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At least 217 records · Page 12

Hot Spot Evolution Measured by High-Resolution X-Ray Spectroscopy at the National Ignition Facility

Evolution of the hot spot plasma conditions was measured using high-resolution x-ray spectroscopy at the National Ignition Facility. The capsules were filled with DD gas with trace levels of Kr and had either a high-density-carbon (HDC) ablator or a tungsten (W)-doped HDC ablator. Time-resolved measurement of the Kr He β spectra, absolutely calibrated by a simultaneous time-integrated measurement, allows inference of the electron density and temperature through observing Stark broadening and the relative intensities of dielectronic satellites. By matching the calculated hot spot emission using a collisional-radiative code to experimental observations, the hot spot size and areal density are determined. Here these advanced spectroscopy techniques further reveal the effect of W dopant in the ablator on the hot spot parameters for their improved implosion performance.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

First-principles determination of the phonon-point defect scattering and thermal transport due to fission products in ThO 2

This work presents the first-principles calculations of the lattice thermal conductivity degradation due to point defects in thorium dioxide using an iterative solution of the Pierels-Boltzmann transport equation. We have used the non perturbative Green’s function methodology to compute the phonon- point defect scattering rates that consider the local distortion around the point defect, including the mass difference changes, interatomic force constants, and structural relaxation near the point defects. The point defects considered in this work include the vacancy of thorium ($V$ $TH$ ) and oxygen ($V$ $O$ ), substitutions of helium ($He$ $Th$ ), krypton ($Kr$ $Th$ ), zirconium ($Zr$ $Th$ ), iodine ($I$ $Th$ ) and xenon ($Xe$ $Th$ ) in the thorium site, and the three different configurations of the Schottky defects. The results of the phonon-defect scattering rate reveal that, among all the considered intrinsic defects, the thorium vacancy and helium substitution in the thorium site scatter the phonon most due to the substantial changes in the force constant and structural distortions. The scattering of phonons due to the substitutional defects unveils that the zirconium atom scatters phonons the least, followed by xenon, iodine, krypton, and helium. This is contrary to the intuition that the scattering strength follows $He$ $Th$ > $Kr$ $Th$ > $Zr$ $Th$ > $I$ $Th$ > $Xe$ $Th$ based on the mass difference. This striking difference in the zirconium phonon scattering is due to the local chemical environment changes. Zirconium is an electropositive element with valency similar to thorium and, therefore, can bond with the oxygen atoms, thus creating less force constant variance compared to iodine, an electronegative element noble gas helium, xenon, and krypton. In conclusion, these results can serve as the benchmark for the analytical models and help the engineering-scale modeling effort for nuclear design.

36 MATERIALS SCIENCE↗

Ion beam irradiation of ABO4 compounds with the fergusonite, monazite, scheelite, and zircon structures

The effects of irradiation on CaWO4, SrWO4, BaWO4, YVO4, LaVO4, YNbO4, and LaNbO4 were investigated on thin crystals using 1.0 MeV Kr ions at 50-1000 K. All of the ABO4 compounds can be amorphized with calculated damage cross sections (σa = 1/Fc0) in the range of ~0.30-1.09 × 10-14 cm2 ion-1 at zero Kelvin. The analysis of fluence-temperature data returned critical temperatures for amorphization (Tc) of 311 ± 1, 358 ± 90, 325 ± 19, 415 ± 17, 541 ± 6, 636 ± 26, and 1012 ± 1 K, respectively, for the compounds listed above. Compared with previous in situ irradiation of ABO4 orthophosphate samples using 0.8 MeV Kr ions, the Tc values of LaVO4 and YVO4 are higher than those of LaPO4 and YPO4 by 82 K and 124 K, respectively. The Tc values of the three scheelite structures, CaWO4, SrWO4, and BaWO4, indicate that they are the most radiation tolerant compounds under these conditions. The A-B cation anti-site energies, EfAB, determined by DFT range from 2.48 to 10.58 eV and are highly correlated with the A-B cation ionic radius ratio, rA/rB, but are not correlated with Tc across the different structure types, suggesting that the formation and migration energies of Frenkel defects play a more important role in damage recovery in these compounds. We also discuss the role of cation and anion charge/iconicity as determined by DFT. ABO4 compounds with the zircon structure and B = P or V have a distinct advantage over those with B = Si as the damaged regions do not appear to be significantly affected by polymerization of (PO4) 3- or (VO4) 3- groups which might stabilize the amorphous fraction and ultimately lead to phase separation as observed in zircon (ZrSiO4).

