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At least 379 records · Page 21

Expanded method for the determination of burnup in nuclear fuels using multiple neodymium isotopes

Established methods for the determination of burnup in nuclear fuels commonly rely on the measurement of 148Nd in the spent fuel in concert with known fission product yields to determine the atom percent of fissions in the fuel. This isotope of neodymium is used for various reasons, including chemical and radioactive stability, ease of measurement, and low rates of formation and destruction due to neutron flux apart from fission. However, careful calculation of effective cumulative fission yields and correction factors for (n,γ) capture reactions allows for additional stable and long-lived isotopes of neodymium to be used to provide additional independent measurements of burnup, reducing statistical uncertainty. This method was developed and successfully applied to measure the burnup of compacts from the Advanced Gas Reactor (AGR) Fuel Development and Qualification Program. The mean burnup measured using 143Nd, 145Nd, 146Nd, 148Nd, and 150Nd was statistically observed to be the same as that measured using 148Nd alone, but the statistical uncertainty in the measurement was reduced by a factor of 2, providing a tighter confidence interval in the final results.

Helmreich, Grant [ORNL] (ORCID:0000000330464394)↗

Los Alamos National Laboratory Release of Cesium-137 Corrective Action Plan

This Corrective Action Plan (CAP) was developed by a team chartered by John Sarrao, Deputy Director for Science, Technology, and Engineering (DDSTE), to review and respond to the findings of the Joint National Nuclear Security Administration/Triad National Security (NNSA/Triad) Investigation Team (JIT) Joint Investigation Report for the “Sealed Source Recovery at the University of Washington Harborview Training and Research Facility Results in Release of Cesium-137 on May 2, 2019,” dated March 30, 2020. On May 2, 2019, International Isotopes, Inc. (INIS), a subcontractor to Triad National Security, LLC, inadvertently breached a sealed cesium-137 source at the University of Washington (UW), Harborview Medical Center Research and Training (HRT) building in downtown Seattle while attempting to recover the source for the National Nuclear Security Administration (NNSA) Off-Site Source Recovery Program (OSRP). The source breach resulted in contamination of personnel and the HRT building, as well as a release of radioactive material to the environment

