the potential for remote detection, detection over 125 m would require 100 laser shots, commensurate with the detection time on the order of 1 s.

54 ENVIRONMENTAL SCIENCES↗

Apparent electrostatic ion cyclotron waves in the diffuse aurora

Emissions that have properties consistent with electrostatic ion cyclotron (EIC) waves have been observed at low altitude in the diffuse aurora by a sounding rocket payload. Peaks were observed in the power spectrum of the electric field near the hydrogen and oxygen ion cyclotron frequencies. Doppler shift and polarization analyses have been performed using EIC wave parameters derived from linear theory. Both analyses indicated that these emissions had properties consistent with those expected for H(+) and O(+) EIC waves. The two analyses indicated that both emission bands were due to waves propagating eastward parallel to the poleward boundary of the diffuse aurora. The large local cold plasma density and resulting Landau damping require that the source be local. Magnetometer data indicated the presence of a downward parallel current density of 5 microamps/sq m. Sufficient free energy for the waves was available from this current, although the waves were observed frequently at altitudes where the ion-neutral collision frequency exceeded the oxygen cyclotron frequency.

Bering, E. A.↗

Observations of two peculiar emission objects in the Large Magellanic Cloud

Ultraviolet and visual wavelength spectra were obtained of two peculiar emission objects, Henize S63 and Sanduleak's star in the Large Magellanic Cloud. Previously not observed in the near- or far-ultraviolet, both objects exhibit strong permitted and semiforbidden line emissions. Estimates based on the absolute continuum flux of the hot companion star in Hen S63 indicate that it rivals the luminosity of the carbon star primary. The emission-line profile structure in both objects does not suggest Wolf-Rayet type emission. Carbon in Sanduleak's star (LMC anonymous) is conspicuously absent, while N V, semiforbidden N IV, and semiforbidden N III dominate the UV emission-line spectrum. Nitrogen is overabundant with respect to carbon and oxygen in both objects. The large overabundance of nitrogen in Sanduleak's star suggests evidence for CNO processes material similar to that seen in Nu Car.

Kafatos, M.↗

Balloon-based interferometric techniques

A balloon-borne triple-etalon Fabry-Perot Interferometer, observing the Doppler shifts of absorption lines caused by molecular oxygen and water vapor in the far red/near infrared spectrum of backscattered sunlight, has been used to evaluate a passive spaceborne remote sensing technique for measuring winds in the troposphere and stratosphere. There have been two successful high altitude balloon flights of the prototype UCL instrument from the National Scientific Balloon Facility at Palestine, TE (May 80, Oct. 83). The results from these flights have demonstrated that an interferometer with adequate resolution, stability and sensitivity can be built. The wind data are of comparable quality to those obtained from operational techniques (balloon and rocket sonde, cloud-top drift analysis, and from the gradient wind analysis of satellite radiance measurements). However, the interferometric data can provide a regular global grid, over a height range from 5 to 50 km in regions of clear air. Between the middle troposphere (5 km) and the upper stratosphere (40 to 50 km), an optimized instrument can make wind measurements over the daylit hemisphere with an accuracy of about 3 to 5 m/sec (2 sigma). It is possible to obtain full height profiles between altitudes of 5 and 50 km, with 4 km height resolution, and a spatial resolution of about 200 km, along the orbit track. Below an altitude of about 10 km, Fraunhofer lines of solar origin are possible targets of the Doppler wind analysis. Above an altitude of 50 km, the weakness of the backscattered solar spectrum (decreasing air density) is coupled with the low absorption crosssection of all atmospheric species in the spectral region up to 800 nm (where imaging photon detectors can be used), causing the along-the-track resolution (or error) to increase beyond values useful for operational purposes. Within the region of optimum performance (5 to 50 km), however, the technique is a valuable potential complement to existing wind measuring systems and can provide a low cost addition to powerful active (LIDAR) wind measuring systems now under development.

