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At least 685 records · Page 38

Harvesting 62 Zn from an aqueous cocktail at the NSCL

“Isotope harvesting” is a technique that offers access to exotic radionuclides created as by-products during nuclear science research. Ongoing exploratory work at the National Superconducting Cyclotron Laboratory (NSCL) is directed towards the production and extraction of rare radionuclides from a flowing-water target and intends to pave the way for future harvesting efforts at the upcoming Facility for Rare Isotope Beams (FRIB). Here in this paper, we present the collection of 62 Zn from an aqueous matrix irradiated with a 150 MeV/nucleon 78Kr beam, while synergistically capturing other gaseous reaction products. In addition to the production rate for 62 Zn (9.08(30)E-5 62 Zn per incoming 78 Kr), the rates of formation for several other radionuclides were determined as well. The purification of 62 Zn from a large number of co-produced radionuclides was performed by anion exchange chromatography, allowing the isolation of 80.5(5.2) % of the generated 62 Zn. With the decay of 62 Zn the radioactive daughter 62 Cu is generated, and with the isolation of pure 62 Cu eluate, the principle of a medical radionuclide generator could be demonstrated. To illustrate the applicability of the obtained 62 Zn, the isolated product was used in free and DTPA-labelled form in a proof of principle plant uptake study with garden cress employing phosphor imaging for visualization.

07 ISOTOPE AND RADIATION SOURCES↗

NEUTRINO-DRIVEN WINDS IN THE AFTERMATH OF A NEUTRON STAR MERGER: NUCLEOSYNTHESIS AND ELECTROMAGNETIC TRANSIENTS

We present a comprehensive nucleosynthesis study of the neutrino-driven wind in the aftermath of a binary neutron star merger. Our focus is the initial remnant phase when a massive central neutron star is present. Using tracers from a recent hydrodynamical simulation, we determine total masses and integrated abundances to characterize the composition of unbound matter. We find that the nucleosynthetic yields depend sensitively on both the life time of the massive neutron star and the polar angle. Matter in excess of up to 9 × 10{sup −3} M{sub ⊙} becomes unbound until ∼200 ms. Due to electron fractions of Y{sub e} ≈ 0.2–0.4, mainly nuclei with mass numbers A < 130 are synthesized, complementing the yields from the earlier dynamic ejecta. Mixing scenarios with these two types of ejecta can explain the abundance pattern in r-process enriched metal-poor stars. Additionally, we calculate heating rates for the decay of the freshly produced radioactive isotopes. The resulting light curve peaks in the blue band after about 4 hr. Furthermore, high opacities due to heavy r-process nuclei in the dynamic ejecta lead to a second peak in the infrared after 3–4 days.

79 ASTRONOMY AND ASTROPHYSICS↗

First principles calculations in support of Pu aging: calculating the effects of lattice imperfections on thermodynamics

Plutonium (Pu) has, in theory, well defined crystal structures: its atoms are arranged in regular spatial patterns. But Pu is radioactive, and as its nuclei decay those regular spatial patterns are interrupted. The interruptions are lattice imperfections, which are known to affect how materials respond to their environment. To adequately model Pu, we need to know which lattice imperfections are present, how they interact with each other, and how they affect the material’s response to its environment. The work presented here aims to use density functional theory (DFT) calculations to begin to answer the latter, in particular, how individual lattice imperfections affect measurable effects including thermal expansion (the change in volume in response to a change in temperature), heat capacity (the amount of thermal energy needed to change a material’s temperature), and elastic moduli (a material’s resistance to applied stresses). Pu poses many computational challenges. The $\textit{f}$ electrons require special attention. Of all the elements, Pu has the largest number of electrons that must be included in the calculations. Thermal effects require calculating the phonons (the lattice vibrations), which for systems containing lattice imperfections demand large, complex computational cells - but computational resources limit the size and complexity. With careful restructuring of how the calculations are performed, all these challenges have been met to enable calculations that provide insight into how lattice imperfections affect Pu’s response to its environment. Reported here are the computational challenges and the advances developed to meet them, along with the first results showing the strong effect that one prototype lattice imperfection (an interstitial Pu atom in a delta-phase Pu lattice) has on Pu’s response to its environment.