07 ISOTOPE AND RADIATION SOURCES↗

Low Count and Background Radionuclides Analysis - 20488

The US Department of Energy (DOE) is often faced with the need to evaluate radionuclides at low concentrations. When site sample data are likely to be close to threshold activity concentrations of interest, then the means by which the radiochemical analysis is performed and reported is critical. This situation can occur when differentiating from zero (presence/absence) for radionuclides that do not occur naturally, close comparison with environmental background for naturally occurring radionuclides, close comparison with a risk- or dose-based threshold concentrations of interest, or even comparisons across studies. There are several analytical issues that are of concern, but the two that appear to cause incorrect decisions to be made most often involve establishing detection limits and subtracting ambient background conditions in the laboratory. These issues are not critical when radionuclide activity concentrations are large relative to thresholds of concern, but they seem to be poorly understood when it matters. When the comparisons are important and are likely to be close to a threshold of interest, then the general contract with the analytical laboratories needs to be changed so that the right or appropriate data are obtained. The concern is that important decisions are made incorrectly more often as greater scrutiny is placed on DoE's radionuclide cleanup or monitoring decisions by the public and other stakeholders. Examples are presented of problems that have been observed for different projects, both within and outside the realm of DOE and NRC remediation and radioactive waste disposal problems, and solutions are offered that should lead to better data from which important decisions need to be made. The first example is from Los Alamos National Laboratory (LANL) and involves radionuclide concentrations in soil and rock beneath LANL's Material Disposal Area (MDA) G. An initial review of the data led to a conclusion that americium and plutonium are a long way present beneath MDA G. A more thorough review of the data that accounted properly for ambient background and the detection limits that had been established led to the opposite conclusion. Another example is from the Nevada National Security Site where tritium results from one of the wells were unexpectedly high. Proper understanding and analysis of ambient background led to the conclusion that the increased concentrations were not so obvious, and that a different contract with the analytical laboratory was needed to provide more appropriate data to support a better determination. Other examples are used from regulatory review of projects in Nevada, where background levels and secular equilibrium for naturally occurring radionuclides are not established correctly because of analytical issues. The same basic issues have also been found to create difficulties analyzing historical data from the West Valley Demonstration Project. There is evidence in the data that the apparent lack of secular equilibrium where it is expected to exist is related to ambient background subtraction or other analytical issues. A final example is presented for analysis of Tc-99 in samples of depleted uranium. In this case, two different studies that were performed only three months apart provide quite different results. The US Environmental Protection Agency (EPA) established the data quality objectives (DQO) process in the mid-1980's to establish decision performance criteria for data collection. EPA guidance (EPA G-4, for example) clearly distinguishes between DQOs and measurement performance objectives (MQOs) that should be addressed for laboratory analysis of samples. The language of DQOs and MQOs has become confused over time it seems, and the subsequent effects seem to include a lack of attention to decision performance and a routine approach to measurement quality. In order to better address radionuclide sample analysis when the concentrations are close to thresholds of concern, which might be zero for some radionuclides, background for others, and risk-based thresholds for yet others, it is important that routine laboratory analysis methods are adjusted, and that the project team and the laboratory work closely together to ensure that the data meets the MQO requirements of laboratory analysis and reporting of results, and that the MQOs effectively support project-specific DQOs. This basic approach will be applied in Los Alamos in the coming year to the collection of moisture data from underneath MDA T that will be analyzed for americium and neptunium isotopes. Proper understanding of the radiochemistry methods and reporting, and of appropriate statistical methods is critical to the success of such projects, ensuring that the right decisions are made. (authors)

07 ISOTOPE AND RADIATION SOURCES↗

Measurement of the Mo 100 ( α , x n ) cross section at weak r -process energies

Here, the weak r process in neutrino-driven winds following a core-collapse supernova is thought to contribute to the cosmic abundances of the first r-process peak elements between Se and Ag. Sensitivity studies have found that the early nucleosynthesis in the weak r process is primarily driven by (α, xn) reactions due to the high temperatures, and that current nuclear physics uncertainties in the (α, xn) rates result in significant uncertainties of the calculated abundances. The weak r-process path proceeds several nuclei away from stability where (α, xn) reaction cross sections have not yet been measured. In this paper we report the 100 Mo (α, xn) cross section (between 8.9 and 13.2 MeV in the center of mass, corresponding to 3.5–6.8 GK) in inverse kinematics using the Multi-Sampling Ionization Chamber (MUSIC) detector at the Argonne Tandem Linac Accelerator System (ATLAS) facility. With this first measurement of the 100 Mo (α, xn) cross section, we have demonstrated the ability of MUSIC to measure (α, xn) cross sections for A up to 100, therefore paving the way for further measurements with radioactive beams at ATLAS or the Facility for Rare Isotope Beams.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Energy requirements for HE-3 mining operations on the Moon

At the present rate of world energy consumption (10 TW-y/y) and allowing for an equilibrium consumption of 20 to 30 TW-y/y in mid 21st century, we will exhaust economically recoverable fossil fuels in the next 50 to 60 years. We will then have to rely on nuclear (fission and fusion) and renewable energy to feed, warm, and protect the world's population. Fusion energy is expected to play an important role in the 21st century and there a 2 billion dollar per year research program to commercialize that energy resource. A serious problem with this is its reliance on the D-T fuel cycle which releases 80 percent of its energy in the form of neutrons. These neutrons cause significant radiation damage and induce large amounts of radioactivity. There is another fusion fuel cycle involving the isotopes of Deuterium and Helium-3 which, if configured properly, releases 1 percent or less of its energy in neutrons. Obviously, such a fuel would be preferred, but there is no large source of He-3 known to satisfy world energy needs. Fortunately, a very large source of He-3 was found on the Moon, implanted over the past 4 billion years by the solar wind. Recent analysis of Apollo and Luna data reveals that over a million tons of He-3 sit on the Moon's surface. The potential energy in this He-3 fuel is 10 times that contained in all the coal, oil, and natural gas on the Earth. The purpose of this paper is to examine the energy required to extract the He-3 from the lunar regolith.

