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DOE OSTI2020

β -decay half-lives of 55 neutron-rich isotopes beyond the N = 82 shell gap

The β -decay half-lives of 55 neutron-rich nuclei Sn 134 - 139 , Sb 134 - 142 , Te 137 - 144 , I 140 - 146 , Xe 142 - 148 , Cs 145 - 151 , Ba 148 - 153 , and La 151 - 155 were measured at the Radioactive Isotope Beam Factory employing the projectile fission fragments of U 238 . The nuclear level structure, which relates to deformation, has a large effect on the half-lives. The impact of newly measured half-lives on modeling the astrophysical origin of the heavy elements is studied in the context of r process nucleosynthesis. For a wide variety of astrophysical conditions, including those in which fission recycling occurs, the half-lives have an important local impact on the second ( A ≈ 130) peak.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

A Comparison of Groundwater Sampling Technologies, Including Passive Diffusion Sampling, for Radionuclide Contamination - 20205

Using traditional high-flow purge methods for long-term water quality monitoring of deep groundwater wells can be expensive, affect contaminant migration, and produce excessive volumes of discharge water that can be difficult to manage. The use of low-flow pumping methods and depth discrete bailers (DDBs) can reduce the cost of sampling deep groundwater wells. In general, using different pumping methods to obtain reproducible and representative groundwater can be challenging. Passive diffusion samplers (PDSs) have successfully been used in long-term monitoring for volatile organic compounds, major ions, and trace-elements, but application has been limited for stable and radioactive isotopes. Beginning in 2018, the United States Geological Survey (USGS) conducted three sampling events to test the ability of PDSs and DDBs to obtain reproducible and representative groundwater samples. The sampled well is completed in a regional, permeable carbonate aquifer and is one in a set of wells that have historically been used for tritium tracer testing. All samples were obtained at 180 m (590 ft) below land surface (bls) in a 13.97 cm (5.5 inch) uncased well that has a total depth of 202 m (662 ft) bls. The first sampling event deployed a regenerated cellulose dialysis membrane (RCDM) PDS for 14 days with deionized water as the blank. The second sampling event deployed a RCDM for 27 days also with deionized water as the blank. The third sampling event deployed a Dual Membrane (DM) PDS for 65 days using a blank of tritium-dead carbonate water. The DM PDS was used to assess the effect of longer term deployment on tritium concentrations and address whether or not the PDSs reached equilibrium with ambient groundwater. The day after each of the three passive samplers were retrieved a DDB was used to obtain discrete non-integrated groundwater samples. For each DDB sampling day, the bailer was lowered into the well 10 consecutive times to determine if the water chemistry changed from the first to the last bailed sample. Quality assurance samples including blanks and duplicates were obtained during all three sampling events. All blank waters had tritium concentrations less than 21±33 pCi/L. Major ion (e.g. calcium, chloride, sodium, and sulfate) results were compared between all samples obtained with RCDM and DDB. Major ion concentrations showed a coefficient of variation of less than 6% between all RCDM and DDB samples; however, the coefficient of variation between the different deployment times and the two different methods for trace-element concentrations was much larger, particularly for manganese (82%), lead (41%), and zinc (33%). Stable isotope values were compared between the RCDM and DDB samples. The DDB sample results all fell within analytical uncertainty and were considered representative of the formation groundwater. The stable isotope values from the RCDM samples indicated that a longer deployment time was necessary to gain equilibrium and to obtain representative groundwater samples. Tritium results from groundwater samples obtained from the RCDM, DM, and DDB indicate that groundwaters obtained with PDSs produced tritium concentrations 2 to 3 times higher (between 1,426 and 3,060±87 pCi/L) than groundwaters obtained with a DDB (479 to 1,219±51 pCi/L). The longer the passive diffusion samplers were deployed, the higher the tritium concentration, suggesting that equilibrium with tritium was not reached within a 27-day deployment. DDB samples showed tritium results declining from the first to the last bailed sample for all three sampling events. This research suggests that tritium results from groundwater samples obtained from PDSs are more reproducible than samples obtained from DDBs. Also, PDSs likely do not accumulate isotopes of water but rather equilibrate with the ambient groundwater. On the other hand, both PDSs and DDBs were able to provide representative groundwater samples for major ions and have the potential to produce representative groundwater samples for stable isotopes of water (δD and δ{sup 18}O). Utilizing the most effective method for sampling groundwater is important for long-term groundwater monitoring. Quantifying the ability of passive diffusion groundwater samplers to obtain representative radioactive chemistry samples will help determine if these methods can be a useful alternative to pumping and purging wells for long-term monitoring. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS1973