36 MATERIALS SCIENCE↗

Short-lived nuclei in the early solar system

An overview is given of the existence and abundance of short-lived nuclei that were present in the early solar system. It is shown that there are excesses of certain isotopes that may be assigned to the decay of short-lived radioactive nuclei corresponding to an abundance of about 0.0001 relative to a neighboring stable isotope. This abundance is roughly similar to the level of general nonlinear isotopic anomalies present in meteoritic material (excluding oxygen) which are not attributable to short-lived nuclei. If these results are representative of the bulk solar system, they indicate that about 0.0001 solar mass of freshly synthesized material of peculiar composition was added to the protosolar nebula as it was formed from the interstellar medium. This material must have been synthesized about three million yr before the formation of the solar system.

Wasserburg, G. J.↗

Gamma-ray observations of NGC 253 and M82 with OSSE

Gamma-ray observations of the nearby starburst galaxies NGC 253 and M82 over the energy range (0.05-10) MeV have been obtained with the Oriented Scintillation Spectrometer Experiment (OSSE) spectrometer on the Compton Gamma-Ray Observatory (CGRO). The priority of these galaxies as OSSE targets had been established on the grounds that the average supernova rate may be high in starbursts as indicated by infrared and radio observations, and at distances of approximately 3 Mpc a significant chance of supernova gamm-ray line detection exists. NGC 253 was detected in continuum emission up to 165 keV with a total significance of 4.4 sigma and an estimated luminosity of 3 x 10(exp 40) ergs/s. The spectrum is best fit by a power law of photon index approximately 2.5. We consider the possible contribution of different emission mechanisms, including inverse Compton scattering, bremsstrahlung, discrete sources, and Type Ia/Ib supernova continuum to the measured flux. No significant continuum flux was observed from M82. A search for the gamma-ray line from the decay of the most abundant radioactive element produced in supernovae (Ni-56 yields Co-56 yields Fe-56) yielded no significant detection: the 3 sigma upper limits to the line fluxes at 0.158, 0.812, 0.847, and 1.238 MeV for both galaxies are obtained.

Bhattacharya, D.↗

Processes in Early Planetesimals: Evidence from Ureilite Meteorites

Ureilites are primitive ultramafic achondrites composed largely of olivine and pigeonite, with minor augite, carbon, sulphide and metal. They represent very early material in the history of the Solar System and form a bridge between undifferentiated chondrites and fully differentiated asteroids. They show a mixture of chemical characteristics, some of which are considered to be nebula-derived (e.g. a negative correlation between Mg/Fe and Delta O-17 that resembles that of the ordinary chondrites but at lower Delta O-17 values) whereas others have been imposed by asteroidal differentiation. Carbon isotope data show a striking negative correlation of delta C-13 values with mg# in olivine. delta C-13 also correlates positively with Delta O-17, and therefore this isotopic variation was probably also nebula-derived. Thus, oxygen and carbon isotope compositions and Fe-Mg systematics of each monomict ureilite were established before differentiation processes began. Heated by decay of short-lived radioactive isotopes, the ureilite asteroid started to melt. Metal and sulphide would have melted first, forming a Fe-S eutectic liquid, which removed chalcophile elements and incompatible siderophile elements, and basaltic melts that removed Al, Ca and the LREE. Several elements show different abundances and/or correlations with Fo content in olivine, e.g. carbon shows a positive correlation in ferroan ureilites, and a weak or even negative correlation in more magnesian compositions. HSE such as Os and Ir also show different distributions, i.e. ureilites with Fo < 82 have very scattered Os and Ir concentrations, which reach high values, whereas ureilites with Fo > 82 tend to have much less scattered and overall lower Os and Ir abundances. A similar change in elemental behaviour is shown by the Fe-Mn relations in ureilitic olivines: those with Fo contents < 85 show a good negative correlation, whereas those with Fo > 85 show much greater scatter. This suggests that a major change affected the parent body at a time when melting had reached relatively magnesian bulk compositions. We consider that this event may have been a hit and run collision in which the ureilite parent body collided with a larger object. During the collision, the ureilite mantle broke up catastrophically but re-accreted in a jumbled state around the still-intact core. Mg-rich basaltic melts that were in the process of being formed at the time of break-up were retained in part as melt clasts that re-accreted to the regolith and are found in polymict ureilites.