Kulcinski, Gerald L.↗

Lunar and Planetary Science XXXV: From Ancient Mists: Presolar and Nebular Processes

The session "From Ancient Mists: Presolar and Nebular Processes" included the following reports: Interpretation of the Meteoritic Extinct Radioactivity - Mean Life Relation; On the Issue of Molybdenum Isotopic Anomalies in Meteorites: Is It Still "FUN"?; (26Al/27Al)o of the Solar Nebula Inferred from Al-Mg Systematic in Bulk CAIs from CV3 Chondrites; Magnesium Isotopic Compositions of Igneous CAIs in the CR Carbonaceous Chondrites: Evidence for an Early and Late-stage Melting of CAIs; The 26Al-26Mg Chronology of a Type C CAI and POIs in Ningqiang Carbonaceous Chondrite; Bulk Compositions of CAIs and Al-rich Chondrules: Implications of the Reversal of the Anorthite / Forsterite Condensation Sequence at Low Nebular Pressures; Synthesis of Refractory Minerals by High-Temperature Condensation of a Gas of Solar Composition; Elemental and Isotopic Fractionation by Diffusion-limited Evaporation; "Nonideal" Isotopic Fractionation Behavior of Magnesium in Evaporation Residues; Determination of Primordial Refractory Inclusion Compositions; Zoning Patterns in Spinel from Type B Ca-Al-rich Inclusions: Constraints on Sub-Solidus Thermal History; Radial Migration of Materials from Inner to Outer Solar Nebula: Evidence from Meteorite Matrix; and Refractory Forsterites in Chondritic Meteorites, a Link Between CAIs and Chondrules.

Source record↗

Helium-Shell Nucleosynthesis and Extinct Radioactivities

Although the exact site for the origin of the r-process isotopes remains mysterious, most thinking has centered on matter ejected from the cores of massive stars in core-collapse supernovae [13]. In the 1970's and 1980's, however, difficulties in understanding the yields from such models led workers to consider the possibility of r-process nucleosynthesis farther out in the exploding star, in particular, in the helium burning shell [4,5]. The essential idea was that shock passage through this shell would heat and compress this material to the point that the reactions 13C(alpha; n)16O and, especially, 22Ne(alpha; n)25Mg would generate enough neutrons to capture on preexisting seed nuclei and drive an "n process" [6], which could reproduce the r-process abundances. Subsequent work showed that the required 13C and 22Ne abundances were too large compared to the amounts available in realistic models [7] and recent thinking has returned to supernova core material or matter ejected from neutron star-neutron star collisions as the more likely r-process sites.

Meyer, B. S.↗

Anode sensitivity calibration of photomultiplier tubes used as a readout of the ELOSS detector

We present and discuss the methodology and results for an anode sensitivity calibration of Photomultiplier Tubes (PMTs) that serve as the optical readout of the Energy Loss Optical Scintillation System (ELOSS). The ELOSS detector, under development at the Facility for Rare Isotope Beams (FRIB), is a gaseous Xe scintillation-based detector designed to identify the atomic number (Z) of nuclear reaction fragments by energy-loss measurement. Variation in the anode sensitivity from tube to tube of commercially available PMTs limits ELOSS from reaching its ultimate Z resolution. A methodical approach to calibrating PMT anode sensitivities to a single target value by systematic PMT gain corrections is presented. Although the calibration process is discussed in terms of its impact on ELOSS performance, the presented method is applicable to any optical detector system composed of a large number of PMTs needing anode sensitivity calibration.