Rees, David↗

X-ray Reflected Spectra from Accretion Disk Models. I. Constant Density Atmospheres

We present new models for illuminated accretion disks, their structure and reprocessed emission. We consider the effects of incident X-rays on the surface of an accretion disk by solving simultaneously the equations of radiative transfer, energy balance and ionization equilibrium over a large range of column densities. We assume plane-parallel geometry and azimuthal symmetry, such that each calculation corresponds to a ring at a given distance from the central object. Our models include recent and complete atomic data for K-shell of the iron and oxygen isonuclear sequences. We examine the effect on the spectrum of fluorescent Ka line emission and absorption in the emitted spectrum. We also explore the dependence of the spectrum on the strength of the incident X-rays and other input parameters, and discuss the importance of Comptonization on the emitted spectrum.

Garcia, Javier↗

Diurnal and Directional Responses of Chlorophyll Fluorescence and the PRI in a Cornfield

Determining the health and vigor of vegetation using high spectral resolution remote sensing is an important goal which has application to monitoring agriculture and ecosystem productivity and carbon exchange. Two spectral indices used to assess whether vegetation is performing near-optimally or exhibiting symptoms of environmental stress (e.g., drought or nutrient deficiency, non-optimal temperatures, etc.) are the Photochemical Reflectance Index (PRI) and solar-induced red and far-red Chlorophyll Fluorescence (Fs). Both the PRI and Fs capture the dynamics of photoprotection mechanisms within green foliage: the PRI is based on the association of the reflected radiation in the green spectrum with the xanthophyll cycle, whereas Fs measures the emitted radiation in the red and far-red spectrum. Fs was determined from retrievals in the atmospheric oxygen absorption features centered at 688 and 760 nm using a modified Fraunhofer Line Depth (FLD) method. We previously demonstrated diurnal and seasonal PRI differences for sunlit vs. shaded foliage in a conifer forest canopy, as expressed in the hotspot and darkspot of the Bidirectional Reflectance Function (BRF). In a USDA-ARS experimental field site located in Beltsville, MD, USA, measurements were acquired over a corn crop from a nadir view in 2008 with an ASD FieldSpec Pro (Analytical Spectral Devices, Inc., Boulder, CO, USA) to study the behavior of the PRI for sunlit and shaded foliage as captured in reflectance variations associated with the BRF, in a I m tall canopy in the vegetative growth stage. Those observations were compared to simulations obtained from two radiative transfer models. Measurements were then acquired to examine whether the PRI and Fs were influenced by view zenith and azimuth geometries at different times of day. Those measurements were made in 2010 with the Ocean Optics USB4000 Miniature Fiber Optic Spectrometer (Ocean Optics Inc., Dunedin, Florida, USA) at several times during the day on multiple days throughout the growing season. We found that the PRI consistently had higher values, indicating lower stress, in the BRF darkspot associated with shaded foliage than in the hotspot associated with sunlit foliage. We also found that Fs exhibited differences associated with sunlit and shaded canopy sectors, which were most pronounced for the red/far-red Fs ratio. Values indicated greater physiological stress in afternoons compared to mornings, and in the early senescent canopy as compared to the vegetative growth stage, BRFs for both the PRI and the red/far-red Fs ratio were bowl-shaped for the full azimuth sweep of the canopy. These two spectral indices (PRI, Fs ratio) provided complementary information on the photosynthetic function of the corn canopy.

Middleton, Elizabeth↗

High-efficiency oxygen reduction to hydrogen peroxide catalyzed by oxidized carbon materials

Improved electrochemical production of hydrogen peroxide is provided with a surface-oxidized carbon catalyst. The carbon can be, for example, carbon black or carbon nanotubes. The oxidation of the carbon can be performed, for example, by heating the carbon in nitric acid, or by heating the carbon in a base. The resulting carbon catalyst can have a distinctive oxygen is peak in its X-ray photoelectron spectrum.

Cui, Yi↗

The Composite Spectrum of QSO Absorption Line Systems in DESI DR2

We present details regarding the construction of a composite spectrum of quasar (QSO) absorption line systems. In this composite spectrum we identify more than 70 absorption lines, and observe oxygen and hydrogen emission features at a higher signal-to-noise ratio than in any previous study. As the light from a distant quasar travels towards an observer, it may interact with the circumgalactic medium environment of an intervening galaxy, forming absorption lines. In order to maximize the signal of these absorption lines, we have selected a sample of 238,838 quasar spectra from the second data release of the Dark Energy Spectroscopic Instrument (DESI), each identified to have absorption lines resulting from such an interaction. By stacking these spectra in the restframe of the absorption, and calculating a median composite spectrum, we are able to isolate and enhance these absorption lines. We provide a full atlas of all detected absorption and emission lines as well as their fit centroids and equivalent width values. This atlas should aid in future studies investigating the compositions and physical conditions of these absorbers.