Mittlefehldt, David W.↗

Aqueous Alteration

A secondary process whereby liquid water modified the nature of anhydrous primary nebular components. In general, this process induced decomposition and changed the structures and compositions of primary minerals and formed secondary minerals in their place. This process occurred in the early history of meteorite parent bodies that contained water ice. The most effective heat source is considered to be the decay of short-lived radioactive nuclide such as Aluminium-26, but other causes have been suggested. The degree of aqueous alteration of meteorites is categorized as type 1 (most altered) to type 3 (least altered), according to mineralogy and petrology.

Kebukawa, Yoko↗

Expanded Content Envelope For The Model 9977 Packaging

An Addendum was written to the Model 9977 Safety Analysis Report for Packaging adding a new content consisting of DOE-STD-3013 stabilized plutonium dioxide materials to the authorized Model 9977 contents. The new Plutonium Oxide Content (PuO{sub 2}) Envelope will support the Department of Energy shipment of materials between Los Alamos National Laboratory and Savannah River Site facilities. The new content extended the current content envelope boundaries for radioactive material mass and for decay heat load and required a revision to the 9977 Certificate of Compliance prior to shipment. The Addendum documented how the new contents/configurations do not compromise the safety basis presented in the 9977 SARP Revision 2. The changes from the certified package baseline and the changes to the package required to safely transport this material is discussed.

42 ENGINEERING↗

High-temperature 205 Tl decay clarifies 205 Pb dating in early Solar System

Radioactive nuclei with lifetimes on the order of millions of years can reveal the formation history of the Sun and active nucleosynthesis occurring at the time and place of its birth. Among such nuclei whose decay signatures are found in the oldest meteorites, 205 Pb is a powerful example, as it is produced exclusively by slow neutron captures (the s process), with most being synthesized in asymptotic giant branch (AGB) stars. However, making accurate abundance predictions for 205 Pb has so far been impossible because the weak decay rates of 205 Pb and 205 Tl are very uncertain at stellar temperatures. To constrain these decay rates, we measured for the first time the bound-state β - decay of fully ionized 205 Tl 81+ , an exotic decay mode that only occurs in highly charged ions. The measured half-life is 4.7 times longer than the previous theoretical estimate and our 10% experimental uncertainty has eliminated the main nuclear-physics limitation. With new, experimentally backed decay rates, we used AGB stellar models to calculate 205 Pb yields. Propagating those yields with basic galactic chemical evolution (GCE) and comparing with the 205 Pb/ 204 Pb ratio from meteorites, we determined the isolation time of solar material inside its parent molecular cloud. We find positive isolation times that are consistent with the other s-process short-lived radioactive nuclei found in the early Solar System. Our results reaffirm the site of the Sun’s birth as a long-lived, giant molecular cloud and support the use of the 205 Pb– 205 Tl decay system as a chronometer in the early Solar System.

79 ASTRONOMY AND ASTROPHYSICS↗

Modular Total Absorption Spectrometer at the HRIBF (ORNL, Oak Ridge)

The Modular Total Absorption Spectrometer (MTAS) array has been designed, constructed, characterized, and applied to the decay studies of {sup 238}U fission products at the Holifield Radioactive Ion Beam Facility (HRIBF) at Oak Ridge National Laboratory. A MTAS commissioning run was performed in January 2012 at the mass separator on-line to the HRIBF Tandem accelerator. Preliminary results of MTAS data confirm known decay patterns of {sup 142}Ba and {sup 142}La deduced from an earlier study using a total absorption spectrometer technique.