The relative abundance of the isotopes of Li, Be and B and the age of cosmic rays

Using a balloon borne double dE/dx total energy telescope, we have determined the isotopic composition of cosmic ray Li, Be and B nuclei in the energy range 100-250 MeV/nuc. The measured mass resolution for these nuclei is about 0.3 AMU. The observed isotopic composition is in agreement with that predicted on the basis of interstellar fragmentation with the exception of a deficiency of Be-10. If the low abundance of Be-10 is attributed to the decay of this radioactive isotope, we obtain a mean cosmic ray lifetime of 3.4 (plus 3.4 or minus 1.3) m.y.

Webber, W. R.↗

DOE OSTI2022

Time-of-flight experiments for nuclear structure and astrophysics

Neutron-rich isotopes are atomic nuclei with a large neutron excess compared to their stable counter parts. Their study provides essential information to understand the properties of the nuclear interaction, and to model nuclear processes in extreme astrophysical environments where neutron-rich isotopes drive the chains of nuclear reactions. Experimentally, these unstable isotopes are difficult to study because of their short half-lives and low production yields at particle accelerator laboratories. The TOF-Bρ technique is a mass measurement technique specialized for experiments with fast beams of short-lived radioactive isotopes. In this project we used the technique for two experiments performed at the National Superconducting Cyclotron Laboratory to measure new masses of isotopes in the region of 112 Mo and 46 S. The experiments at the NSCL were complemented by the development of new timing radiation detectors and experimental techniques to improve the performance and reach of mass measurements on neutron-rich isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Radiological Source Term Estimation and Isotopic Identification with Parallel Log Domain Particle Filters

This paper presents a parallel log-domain particle filtering algorithm combined with gamma spectrum unfolding to perform localization, identification, and evaluation of multiple point sources of various isotopes in an environment with attenuating obstacles. The method uses sets of precomputed attenuation kernels that map the attenuation characteristics of the environment. These kernels are specific to the energy level of a photopeak of interest. The spectral measurements are deconvolved into count measurements of each photopeak. These count measurements are fed into a set of parallel particle filters using attenuation kernels computed for that photopeak’s energy level. The individual regularized particle filters perform all likelihood calculations in the logarithmic domain to mitigate the effects of particle degeneracy. The output of each particle filter is combined to estimate which isotopes are present as well as their positions and strengths. The performance of the algorithm is characterized in a lab-scale environment using a mobile robot equipped with a gamma ray spectrometer in the presence of up to three different radioactive isotopes simultaneously. The sources were localized to within 10 cm, and their strengths were estimated within 10% of their true values. Furthermore, the isotopes were all correctly identified, and no spurious sources were reported.

42 ENGINEERING↗

DOE OSTI2023

Cubical moderators for the Neutron Target Demonstator (NTD)

Neutron capture cross sections of unstable isotopes are important for neutron induced nucleosynthesis as well as for technological applications. The traditional time-of-flight method reaches its limits once the necessary detection of the reaction products is hampered by the size (mass) of the sample. Several factors may limit the sample mass: The decay properties of radioactive isotopes interfere with the signals from the neutron capture or neutron-induced fission reactions; The limited range of charged reaction products requires a thin sample. In both cases, an increased neutron fluence at the sample position with ever improved neutron sources overcomes the lack of reaction rate. Reference proposed a combination of a radioactive beam facility, an ion storage ring and a spallation neutron source surrounded by neutron moderator. This idea is part of the LANSCE strategy to stay a worldwide leader for neutron induced research. Figure 1 shows a sketch of the proposed future setup.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Replacement of Fly Ash with Natural Pozzolans in Cementitious Waste Forms: Progress Report