Instrumentation for heavy-ion accelerators↗

Production of the most neutron-deficient Zn isotopes by projectile fragmentation of Kr 78

The cross sections for the production of three most neutron-deficient zinc isotopes, 54–56 Zn, in the projectile fragmentation of 78 Kr at 345 MeV/nucleon on a beryllium target, were measured. Although the results are smaller by over an order of magnitude from those obtained with a 58 Ni beam at 75 MeV/nucleon on a nickel target, the rates of reaction products are found to be larger in the case of high-energy fragmentation of 78 Kr. The experimental cross sections for the most neutron-deficient isotopes of even-Z nuclei between zinc and krypton were analyzed in the framework of the abrasion-ablation model. A very good agreement with the data was found when the nuclear masses predicted by a particular variant of the Hartree-Fock-Bogoliubov mass model were used. The prospects for the observation of more exotic isotopes in this region are discussed in context of 2p radioactivity.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Abundance of the Radioactive Be-10 in the Cosmic Radiation up to 2 GeVnucleon-l with the Balloon-borne Instrument ISOMAX1998

The Isotope Magnet Experiment (ISOMAX) a balloon-borne superconducting magnet spectrometer was designed to measure the isotopic composition of the light isotopes (3 less than or equal to Z less than or equal to 8) of the cosmic radiation up to 4 GeV nucleon (exp -1) with a mass resolution of better than 0.25 amu by using the velocity vs. rigidity technique. To achieve this stringent mass resolution ISOMAX was comprised of three major detector systems, a magnetic rigidity spectrometer with a precision drift chamber tracker in conjunction with a three-layer time-of-flight system and two silica-aerogel Cherenkov counters for the velocity determination. A special emphasis of the ISOMAX program was the accurate measurement of radioactive Be-10 with respect to its stable neighbor isotope Be-9, which provides important constraints on the age of cosmic rays in the Galaxy. ISOMAX had its first balloon flight on August 4-5, 1998, from Lynn Lake, Manitoba, Canada. Thirteen hours of data were recorded during this flight at a residual atmosphere of less than 5 g per square centimeter. The isotopic ratio at the top of the atmosphere for Be-10/Be-9 was measured to be 0.195 plus or minus 0.036 (statistical) plus or minus 0.039 (systematic) between 0.26 - 1.03GeV nucleon (exp -1) and 0.317 plus or minus 0.109 (statistical) plus or minus 0.042 (systematic) between 1.13 - 2.03GeV nucleon(exp -1). This is the first measurement of its kind above 1 GeV nucleon (exp -1). ISOMAX results tend to be higher than predictions from current propagation models.

Hams, T.↗

An approach for spent nuclear fuel containment integrity verification using gas tagging

Verification of containment integrity is required for spent nuclear fuel (SNF) managed by the commercial nuclear industry and U.S. Department of Energy (DOE), especially after extended storage. Certain SNF storage systems, such as the DOE road-ready dry storage system, hold several packaged containments within a welded over-canister. These packaged containments are called Department of Energy Standard Canisters (DOESCs). DOESC leakage identification is challenging because their containment boundary cannot be accessed for testing and their contents (i.e., SNF and fill gas) are often similar. There are concerns that this could result in costly characterization and repackaging operations of DOE road-ready dry storage systems if compromised DOESCs are suspected. Here, to address these concerns, this paper presents an approach for applying a gas tagging process using xenon to uniquely identify compromised inaccessible containments following extended storage. The containments considered for this application are seven DOESCs, each packaged within a single over-canister. Two different SNF loading configurations from the Advanced Test Reactor and Fort Saint Vrain nuclear power plant are considered. These configurations are used to represent research reactor aluminum-clad spent nuclear fuel (ASNF) and TRi-structural ISOtropic (TRISO) SNF types. Results for this application show that for ASNF and TRISO type fuels for which the selected fuels are representative, the volume of taggant required at loading is determined primarily by the lower detection limit and leak rate of taggant from a compromised DOESC, rather than the amount of fission-generated xenon in the loaded fuel. While the application presented is suited for larger leaks, smaller leaks could be detected by modifying certain design parameters. This gas tagging approach can also be applied to other DOE containments and advanced reactor SNF storage systems.