43 PARTICLE ACCELERATORS↗

KATRIN background due to surface radioimpurities

The goal of the KArlsruhe TRItrium Neutrino (KATRIN) experiment is the determination of the effective electron antineutrino mass with a sensitivity of 0.2 eV/c 2 at 90 % C.L. 1 . This goal can only be achieved with a very low background level in the order of 10 mcps 2 in the detector region of interest. A possible background source are α-decays on the inner surface of the KATRIN Main Spectrometer. Rydberg atoms, produced in sputtering processes accompanying the α-decays, are not influenced by electric or magnetic fields and freely propagate inside the vacuum of the Main Spectrometer. Here, they can be ionized by thermal radiation and the released electrons directly contribute to the KATRIN background. Two α-sources, 223 Ra and 228 Th, were installed at the Main Spectrometer with the purpose of temporarily increasing the background in order to study α-decay induced background processes. In this paper, we present a possible background generation mechanism and measurements performed with these two radioactive sources. Our results show a clear correlation between α-activity on the inner spectrometer surface and background from the volume of the spectrometer. Two key characteristics of the Main Spectrometer background – the dependency on the inner electrode offset potential, and the radial distribution – could be reproduced with this artificially induced background. These findings indicate a high contribution of α-decay induced events to the residual KATRIN background.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Investigation of the excited states of 114 Sn using the GRIFFIN spectrometer at TRIUMF

The semi-magic 110-122 Sn isotopes display signs of shape coexistence in their excited 0 + states, which, in contrast to the spherical 0+ ground states, are deformed. Here, this paper investigates the nuclear structure of 114 Sn using the competing β + decay and electron capture of a radioactive beam of 114 Sb produced at the TRIUMF-ISAC facility using the GRIFFIN spectrometer. This study will allow for an in-depth understanding of the excited 0 + states in 114 Sn, by focusing on their decay patterns. In the present experiment, transitions at 856.2-keV and 1405.0-keV, which were observed in an earlier β + decay study but not placed in the 114 Sn level scheme, have been Physics, assigned to the level scheme in connection to the 0$^+_3$ level at 2156.0-keV. Properly assigning these transitions refines the level scheme and enhances our understanding of the nuclear structure in 114 Sn.

GRIFFIN↗

Ion Manipulation from Liquid Xe to Vacuum: Ba-Tagging for a nEXO Upgrade and Future 0 νββ Experiments

Neutrinoless double beta decay (0𝜈𝛽𝛽) provides a way to probe physics beyond the Standard Model of particle physics. The upcoming nEXO experiment will search for 0𝜈𝛽𝛽 decay in 136 Xe with a projected half-life sensitivity exceeding 10 28 years at the 90% confidence level using a liquid xenon (LXe) Time Projection Chamber (TPC) filled with 5 tonnes of Xe enriched to ∼90% in the 𝛽𝛽-decaying isotope 136 Xe. In parallel, a potential future upgrade to nEXO is being investigated with the aim to further suppress radioactive backgrounds and to confirm 𝛽𝛽-decay events. This technique, known as Ba-tagging, comprises extracting and identifying the 𝛽𝛽-decay daughter 136 Ba ion. One tagging approach being pursued involves extracting a small volume of LXe in the vicinity of a potential 𝛽𝛽-decay using a capillary tube and facilitating a liquid-to-gas phase transition by heating the capillary exit. The Ba ion is then separated from the accompanying Xe gas using a radio-frequency (RF) carpet and RF funnel, conclusively identifying the ion as 136 Ba via laser-fluorescence spectroscopy and mass spectrometry. Simultaneously, an accelerator-driven Ba ion source is being developed to validate and optimize this technique. The motivation for the project, the development of the different aspects, along with the current status and results, are discussed here.

a-tagging↗

Feasibility study of SiGHT: a novel ultra low background photosensor for low temperature operation

Rare event search experiments, such as those searching for dark matter and observations of neutrinoless double beta decay, require ultra low levels of radioactive background for unmistakable identification. In order to reduce the radioactive background of detectors used in these types of event searches, low background photosensors are required, as the physical size of these detectors become increasing larger, and hence the number of such photosensors used also increases rapidly. Considering that most dark matter and neutrinoless double beta decay experiments are turning towards using noble liquids as the target choice, liquid xenon and liquid argon for instance, photosensors that can work well at cryogenic temperatures are required, 165 K and 87 K for liquid xenon and liquid argon, respectively. The Silicon Geiger Hybrid Tube (SiGHT) is a novel photosensor designed specifically for use in ultra low background experiments operating at cryogenic temperatures. It is based on the proven photocathode plus silicon photomultiplier (SiPM) hybrid technology and consists of very few other, but also ultra radio-pure, materials like fused silica and silicon for the SiPM. Lastly, the introduction of the SiGHT concept, as well as a feasibility study for its production, is reported in this article.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Choosing the Best Modeling Platform for Radiological Risk Assessment Models - 20468