Napolitano, Lucas [Wyoming U.] (ORCID:000000025166↗

Threshold Ionization Spectroscopy and Theoretical Calculations of LnO (Ln = La and Ce)

Mass-analyzed threshold ionization (MATI) spectroscopy was used to measure the vibronic spectra of LnO (Ln = La and Ce). Single-reference coupled cluster and relativistic multireference configuration calculations were carried out to compare with the measured vibronic energies. The spectrum of LaO displays a single vibronic band system, while that of CeO shows multiple ones. The ionization energies of LaO and CeO are measured as 5.2446 (6) and 5.3332(6) eV, respectively, which are a hundredfold improvement over the literature values. The vibrational energies of the neutral molecule and corresponding ion reveal the charge effect on the metal-oxygen bond of both species. The single band system in the spectrum of LaO arises from the transition of the ground state of the neutral molecule with the La(6s 1 )O(2p 6 ) valence configuration to the ground state of the singly charged ion with the La(6s o )O(2p 6 ) configuration. Here, the multiple band systems in the spectrum of CeO are attributed to the spin-orbit coupling for the Ce(4f 1 6s 1 )O(2p 6 ) configuration of the neutral molecule and an excited state for the Ce(4f 1 )O(2p 6 ) configuration of the ion.

74 ATOMIC AND MOLECULAR PHYSICS↗

Far UV camera/spectrograph

In March 1610, Galileo Galilei reported the first use of a telescope to view mountains and maria on the Moon. On April 21, 1972, the Apollo 16 commander pointed a somewhat more complex optical instrument at the Earth from the Moon and obtained several remarkable photographs showing atmospheric rather than surface features. The optical part of the far UV camera (aperture, 7.5 cm) was not much larger than Galileo's telescope. Like his, this instrument was also pointed at other celestial objects that Galileo viewed, including the Milky Way and Jupiter, and the Large Magellanic Cloud (LMC), which is not visible from Italy. More important, the far UV camera/spectrograph recorded light in the invisible band of wavelengths between 50 and 160 nm, approximately one-third the wavelength that can penetrate the atmosphere of the Earth to ground-based telescopes. As described in more detail in this section, these UV observations from the Moon allow study of the entire atmosphere of the Earth and the geocorona. The photographs show hydrogen and other gases in the solar wind and interplanetary media, and they provide new data on stars, nebulae, and galaxies much farther away. When used as a spectrograph, the instrument distributes the light it receives according to wavelength, and the resulting spectrum shows bright lines or gaps known to be characteristic of various gases, such as hydrogen (H), helium (He), oxygen (O), nitrogen (N), and neon (Ne). If a gas cloud is hot, the atoms are excited and the spectrum shows bright emission lines; if it is cool, the atoms absorb light, leaving gaps or absorption lines. The far UV camera is blind to ordinary visible light; for that reason, the photographs show very few of the stars mapped by ground-based telescopes. Only the very-high-temperature (blue) stars of spectral classes O, B, and possibly A (temperatures from 50000 ° down to 10000°K) are expected to be recorded. Image blackness or density on the negatives also depends on the brightness of the star, which astronomers measure in an inverted logarithmic scale of magnitudes. A star of 6 magnitudes (mag.) can barely be seen with the unaided eye. An 11-mag. star is 100 times fainter, and a 12-mag. star is 2.5 times fainter yet. The faintest star recorded by the far UV camera is at least 11 mag., which is called the limiting magnitude.