amorphization↗

Fine structure in the α decay of $^{179}$Hg and $^{177}$Au

Abstract The$$\upalpha $$ α -decay fine structure of$$^{179}$$ 179 Hg and$$^{177}$$ 177 Au was studied by means of decay spectroscopy. Two experiments were performed at the Accelerator Laboratory of the University of Jyväskylä (JYFL), Finland, utilizing the recoil separator RITU and a digital data acquisition system. The heavy-ion induced fusion-evaporation reactions$$^{82}_{36}$$ 36 82 Kr + $$^{100}_{44}$$ 44 100 Ru and$$^{88}_{38}$$ 38 88 Kr + $$^{92}_{42}$$ 42 92 Mo were used to produce the$$^{179}$$ 179 Hg and$$^{177}$$ 177 Au nuclei, respectively. Studying the evaporation residues (ER, recoils)-$$\alpha _1$$ α 1 -$$\alpha _2$$ α 2 correlations and$$\upalpha $$ α -$$\gamma $$ γ coincidences, a new$$\upalpha $$ α decay with E$$_\alpha $$ α = 6156(10) keV was observed from$$^{179}$$ 179 Hg. This decay populates the (9/2$$^-$$ - ) excited state at an excitation energy of 131.3(5) keV in$$^{175}$$ 175 Pt. The internal conversion coefficient for the 131.3(5) keV transition de-exciting this state was measured for the first time. Regarding the$$^{177}$$ 177 Au nucleus, a new$$\upalpha $$ α decay with E$$_\alpha $$ α = 5998(9) keV was observed to populate the 156.1(6) keV excited state in$$^{173}$$ 173 Ir. Two de-excitation paths were observed from this excited state. Moreover, a new 215.7(13) keV transition was observed to depopulate the 424.4(13) keV excited state in$$^{173}$$ 173 Ir. Properties of the$$^{179}$$ 179 Hg and$$^{177}$$ 177 Au$$\upalpha $$ α decays were examined in a framework of reduced widths and hindrance factors. For clarity and simplicity, the spin and parity assignments (e.g.$$J^{\pi }$$ J π ) are presented without brackets throughout the text.

Physics↗

Safety Testing of AGR-5/6/7 Compacts 2-2-2 and 2-2-4

Compacts 2-2-2 and 2-2-4 from the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program’s final irradiation campaign (AGR-5/6/7) were each separately subjected to a thermal soak at 1600°C for 300 h under flowing helium to simulated conditions experienced during a postulated high-temperature gas-cooled reactor (HTGR) depressurization conduction cooldown event. The safety testing of the fuel compacts’ performance under accident conditions was conducted in the Oak Ridge National Laboratory (ORNL) Core Conduction Cooldown Test Facility (CCCTF), which utilizes a stand-alone hot cell at the Irradiated Fuels Examination Laboratory (IFEL). The CCCTF heats fuel to temperatures up to 1900°C in a non-oxidizing environment while continuously monitoring the sweep gas for radioactive 85 Kr to detect release levels associated with hermetic failure of the tristructural-isotropic (TRISO) coating surrounding each fuel kernel. In addition, certain metallic radionuclides that escape the fuel compact are collected on deposition cups that are periodically exchanged with a new cup to obtain information on the overall retention behavior of the TRISO coating layers. Because cesium can diffuse through intact pyrocarbon layers, abnormal degradation of the silicon carbide (SiC) layer in the absence of holistic TRISO coating failure is indicated by release of 134 Cs at levels equivalent to an individual particle inventory in the absence of significant 85 Kr release (Hunn et al. 2014). Additional description of the CCCTF system is provided in Appendix A.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