The Department of Energy Environmental Management (DOE EM) Office is currently responsible for treating radioactive and mixed waste, environmental restoration, and closing contaminated tanks and facilities resulting from radioactive isotope production for defense applications during the Cold War. Cementitious reagents are the most widely used materials for (1) chemically stabilizing and encapsulating radionuclides and hazardous metals contaminated with radionuclides and Resource Conservation and Recovery Act (RCRA) hazardous metals and (2) solidifying radioactive and mixed wastewater for final disposal. Cementitious grouts and flowable concretes are also the most widely used materials for DOE waste tank and facility closures.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

MeV Gamma Rays from Fission: A Distinct Signature of Actinide Production in Neutron Star Mergers

Neutron star mergers (NSMs) are the first verified sites of rapid neutron capture (r-process) nucleosynthesis, and could emit gamma rays from the radioactive isotopes synthesized in the neutron-rich ejecta. These MeV gamma rays may provide a unique and direct probe of the NSM environment as well as insight into the nature of the r process, just as observed gammas from the 56 Ni radioactive decay chain provide a window into supernova nucleosynthesis. In this work, we include the photons from fission processes for the first time in estimates of the MeV gamma-ray signal expected from an NSM event. We consider NSM ejecta compositions with a range of neutron richness and find a dramatic difference in the predicted signal depending on whether or not fissioning nuclei are produced. The difference is most striking at photon energies above ~3.5 MeV and at a relatively late time, several days after the merger event, when the ejecta is optically thin. We estimate that a Galactic NSM could be detectable by a next generation gamma-ray detector such as AMEGO in the MeV range, up to ~104 days after the merger, if fissioning nuclei are robustly produced in the event.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2026

Presupernova O–C Shell Mergers Could Produce More 44 Ti than the Explosion

The formation of 44 Ti in massive stars is thought to occur during explosive nucleosynthesis; however, recent studies have shown it can be produced during O–C shell mergers prior to core collapse. We investigate how mixing according to 3D macrophysics derived from hydrodynamic simulations impacts presupernova O–C shell merger nucleosynthesis and if it can dominate explosive supernova production of 44 Ti and other radioactive isotopes. We compare a range of observations and models of explosive 44 Ti yields to preexplosive multizone mixing–burning nucleosynthesis simulations of an O–C shell merger in a 15 M ⊙ Z = 0.02 stellar model with mixing conditions corresponding to different 3D hydrodynamic mixing scenarios. Radioactive species produced in the O shell have a multidex spread in preexplosive yield predictions across different 3D mixing scenarios of 1.54 and 2.14 dex on average, depending on mass cut. 44 Ti has the largest spread of 4.78 and 4.81 dex depending on mass cut. Further, we show that the preexplosive production of 44 Ti can be larger than the explosive production of models and can match observations. Our results also show that 3D mixing physics enhances 44 Ti in 1D models without modifying 56 Ni yields. We conclude that quantitative predictions of 44 Ti and other radioactive species more broadly require an understanding of the 3D hydrodynamic mixing conditions present during the O–C shell merger.

Issa, Joshua [University of Victoria, BC (Canada);↗

DOE OSTI2020

The ENDF/B-VIII.0 Compendium Volume I: Neutron Cross Section Plots

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2020

The ENDF/B-VIII.0 Compendium Volume II: Neutron Cross Section Rank-Order Analyses

Version 8 of the Evaluated Nuclear Data File (ENDF/B-VIII.0) contains a wealth of nuclear data representing the most recent collection of evaluated neutron cross section measurements, isotopic radioactive decay, and much more. This Compendium has been prepared as a easily-navigable reference of the contents of the ENDF/B-VIII.0 library, while making no statement regarding the accuracy of those contents. The Compendium is split into four volumes. Volume II presents a series of tables of reaction cross section values for thermal (0.025 eV), fission (1 MeV), and fusion (14 MeV) energies, each sorted by cross section value, isotope, and element-then-isotope to facilitate quick searches.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2024

Galactic chemical evolution with the short-lived isotopes 53 Mn, 60 Fe, 182 Hf, and 244 Pu