George R. Carruthers↗

Effect of 60 Co γ-radiation on the tetrafluoroethylene/perfluoro(methyl vinyl ether) copolymer

The chemical and paramagnetic composition of the surface of the tetrafluoroethylene / perfluoro(methyl vinyl ether) copolymer (MFA) was investigated before and after γ-irradiation. The content of fluorine and carbon decreases at radiolysis of MFA, as well as the proportion of oxygen increases as a result of the oxidation reaction of radicals formed during γ-irradiation. The electron paramagnetic resonance (EPR) spectrum of the copolymer irradiated at 77 K contains the radicals ~CF 2 C∙FCF 2 ~ (1) and >CFOC∙F 2 (2). The absence of ~CF 2 C∙F 2 radicals, which can be formed at radiolytic rupture of the C—C bond of the copolymer main chain is associated with the effect of recombination of the resulting radical pair. The EPR spectrum of irradiated MFA at 300 K only recorded radical (1), which transform into peroxide radicals when air oxygen is introduced into the irradiated sample. Thermomechanical curves of native and radiolyzed MFA show three structural states of the amorphous block (glass, transition region, plateau of highly elastic deformation), as well as melting and molecular flow of the copolymer. The radio thermoluminescence curve shows five maxima associated with the emission of light during the recombination of stabilized ions and radicals during heating of the pre-irradiated MFA at 77 K. The temperature of the luminescence peak maximum at 336 K is close to the temperature of the onset of the devitrification of the chains of the amorphous block of MFA on the thermomechanical curve at 341 K. Irradiation leads to an increase in crystallinity of MFA. The heat of fusion of irradiated MFA on the Differential Scanning Calorimeter (DSC) curve is 50 % higher than the fusion heat of native copolymer. During the heating of γ-irradiated MFA, the relative content of COF molecules in the thermal decomposition products increases by an order of magnitude.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Excitation of MHD waves upstream of Jupiter by energetic sulfur or oxygen ions

Large fluxes of heavy ions have been reported upstream of Jupiter's bow shock as Voyager 1 approached the planet (Zwickl et al., 1981; Krimigis et al., 1985). Enhanced low-frequency magnetic wave activity was also observed during the particle events. The fluctuations are left-handed, elliptically polarized in the plasma frame. The spectrum of these fluctuations contains a peak close to the Doppler-shifted resonance frequency of a sulfur or oxygen beam with streaming energy of approximately 30 keV. These fluctuations are also present in the spectrum of the magnitude of the field. It is concluded that the observations result from an instability driven by an energetic beam of either sulfur or oxygen. The wave observations can be described by a heavy ion distribution with both a streaming anisotropy and a temperature anisotropy. This class of heavy ion streaming instabilities may also play a role in wave-particle interactions in the vicinity of comets.

Goldstein, M. L.↗

Atomic Oxygen Abundance in Molecular Clouds: Absorption Toward Sagittarius B2

We have obtained high-resolution (approximately 35 km/s) spectra toward the molecular cloud Sgr B2 at 63 micrometers, the wavelength of the ground-state fine-structure line of atomic oxygen (O(I)), using the ISO-LWS instrument. Four separate velocity components are seen in the deconvolved spectrum, in absorption against the dust continuum emission of Sgr B2. Three of these components, corresponding to foreground clouds, are used to study the O(I) content of the cool molecular gas along the line of sight. In principle, the atomic oxygen that produces a particular velocity component could exist in any, or all, of three physically distinct regions: inside a dense molecular cloud, in the UV illuminated surface layer (PDR) of a cloud, and in an atomic (H(I)) gas halo. For each of the three foreground clouds, we estimate, and subtract from the observed O(I) column density, the oxygen content of the H(I) halo gas, by scaling from a published high-resolution 21 cm spectrum. We find that the remaining O(I) column density is correlated with the observed (13)CO column density. From the slope of this correlation, an average [O(I)]/[(13)CO] ratio of 270 +/- 120 (3-sigma) is derived, which corresponds to [O(I)]/[(13)CO] = 9 for a CO to (13)CO abundance ratio of 30. Assuming a (13)CO abundance of 1x10(exp -6) with respect to H nuclei, we derive an atomic oxygen abundance of 2.7x10(exp -4) in the dense gas phase, corresponding to a 15% oxygen depletion compared to the diffuse ISM in our Galactic neighborhood. The presence of multiple, spectrally resolved velocity components in the Sgr B2 absorption spectrum allows, for the first time, a direct determination of the PDR contribution to the O(I) column density. The PDR regions should contain O(I) but not (13)CO, and would thus be expected to produce an offset in the O(I)-(13)CO correlation. Our data do not show such an offset, suggesting that within our beam O(I) is spatially coexistent with the molecular gas, as traced by (13)CO. This may be a result of the inhomogeneous nature of the clouds.