SATS Transient Fission Gas Release Test with Irradiated Fuel under Loss of Coolant Accident Conditions

The transient fission gas release (tFGR) during the temperature ramp associated with a loss-of-coolant accident (LOCA) in light-water reactors (LWRs) is likely a significant contribution to the total pressure in a fuel rod and may cause an unexpected rod burst. The lack of data related to tFGR continues to be a key gap in understanding LWR cladding burst behavior under LOCA conditions. To fully characterize this behavior, tFGR data must be collected from several different systems that can capture all relevant testing conditions. Oak Ridge National Laboratory (ORNL) has developed a system to measure the integral tFGR from irradiated fuel segments. This system was designed to integrate with the existing Severe Accident Test Station (SATS) and to build upon decades of experience capturing fission gas to characterize fuel behavior. The tFGR system consists of a sweep gas system to transport gases from the in-cell SATS apparatus to an out-of-cell fission gas detection system composed of a series of cold traps to capture the off-gas from the heating tests and a gamma spectrometry system to detect and measure 85 Kr. Initial system testing operations were completed during which 85 Kr collection and measurement were verified along with the ability to detect stable inert gases. A tFGR test with a high-burnup fuel specimen was successfully conducted by the in-cell SATS-tFGR system at ORNL. The posttest examination is under way, the result of which will be reported in FY24.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Metal Organic Frameworks for Noble Gas Isotope Harvesting at FRIB (Final Technical Report)

This project was a collaborative effort between Lawrence Livermore National Laboratory (LLNL) and Michigan State University (MSU) to investigate the use of promising metal organic frameworks (MOFs) for radioactive noble gas capture, with a focus on harvesting exotic radiokryptons from FRIB. After screening several candidate materials, two MOFs were selected for testing: SIFSIX-3Cu and SBMOF-1. Further evaluation showed that although SIFSIX-3Cu has a high selectivity for Kr, SBMOF-1 is less sensitive to the humidity that is present in the FRIB harvesting system and is more readily integrated into the harvesting infrastructure. SBMOF-1 was then evaluated for temperature-dependent Kr and Xe uptake in order to determine the sorption enthalpy. The SBMOF-1 data led to the design of a noble gas capture system that will be fabricated and put into service for isotope harvesting at FRIB as part of a separate project.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Xe Recovery from Nuclear Power Plants Off-Gas Streams: Molecular Simulations of Gas Permeation through DD3R Zeolite Membrane

Recent experimental work has shown zeolite membrane-based separation as a promising potential technology for Kr/Xe gas mixtures due to its much lower energy requirements in comparison to cryogenic distillation, the conventional separation method for such mixtures. Such a separation is also economically rewarding because Xe is in high demand, as a valuable product for many applications/processes. In this work, we have used Molecular Dynamics (MD) simulations to study the effects of different conditions, i.e., temperature, pressure, and gas feed composition, on Kr/Xe separation performance via DD3R zeolite membranes. We provide a comprehensive study of the permeation of the different gas species, density profiles, and diffusion coefficients. Molecular simulations show that if the feed is changed from pure Kr/Xe to an equimolar mixture, the Kr/Xe separation factor increases, which agrees with experiments. In addition, when Ar is introduced as a sweep gas, the adsorption of both Kr and Xe increases, while the permeation of pure Kr increases. A similar behavior is observed with equimolar mixtures of Kr/Xe with Ar as the sweep gas. High-separation Kr/Xe selectivity is observed at 50 atm and 425 K but with low total permeation rates. Changing pressure and temperature are found to have profound effects on optimizing the separation selectivity and the permeation throughput.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Turbulent Acceleration of Interstellar Pickup Ions at the Heliospheric Termination Shock Forms the Global ENA Spectrum