Radiological risk assessments, in the form of performance or safety assessments, are often required under regulations or guidance for remediation of contaminated land, decommissioning of contaminated buildings or structures, and radioactive waste disposal. These risk assessments are usually supported by fate and transport models that address decay and ingrowth of radionuclides, as well as their movement through engineered systems and the natural environment. These models are often projected thousands, or more, years into the future, largely because the radioactive species change through decay and ingrowth, and hence the magnitude of the radioactive effect changes with time. There are many computer codes that are available to address this type of modeling. They range from addressing specific pathways or processes such as infiltration of water, groundwater, surface water, air, biota, diffusion and advection of water and gases, to those that try to couple all processes together to evaluate the impact of fate and transport through the entire system to places in space and time to which access is assumed. These different types of codes are sometimes separated with the monikers process-level and systems-level codes, although it is often not clear that this separation does justice to the capabilities of the many codes that are available to evaluate fate and transport of radionuclides. The focus of this paper is the latter group of modeling codes. Several systems level modeling codes exist and are used. There are differences between these codes in terms of utility, flexibility, complexity and cost. The purpose of this paper is to compare a few of these codes in the context of work currently being performed by the International Atomic Energy Agency (IAEA) Modeling and Data for Radiological Impact Assessments (MODARIA) II Working Group 1 (WG1). The MODARIA II WG1's main focus is how stakeholder engaged decision analysis can, or should, be applied to radiological contamination problems so that better, longstanding, sustainable, solutions are reached. However, the WG1 also recognizes the potential impact of the modeling tools that are chosen to address radiological risk, which is often a primary objective of decision making for radiological problems. Other objectives might also be important, such as constraining costs, obtaining financing, minimizing impact on ecosystems, saving cultural resources, saving jobs, farmland, environmental justice, etc., in a full decision analysis for a given radiological contamination problem, but none of these other objectives have the same types of complex modeling needs as minimize radiological dose. Consequently, a further focus of WG1 is to evaluate the potential impacts on decision making of the choice of fate and transport, and risk assessment, modeling codes that are used to support decision making. The WG1 will produce a report at the end of 2020 that will focus on an approach to effective decision making and stakeholder engagement. The report will also consider the role that performance assessment modeling should play in the decision-making process, including the impact of the choice of modeling tools or computer codes on risk-informed decision making. Several sites around the World have been made available by Member States for these model comparisons, and several modeling tools have been considered. However, the focus of this paper is on two of the sites, one in Belgium and one in Ukraine, and on three of the tools: NORMALYSA (NORM And Legacy Site Assessment); GoldSim{sup C}, and AMBER{sup C}. The final report from this working group will also cover other modeling tools, including RESRAD, and PC-Cream{sup R}. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

FY14 Annual Report

The neutrinos and neutrons emitted in nuclear β decay can be precisely studied using radioactive ions held in a radiofrequency-quadrupole ion trap. The momentum and energy of particles that would otherwise be difficult (or even impossible) to detect can be reconstructed from the momentum imparted to the recoiling nucleus. The β-delayed neutron emission for isotopes of interest for r-process nucleosynthesis is being studied. Measurements of β-decay angular correlations, which are sensitive to exotic particles and other phenomena beyond the Standard Model, can be improved by reconstructing the complete decay kinematics of the mirror 8 Li and 8 B β ± decays. This research is well aligned with the Nuclear Science Advisory Committee Long Range Plan under NSAC Performance Evaluation Milestones: (1) NA6, part of which is to measure decay properties of selected neutron-rich nuclei in the r-process, and (2) FI4, to improve measurements of nuclear β decay to constrain physics beyond the Standard Model.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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)↗