We investigate the oxidation of uranium (U) species, the physical conditions leading to uranium monoxide (UO) formation and the interplay between plume hydrodynamics and plasma chemistry in a ...laser-produced U plasma. Plasmas are produced by ablation of metallic U using nanosecond laser pulses. An ambient gas environment with varying oxygen partial pressures in 100 Torr inert Ar gas is used for controlling the plasma oxidation chemistry. Optical emission spectroscopic analysis of U atomic and monoxide species shows a reduction in the emission intensity and persistence with increasing oxygen partial pressure. Spectral modelling is used for identifying the physical conditions in the plasma that favor UO formation. The optimal temperature for UO formation is found to be in the temperature range of ∼1500-5000 K. The spectrally integrated and spectrally filtered (monochromatic) imaging of U atomic and molecular species reveals the evolutionary paths of various species in the plasma. Our results also highlight that oxidation in U plasmas predominantly occurs at the cooler periphery and is delayed with respect to plasma formation, and the dissipation of molecular species strongly depends on oxygen partial pressure.
The complex interplay between plume hydrodynamics and chemistry impacts physical conditions leading to UO molecular formation in laser-plasmas.
Gas-phase oxidation of uranium (U), plume chemistry, and the corresponding impact on optical emission features of the U plasma are investigated. Plasmas were produced
via
nanosecond laser ablation of ...a natural U target in a chamber where U oxidation was controlled by varying the oxygen partial pressure in an argon cover gas. Monochromatic imaging of U atoms and monoxide (UO) molecules was performed using narrow bandpass optical filters. Results reveal the spatio-temporal evolution of atomic and molecular species in the plasma. U oxides are found to be formed further from the target (in comparison to U atoms), where lower temperatures favor molecular recombination. Segregation between the distribution of U atoms and UO species is observed at later times of plasma evolution, and is more apparent at lower oxygen partial pressures. At higher oxygen partial pressures, significant variation in plume morphology is noticed for UO species, which can be attributed to the higher oxide (U
x
O
y
) formation further from the target. The monochromatic images of U atoms and UO molecules and corresponding spectral features at various oxygen partial pressures presented here provide unique insight into gas-phase, high-temperature U oxidation and chemistry, with implications for a wide range of nuclear applications, from stand-off detection of radioisotopes to forensics and safeguards.
Spatial temporal contours of atoms and molecules in uranium plasmas reveal complex plasma-chemical interaction between plume and oxygen-containing ambient gas.
Pacific Northwest National Laboratory has recently opened a shallow underground laboratory intended for measurement of low-concentration levels of radioactive isotopes in samples collected from the ...environment. The development of a low-background liquid scintillation counter is currently underway to further augment the measurement capabilities within this underground laboratory. Liquid scintillation counting is especially useful for measuring charged particle (e.g., β and α) emitting isotopes with no (or very weak) gamma-ray yields. The combination of high-efficiency detection of charged particle emission in a liquid scintillation cocktail coupled with the low-background environment of an appropriately designed shield located in a clean underground laboratory provides the opportunity for increased-sensitivity measurements of a range of isotopes. To take advantage of the 35m-water-equivalent overburden of the underground laboratory, a series of simulations have evaluated the scintillation counter's shield design requirements to assess the possible background rate achievable. This report presents the design and background evaluation for a shallow underground, low background liquid scintillation counter design for sample measurements.
•Graded-shielding can produce an ultra-low-background liquid scintillation counter.•Location in a shallow underground cleanroom further enhances background reduction.•A novel light collection design and selected low background materials are utilized.•The background is predicted to be 10–100 times below typical commercial systems.•Simulations tentatively predict a background rate of order 10 counts per day.
The Ultra-Low Background Liquid Scintillation Counter developed by Pacific Northwest National Laboratory will expand the application of liquid scintillation counting by enabling lower detection ...limits and smaller sample volumes. By reducing the overall count rate of the background environment approximately 2 orders of magnitude below that of commercially available systems, backgrounds on the order of tens of counts per day over an energy range of ~3–3600keV can be realized. Initial test results of the ULB LSC show promising results for ultra-low background detection with liquid scintillation counting.
•Observed background is within a factor of 2 of the predictions from simulation.•Background achieved is 2 orders of magnitude below commercially available systems.•Backgrounds are in tens of counts per day over an energy range of ~3– 3600keV.•Initial results show promise for ultra-low background detection with the ULB LSC.