The heliospheric energetic neutral atom spectrum observed by the Interstellar Boundary Explorer (IBEX) reveals that the heliosheath proton distribution is consistent with a power law. The origin of the spectrum is likely from interstellar pickup ions (PUIs) accelerated at the heliospheric termination shock (HTS). We present an explanation of the proton spectrum origin using a test particle simulation of PUIs accelerated at the HTS. PUIs experience preferential heating by the motional electric field in the shock foot, but do not develop a power-law tail without the presence of turbulence at wavenumbers (k) close to the PUI gyroradius scale (R g ). Voyager 2 observations of the magnetic field downstream of the HTS indicate a moderate amount of turbulence at kR g ≅ 1, (δB /B 0 ) 2 @ 0.01, which we find to be sufficient for producing a downstream suprathermal PUI tail but not at intensities observed by IBEX. Within the shock ramp, however, Voyager observed the turbulence power at much smaller scales to be nearly 100 times stronger, suggesting the possibility of strong turbulence at the PUI gyroradius scale. We show that a proton distribution can develop a power law downstream of the HTS consistent with IBEX observations if (δB /B 0 ) 2 ≳ 0.1 at kR g ≅ 1 in the shock foot. Shock drift acceleration of PUIs by the motional electric field is aided by interactions with turbulence upstream of the shock overshoot. Steepening of the IBEX proton spectrum in directions farther from the heliospheric nose suggests the HTS compression ratio and/or turbulence power weakens near the heliotail.

79 ASTRONOMY AND ASTROPHYSICS↗

The interaction of O(plus) ions with the interior surface of a copper chamber

Modulated beams of 0(+), Ar(+), and Kr(+) in the 100-300 eV range are directed into a copper box simulating the ante-chamber of an orbiting mass spectrometer. An RF quadrupole mass spectrometer and phase sensitive detection extract the component of the internal mass spectrum correlated with the beam. Intense Ar and Kr signals are observed; however, no O or O2 is detectable, indicating loss of the primary O(+) beam to surface interactions. All four primary ions stimulate sizeable signals at masses 26 and 28. The relevance of these experiments to the interpretation of mass spectra obtained by orbiting satellites is discussed.

Siegel, M. W.↗

Origin of planetary primordial rare gas - The possible role of adsorption.

The degree of physical adsorption of Ne, Ar, Kr, and Xe on pulverized samples of the Allende meteorite at 113 K has been measured. The observed pattern of equilibrium enrichment of heavy rare gases over light on the pulverized meteorite surfaces relative to the gas phase is similar to the enrichment pattern exhibited by planetary primordial rare gas when compared with the composition of solar rare gas. Results indicate that, at 113 K, a total nebular pressure of from .01 to .001 atm would be required to explain the Ar, Kr, and Xe abundances in carbonaceous chondrites with an adsorption mechanism. This pressure estimate is compatible with the range of possible nebular pressures suggested by astrophysical arguments. However, the subsequent mechanism by which initially adsorbed gas might have been transferred into the interiors of grains cannot be identified at present.

Fanale, F. P.↗

Relative transition probabilities for krypton.

First experimental line strength data for the visible Kr II lines and for several of the more prominent Kr I lines are given. The spectroscopic light source used is the thermal plasma behind the reflected shock wave in a gas-driven shock tube. A 3/4-m spectrograph and a 1-m spectrograph were employed simultaneously to provide redundant photometry. The data are compared with other measurements and with theoretical calculations.

Miller, M. H.↗

Mariner 9 ultraviolet spectrometer experiment: Mars atomic oxygen 1304-Angstrom emission

Selected results are presented for a considerable quantity of Mariner 9 1304-A data for the first 100 revolutions from both the bright limb and disk of Mars. The limb data suggest that the exospheric temperature is less than it was in 1969 when Mariners 6 and 7 encountered the planet. Similar (O) concentrations (0.5 to 1%) are derived for a temperature of about 300 K. Structure in the limb profiles below 200 km suggests the possibility that about 0.2 kR of the observed approximately 0.8 kR near 150 km is due to dissociative excitation of CO2. Significant differences in selected limb profiles suggest that local as well as random variations in (O) occur.