Lis, D. C.↗

Electronic structure of compressively strained thin film La$_2$PrNi$_2$O$_7$

The discovery of superconductivity in the bulk nickelates under high pressure is a major advance in physics. The recent observation of superconductivity at ambient pressure in compressively strained bilayer nickelate thin films has now enabled direct characterization of the superconducting phase through angle resolved photoemission spectroscopy (ARPES). Here we present an in-situ ARPES study of compressively strained La$_2$PrNi$_2$O$_7$ films grown by oxide molecular beam epitaxy, and the ozone treated counterparts with an onset T$_c$ of 40 K, supplemented with results from pulsed laser deposition films with similar T$_c$. We resolve a systematic strain-driven electronic band shift with respect to that of bulk crystals, in qualitative agreement with density functional theory (DFT) calculations. However, the strongly renormalized flat 3$d_{z2}$ band shifts a factor of 5-10 smaller than anticipated by DFT. Furthermore, it stays ~70 meV below the Fermi level, contradicting the expectation that superconductivity results from the high density of states of this band at the Fermi level. We also observed a non-trivial k$_z$ dispersion of the cuprate-like 3$d_{x2-y2}$ band. Combined with results from both X-ray diffraction and DFT, we suggest that the strained films are under ~5 GPa effective pressure, considerably larger than the naïve expectation from the DFT relaxed structure. Finally, the ~70 meV energy position is intriguingly close to the collective mode coupling more prominently seen in thin films, in the energy range of both oxygen related phonons and the maximum of the spin excitation spectrum.

FOS: Physical sciences↗

Origin and composition of heavy nuclei between 10 and 60 MeV per nucleon during interplanetary quiet times in 1968-1972

Results are reported for measurements of the relative abundances of nuclei from boron through iron in the energy range between 10 and 60 MeV/nucleon which were made with an instrument on board OGO 5 during the period of changing solar modulation from 1968 to 1971. The investigation was conducted to determine whether the heavy nuclei in this energy range were of solar or galactic origin. It is found that the relative abundances are in good agreement with the nuclear abundances of galactic cosmic rays, that the differential energy spectra of carbon and oxygen at these energies diverged from the characteristic modulated galactic spectrum, that changes in the C + N + O flux during this period underwent a temporal phase lag with respect to high-energy galactic cosmic rays, and that this phase lag was the same as that for helium nuclei of galactic origin with energies of 30 to 100 MeV/nucleon. It is concluded that the experimental evidence favors a galactic origin for the present nuclei. Some implications of the energy-spectrum results for cosmic-ray modulation theory are discussed.

Mogro-Campero, A.↗

Organometallic catalysts for primary phosphoric acid fuel cells

A continuing effort by the U.S. Department of Energy to improve the competitiveness of the phosphoric acid fuel cell by improving cell performance and/or reducing cell cost is discussed. Cathode improvement, both in performance and cost, available through the use of a class of organometallic cathode catalysts, the tetraazaannulenes (TAAs), was investigated. A new mixed catalyst was identified which provides improved cathode performance without the need for the use of a noble metal. This mixed catalyst was tested under load for 1000 hr. in full cell at 160 to 200 C in phosphoric acid H3PO4, and was shown to provide stable performance. The mixed catalyst contains an organometallic to catalyze electroreduction of oxygen to hydrogen peroxide and a metal to catalyze further electroreduction of the hydrogen peroxide to water. Cathodes containing an exemplar mixed catalyst (e.g., Co bisphenyl TAA/Mn) operate at approximately 650 mV vs DHE in 160 C, 85% H3PO4 with oxygen as reactant. In developing this mixed catalyst, a broad spectrum of TAAs were prepared, tested in half-cell and in a rotating ring-disk electrode system. TAAs found to facilitate the production of hydrogen peroxide in electroreduction were shown to be preferred TAAs for use in the mixed catalyst. Manganese (Mn) was identified as a preferred metal because it is capable of catalyzing hydrogen peroxide electroreduction, is lower in cost and is of less strategic importance than platinum, the cathode catalyst normally used in the fuel cell.

Walsh, Fraser↗