07 - ISOTOPES AND RADIATION SOURCES↗

The Chronology of Asteroid Accretion, Differentiation, and Secondary Mineralization

We evaluate initial (Al-26/Al-27)(sub I), (Mn-53/Mn-55)(sub I), (Hf-182/Hf-180)(sub I), and Pb-207/Pb-206 ages for igneous differentiated meteorites and chondrules from ordinary chondrites for consistency with radioactive decay of the parent nuclides within a common, closed isotopic system, i.e., the early solar nebula. We find that the relative abundances of Al-26, Mn-53, and Hf-182, here denoted by I(Al)(sub CAI, I(Mn)(sub CAI) and I(Hf)(sub CAI), are consistent with decay from common initial values for the bulk solar system. I(Mn)(sub CAI) and I(Hf)(sub CAI) = 9.1+/-1.7 x 10(exp -6) and 1.06+/-0.09 x 10(exp -6) respectively, correspond to the canonical value of I(Al)(sub CAI) = 5.1 x 10(exp -5). I(Hf)(sub CAI) thus determined is consistent with I(Hf)(sub CAI) = 1.003+/-0.045 x 10(exp -6) directly determined in separate work. I(Mn)(sub CAI) is within error of the lowest value directly determined for CAI. We suggest that erratically higher values directly determined for CAI in carbonaceous chondrites reflect proton irradiation of unaccreted CAIs by the early Sun after other asteroids destined for melting by Al-26 decay had already accreted. The Mn-53 incorporated within such asteroids would have been shielded from further "local" spallogenic contributions. The relative abundances of the short-lived nuclides are less consistent with the Pb-207/Pb-206 ages of the corresponding materials with the best consistency being obtained between (Hf-182/Hf-180)(sub I) and Pb-207/Pb-206 ages of angrites. (Hf-182/Hf-180)(sub I) decreases with decreasing Pb-207/Pb-206 ages at the rate expected from the 8.90+/-0.09 Ma half-life of Hf-182. However, the model "CAI age" thus determined, T(sub CAI,Mn-W) = 4568.6+/-0.7 Ma, is older than the commonly accepted directly measured value T(sub CAI) = 4567.l+/-0.2 Ma. I(Al)(sub I), and (Mn-53/Mn-55)(sub I) are less consistent with Pb-207/Pb-206 ages, but determine T(sub CAI, Mn-Cr) = 4568.3+/-0.5 Ma relative to I(AI)(sub CAI)= 5.1 x 10(exp -5) and a Pb-207/Pb-206 age of 4558.6 Ma for the LEW86010 angrite. However. the (Mn-53/Mn-55)(sub I) and Pb-207/Pb-206 ages of "intermediate" age D'Orbigny-clan angrites and Asuka 881394 are inconsistent with radioactive decay from CAI values with a Mn-55 half-life of 3.7+/-0.4 Ma. in spite of consistency between (Mn-53/Mn-55)(sub I) and (Al-26/Al-27)(sub I). Nevertheless, it appears that the Mn-Cr method with I(Mn)(sub CAI) = 9.1+/-1.7 x 10(exp -6) can be used to date primary igneous events and also secondary mineralization on asteroid parent bodies. We summarize ages thus determined for igneous events on differentiated asteroids and for carbonate and fayalite formation on carbonaceous asteroids.

Nyquist, L. E.↗

Implications of Underground Nuclear Explosion Cavity Evolution for Radioxenon Isotopic Composition