Strickland, D. J.↗

Solubilities of noble gases in magnetite - Implications for planetary gases in meteorites.

Solubilities of noble gases in magnetite were determined by growing magnetite in a noble-gas atmosphere between 450 and 700 K. Henry's law is obeyed at pressures up to .01 atm for He, Ne, Ar and up to .00001 atm for Kr, Xe, with the following distribution coefficients at 500 K: He 0.042, Ne 0.016, Ar 3.6, Kr 1.3, Xe 0.88, some 100 to 100,000 times higher than previous determinations on silicate and fluoride melts. Apparent heats of solution are in sharp contrast with earlier determinations on melts which were small and positive, but are comparable to the values for clathrates. Presumably the gases are held in anion vacancies.

Lancet, M. S.↗

Mariner 9 ultraviolet spectrometer experiment - Mars atomic oxygen 1304-A emission.

Selected results are presented for an analysis of Mariner 9 1304-A data from the first 100 passes. Based on a comparison of limb data, the exospheric temperature appears lower on several Mariner 9 passes than when Mariner 6 and 7 encountered the planet in 1969. Temperatures of 300 and 350 K are considered in the atmospheric modeling. At 300 K, derived values of the atomic oxygen concentration are typically between 0.5 and 1% of the total density at 135 km, based on fitting theoretical intensities to limb data from several passes. Structure in the limb data below 200 km suggests the possibility that approximately 0.2 kR of the observed approximately 0.8 kR near 150 km is due to dissociative excitation of CO2. There is variability in limb profiles, thus indicating changes in the O distribution with time. The variability does not appear to follow a recognizable pattern. Interpretation of the 1304-A disk data shows a correlation in intensity with the 10.7-cm solar flux and larger O concentrations in the afternoon than in the morning. The correlation in intensity with the 10.7-cm flux is probably due largely to variation in the solar 1304-A fluxes.

Strickland, D. J.↗

Lunar surface dynamics: Some general conclusions and new results from Apollo 16 and 17

Exposure ages of Apollo 17 rocks as measured by tracks and the Kr-Kr rare gas method are reported. Concordant ages of 22 - or + 1 million year (my) are obtained for the station 6 boulder sample 76315. This value is interpreted as the time when the station 6 boulder was emplaced in its present position. Reasonable agreement is also obtained by the two methods for another station 6 boulder, sample 76015. Discordant ages (respectively 5 and 28 my by the track and rare gas methods) are obtained for the station 7 boulder sample, 77135, indicating that the boulder was emplaced at least 5 my ago. The 72 my exposure age of 75035, in general agreement with previous measurements of approximately 85 my for another Camelot boulder, may well date the formation of Camelot. Rock 76015 was split and one surface exposed to the sky through a very small solid angle.

Crozaz, G.↗

Cosmic-ray exposure history at the Apollo 16 and other lunar sites - Lunar surface dynamics

Concordant Kr-81/Kr exposure ages for four station 11 breccias indicate an age of 50.3 plus or minus 0.8 m.y. for North Ray Crater. Ray structures visible from orbital photography suggest that stations 8 and 9 should contain a substantial amount of South Ray ejecta. Concordant Kr-81/Kr exposure ages at these sites indicate an age for South Ray Crater of 2.04 plus or minus 0.08 m.y. Surface effects show good general agreement with this young age, but discrepancies on a sample-by-sample basis seem to indicate that extensive presurface irradiations must have occurred.

Drozd, R. J.↗

The San Juan Capistrano meteorite

The San Juan Capistrano chondrite fell on 15 March 1973; the total recovered mass was 56 g. Electron microprobe, chemical and petrographic studies show it to be a member of the H group and of petrologic type 6. Rare gas studies show that only minor radiogenic gas loss has occurred and yield a K-Ar age of 4.6 billion years and a Kr-Kr exposure age of 29 million years.

Finkel, R. C.↗