We run a three-dimensional Galactic chemical evolution (GCE) model to follow the propagation of 53 Mn from supernovae of type Ia (SNIa), 60 Fe from core-collapse supernovae (CCSNe), 182 Hf from intermediate mass stars (IMSs), and 244 Pu from neutron star mergers (NSMs) in the Galaxy. We compare the GCE of these short-lived radioactive isotopes (SLRs) to recent detections on the deep-sea floor. We find that although these SLRs originate from different sites, they often arrive conjointly on Earth.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Mitigation of Cosmic Rays-Induced Errors in Superconducting Quantum Processors

Environmental radioactivity and cosmic-rays have recently been identified as a source of decoherence in super-conducting quantum bits (qubits). In particular, the absorption of cosmic-ray muons and gamma rays emitted by naturally occurring radioactive isotopes in the qubit substrate leads to correlated errors in superconducting quantum processors, posing significant challenges to quantum error correction. To enable quantum computing to scale, it is therefore necessary the devel-opment of mitigation strategies to prevent, or keep under control, error bursts due to particle impacts in the chip. While most environmental radioactive sources can be effectively suppressed using dedicated shielding, cosmic-ray muons, with their high penetration capability, can only be mitigated by moving the entire facility in a deep underground laboratory. This work explores the potential for developing a novel class of quantum processors equipped with an active veto system to protect superconducting-based quantum computers from the detrimental effects of atmospheric muons. Such a device would enable the identification of an atmospheric muon interaction within the processor and veto all operations performed during the occurrence of such an interaction. By demonstrating high detection efficiency and negligible dead time, we aim to establish that the future of quantum processors can be envisioned in above-around facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA NTRS2004

Nuclear Physics in Space: What We Can Learn From Cosmic Rays

Studies and discoveries in cosmic-ray physics and generally in Astrophysics provide a fertile ground for research in many areas of Particle Physics and Cosmology, such as the search for dark matter, antimatter, new particles, and exotic physics, studies of the nucleosynthesis, origin of Galactic and extragalactic gamma-ray diffuse emission, formation of the large scale structure of the universe etc. In several years new missions are planned for cosmic-ray experiments, which will tremendously increase the quality and accuracy of cosmic-ray data. On the other hand, direct measurements of cosmic rays are possible in only one location on the outskirts of the Milky Way galaxy and present only a snapshot of very dynamic processes. It has been recently realized that direct information about the fluxes and spectra of cosmic rays in distant locations is provided by the Galactic diffuse gamma-rays, therefore, complementing the local cosmic-ray studies. A wealth of information is also contained in the isotopic abundances of cosmic rays, therefore, accurate evaluation of the isotopic production cross sections is of primary importance for Astrophysics of cosmic rays, studies of the galactic chemical evolution, and Cosmology. In this talk, I will show new results obtained with GALPROP, the most advanced numerical model for cosmic-ray propagation, which includes in a self-consistent way all cosmic-ray species (stable and long-lived radioactive isotopes from H to Ni, antiprotons, positrons and electrons, gamma rays and synchrotron radiation), and all relevant processes and reactions.

Moskalenko, Igor V.↗

NASA NTRS1985

The isotopic composition of cosmic ray chlorine

The isotopic composition of galactic cosmic ray chlorine (approx. = 225 MeV/amu) has been studied using the high energy cosmic ray experiment on the International Sun Earth Explorer 3 (ISEE-3) spacecraft. The abundances of 35C1 and 37C1 are found to be consistent with the secondary production expected from a propagation model developed to account for both light and subiron secondaries. An upper limit on the abundance of the radioactive isotope 36C1 (halflife approx. = 0.3 Myr) is used to set a lower limit on the confinement time of cosmic rays of approximately 1 Myr.