Abstract Isotopic ratios of radioxenons sampled in the atmosphere or subsurface can be used to verify the occurrence of an underground nuclear explosion (UNE). Differences in the half-lives of radioactive xenon precursors and their decay-chain networks produce different time-dependent concentration profiles of xenon isotopes allowing isotopic ratios to be used for tracking UNE histories including estimating the time of detonation. In this study, we explore the potential effects of post-detonation cavity processes: precipitation of iodine precursors, gas seepage, and prompt venting on radioxenon isotopic evolution which influences UNE histories. Simplified analytical models and closed-form solutions yielding a potentially idealized radioactive decay/ingrowth chain in a closed and well-mixed system typically have limited application by not including the partitioning of the radionuclide inventory between a gas phase and rock melt created by the detonation and by ignoring gas transport from the cavity to host rock or ground surface. In reality, either subsurface transport or prompt release that is principally responsible for gas signatures violates the closed-system (or batch-mode) assumption. A closed-form solution representing time-dependent source-term activities is extended by considering the cavity partitioning process, slow seepage, and/or prompt release of gases from the cavity and applied to realistic systems.

Sun, Yunwei (ORCID:0000000194801439)↗

Radioactivities induced in some LDEF samples

Final activities are reported for gamma ray emitting isotopes measured in 35 samples from LDEF. In 26 steel trunnion samples, activities of Mn-54 and Co-57 were measured and limits set on other isotopes. In five Al end support retainer plates and two Al keel plate samples, Na-22 was measured. In two Ti clip samples, Na-22 was measured, limits for Sc-46 were obtained, and high activities for impurity Uranium and daughter isotopes were observed. Four sets of depth vs activity profiles were measured for the D sections of the trunnion. For all 4 profiles, the activities first decreased with increasing distance from the surface of the trunnion but were fairly flat near the center. These profiles are consistent with production by both the lower energy (approx. 100 MeV) trapped particles and high energy (approx. 10 GeV) galactic-cosmic ray particles. For the near surface samples, the earth quadrant had more Mn-54 than the space quadrant. For the D sections, there was less Mn-54 in the east trunnion than in the west trunnion. Comparisons are made among the samples and with activities measured by others. The limit for Sc-46 in the Ti clips is compared with the activities of Mn-54 produced in the steel pieces by similar reactions. Activities predicted by several models are compared with the measured activities.

Reedy, Robert C.↗

Decay spectroscopy in the neutron-rich Mo–Ru–Pd region

A leading challenge of nuclear-structure research is to understand the properties of nuclides of extreme isospin. Experiments at radioactive-ion-beam facilities, such as the Facility for Rare Isotope Beams in the US, may answer key questions that address diverse topics including fundamental nuclear physics, stellar nucleosynthesis and nuclear applications. The neutron-rich Mo–Ru–Pd (Z = 42 – 46) nuclides are hypothesised to exhibit triaxial-oblate deformation. We performed an experiment with the Facility for Rare Isotope Beams Decay Station initiator (FDSi) to study the structure and decay properties of nuclides in this region. Over 100 different nuclides have been identified in a preliminary analysis of the data. This work presents a first look at several examples between Rb (Z = 37) and Ag (Z = 47). Performance of the FDSi and methods developed to measure ground-state and excited-state lifetimes are presented, and plans for future work are also discussed.

Allmond, James [ORNL] (ORCID:0000000165338721)↗

First measurement of proton decay from a transfer reaction to 21 Na

Decay protons from excited states in Na 21 populated through a previously reported Mg 24 ( p , α ) Na 21 transfer reaction [Cha et al. , Phys. Rev. C 96 , 025810 (2017) ] were analyzed to extract the proton branching ratios of the energy levels. Additionally, by utilizing 31-MeV proton beams from the Holifield Radioactive Ion Beam Facility of Oak Ridge National Laboratory and isotopically enriched Mg 24 solid targets, the decay protons were detected in coincidence with α particles from the ( p , α ) reaction using a silicon strip detector array. Proton decay branching ratios of several Na 21 levels were deduced for the p 0 and p 1 decay channels to the ground and first excited states in Ne 20 , respectively.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Search for and analysis of radioactive halos in lunar material

The lunar halo search was conducted because halos in terrestrial minerals serve as pointers to localized radioactivity, and make possible analytical studies on the problems of isotopic dating and mode of crystallization of the host mineral. Ancillary studies were conducted on terrestrial halos and on certain samples of special origin such as tektites and meteorites.

Gentry, R. V.↗