During its approach to asteroid (101955) Bennu, NASA’s Origins, Spectral Interpretation, Resource Identification, and Security-Regolith Explorer (OSIRIS-REx) spacecraft surveyed Bennu’s immediate ...environment, photometric properties, and rotation state. Discovery of a dusty environment, a natural satellite, or unexpected asteroid characteristics would have had consequences for the mission’s safety and observation strategy. Here we show that spacecraft observations during this period were highly sensitive to satellites (sub-meter scale) but reveal none, although later navigational images indicate that further investigation is needed. We constrain average dust production in September 2018 from Bennu’s surface to an upper limit of 150 g/s averaged over 34 min. Bennu’s disk-integrated photometric phase function validates measurements from the pre-encounter astronomical campaign. We demonstrate that Bennu’s rotation rate is accelerating continuously at 3.63 ± 0.52 × 10^(–6) degrees/sq. day, likely due to the Yarkovsky–O’Keefe–Radzievskii–Paddack (YORP) effect, with evolutionary implications.
Helicopter-mounted gamma-ray detectors can provide law enforcement officials the means to quickly and accurately detect, identify, and locate radiological threats over a wide geographical area. The ...ability to accurately distinguish radiological threat-generated gamma-ray signatures from background gamma radiation in real time is essential in order to realize this potential. This problem is non-trivial, especially in urban environments for which the background may change very rapidly during flight. This exacerbates the challenge of estimating background due to the poor counting statistics inherent in real-time airborne gamma-ray spectroscopy measurements. To address this challenge, we have developed a new technique for real-time estimation of background gamma radiation from aerial measurements without the need for human analyst intervention. The method can be calibrated using radiation transport simulations along with data from previous flights over areas for which the isotopic composition need not be known. Over the examined measured and simulated data sets, the method generated accurate background estimates even in the presence of a strong, 60Co source. The potential to track large and abrupt changes in background spectral shape and magnitude was demonstrated. The method can be implemented fairly easily in most modern computing languages and environments.
Uranium Oxide Emission from Laser-Produced Plasma Harilal, S. S.; Brumfield, B. E.; Bernacki, B. E. ...
2018 IEEE International Conference on Plasma Science (ICOPS),
2018-June-24
Conference Proceeding
The formation and emission of molecular species in a laser-produced plasma have been the subject of a number of recent studies. In laser-induced plasmas molecules are formed through a number of ...reaction pathways: combustion (oxidation) by direct interaction with the ambient atmosphere, recombination between species present within the plasma, and fragmentation of larger molecular clusters. However, even though extensive studies are available in the literature, still there exists a lack of knowledge about when and where the molecules are formed in a transient plasma system like a LPP. Typically, the molecular emissions are observed when the plasma has cooled and undergone significant expansion into the ambient atmosphere, and molecular emission persist for longer periods compared to the excited atomic and ionic emissions. Recent studies have shown that shock waves formed during LPP expansion hinder molecular formation through combustion at early times of its evolution. 1 The emission intensity, delay, and persistence of the atomic, ionic, and molecular emissions are influenced by the plasma chemistry.
Uranium and plutonium oxidize very rapidly in an oxygen-rich environment like air. Understanding the gas-phase actinide oxide molecular formation through plasma- and thermochemistry is very important ...for numerous fields including forensic analysis, environmental monitoring, debris analysis in a weapons detonation event, or reactor accident scenario, and actinide nucleation physics. There have been significant recent efforts to understand the chemical progression from U atoms to diatoms (UO) and polyatomic molecules (U x O y ). 1-3 However, emission analysis of high-temperature gas-phase oxidation of U and Pu and the corresponding plasma chemistry are very complex considering their very congested spectral features. In addition to these, the spectra may contain isotopic shifts and hyperfine structures if the sample is enriched.
Thermal inertia and surface roughness are proxies for the physical characteristics of planetary surfaces. Global maps of these two propertiesdistinguish the boulder population on near-Earth asteroid ...(NEA) (101955)Bennuinto two typesthat differ in strength,andboth havelower thermal inertiathan expectedfor boulders and meteorites. Neither has strongly temperature-dependent thermal properties. The weakerbouldertypeprobably would not survive atmospheric entry and thus may not berepresented in the meteorite collection. The maps also show ahigh-thermal-inertia band at Bennu’s equator, which might be explained by processes such as compaction or strength sorting during mass movement, but these explanations are not wholly consistent with other data. Our findings imply that other C-complex NEAs likely have boulderssimilar to those on Bennu,rather than finer-particulate regoliths.A tentative correlation between albedo and thermal inertia of C-complex NEAs may be due to relative abundances of boulder types.
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