Wiedenbeck, M. E.↗

DOE OSTI2020

Management of Fissionable Equivalent Mass Materials at ORNL - 20146

The US DOE manages an inventory of materials that contains a range of long-lived radioactive isotopes that were produced from the 1960's through the 1980's by irradiating targets in production reactors to produce special heavy isotopes for US DOE programmatic use, scientific research, and industrial and medical applications. Since the production reactors and enrichment facilities that produced many of these materials have been shut down, they are considered unique materials that are not likely to be produced again. ORNL uses these materials in US DoE's center for production, storage, and distribution of TRU isotopes (plutonium through californium) and other related nuclear research programs. ORNL also operates the High Flux Isotope Reactor, which provides a high neutron source for production of isotopes for medical, industrial, and nuclear research programs. As a result, ORNL has an inventory of radioisotopes that are being managed for ongoing research programs and being held for reuse because they have potential intrinsic value to US DOE. An initiative is underway at ORNL to better manage these materials, particularly focusing on those with high fissionable equivalent mass that could impact the ability to perform ongoing or new research projects. This paper describes the actions ORNL is taking to manage these inventories, many of which consist of TRU materials, through reuse and disposal. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Test for Reconditioning RA Waste with Simulated Bitumen and Concrete in a 1,2 MW Plasma Test Facility - 20092

The operation and maintenance of nuclear power plants, the non nuclear fuel cycle, etc generate low-level radioactive waste which, along with the historical radioactive waste from past nuclear activities, needs to be treated and stored, awaiting final disposal. Plasma technology offers a very effective way of treating this waste with a high volume reduction factor (VRF), free from organics, liquids and moisture, and meets without a doubt the acceptance criteria for safe storage and disposal. By means of a plasma beam of approximately 5000 deg. C, the inorganic materials are melted into a glassy slag, containing most of the radioactive isotopes while the organic material is gasified, oxidized and purified in an off-gas cleaning system. First the paper describes the new full-scale Plasma Melting Facility (PMF) at the Kozloduy Nuclear Power Plant in Bulgaria which was taken in nuclear operation In May 2018. The plant has a capacity of 250 tons per year and the maximum contact dose rates of the incoming waste is 2 mSv/h. Different mixtures of radioactive waste packed in 200 l drums were successfully treated resulting in a glassy slag free from liquids and organic material with an important volume reduction factor (VRF). The Project was co-financed through a grant by Kozloduy International Decommissioning fund (KIDSF) administrated by the EBRD through Bulgarian national funding. Plasma is a suitable technology for treatment of problematic waste or even reconditioning waste so Belgoprocess was contracted to do plasma tests with simulated conditioned waste types. One can do tests on a laboratory scale on smaller samples and torch capacities of e.g. 50 kW but Belgoprocess wanted to do more realistic and reliable tests. So Belgoprocess contracted Phoenix Solutions Co who has a full-scope test facility equipped with a 1200 kW plasma torch for full-scope treatment of simulated conditioned waste. For a first confidential contract simulated 200 l (55 gallon) bitumen drums were treated. The drums contained different pucks of compacted waste such as rags, used filters, granulates, etc. The pucks were stacked in the 200 l drums and subsequently embedded with bitumen. A total of 6 drums were treated in the plasma facility. For a second contract simulated homogeneous 200 l (55 gallon) concrete drums with on the one hand concentrates and on the other hand spent resins were selected. A total of 6 drums with concrete and spent resins were treated and melted in the plasma testing facility. The paper describe the test facility, volume reduction factor (VRF) of different waste streams and most important parameters. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Investigating radioactive negative ion production via double electron capture

The relative cross sections for radioactive negative ion production via double electron capture have been measured for collisions between a 40 keV projectile beam of uranium-238 and potassium vapor. This was performed at the collinear resonance ionization spectroscopy (CRIS) experiment at CERN-ISOLDE and is a step towards measuring the electron affinities (EAs) of elements that cannot be efficiently produced in negative ion sources at radioactive ion beam (RIB) facilities. This includes short-lived radioactive isotopes that have low production quantities and heavy and superheavy elements that systematically have smaller EAs than work functions of available ion source materials. Negative ions are particularly sensitive to electron–electron correlation effects, which make such studies ideal for benchmarking atomic structure models that go beyond the independent particle model. While the EAs of most light elements have been measured, experimental investigations on heavier elements, namely the actinides, remain scarce due to their radioactive nature and production difficulty. By developing negative ion production by charge exchange, we aim to make these studies feasible at RIB facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