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At least 343 records · Page 19

Discovering the nature of neutrinos: How nuclear theory will advance this grand endeavor. Final report

Why is there more matter than antimatter in the visible universe? Are neutrinos their own antiparticles? These are some of the most profound questions in science. The detection of a (0vββ) neutrinoless doublebeta decay and the measurement of its half-life is one of the most important experimental endeavors in science because it will answer these questions. Paramount to these measurements are accurate predictions with quantified uncertainties of the 0vββ-decay nuclear transitions, especially for the germanium-76 and xeon-136 nuclei, two candidate materials for building the next generation of DOE funded 0vββ-decay experiments. These predictions will guide the Office of Science’s down selection of experiments as well as aid in determining how much material is needed by these experiments. We studied a specific difficult to assess source of uncertainty that will impact coming microscopic predictions, uncertainty which arises from an incomplete yet systematically improvable model of interactions between nucleons and of nucleons with the other particles involved in decay process, referred to as the theory uncertainty. We employed a surrogate model of the germanium-76 nucleus, and its decay products, just detailed enough to adequately mimic the decaying nucleons need for a reasonable measure of this uncertainty and nothing more, avoiding the immense computational expense required in quantifying uncertainties of the full calculation. We found that microscopic calculations of this process can be expected to achieve relative theory uncertainties around 30%, including an unconstrained contribution that had the potential to spoil microscopic calculations. This results in a nearly order of magnitude on previously estimated uncertainties for this rare decay process.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Evaluation of a Combined Raffinate Waste Stream for Mo-99 Production

Niowave, Inc., based in Lansing, Michigan, intends to produce Mo-99 from the fission of low enriched uranium (LEU) targets. In FY20, SRNL was tasked to provide technical assistance in identifying the primary waste raffinate present in Niowave’s commercial scale system and evaluating methods for disposal. Due to limited information on Niowave’s complete flowsheet and isotope recovery plans, a combined raffinate stream including the entire radionuclide inventory from the irradiated fuel was used for this evaluation. Results of the evaluation indicated the majority of the waste generated can be expected to be Class A; however radioisotopes such as Pu-239, Cs-137, Sr-90, and some of the shorter lived (< 5 year half-life) may challenge Niowave’s ability to meet the waste acceptance criteria for land burial. With appropriate waste management strategies, it is probable that Niowave’s waste could meet Class C requirements for all constituents, with the possible exception of Pu-239. More detailed information of Niowave’s processes are needed to form a more accurate understanding required to execute and effective, economic, and feasible waste management strategy.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Understanding Materials Characteristics of Palladium Lanthanide Cermet Wires as a Mimic of Californium Wire Production

Californium-252 (Cf-252) has been synthesized on a large scale (mg) since the 1970s for use as a portable neutron source. With a half-life of 2.645 years and a spontaneous fission fraction of 3.09%, Cf-252 emits 2.31 × 10 12 neutrons/gram second. Today most of the Cf-252 produced in the world is made at Oak Ridge National Laboratory (ORNL) using the High Flux Isotope Reactor (HFIR) and the Radiochemical Engineering Development Center (REDC). Because of its highly radioactive nature, all manipulations of Cf-252 need to be performed in hot cell facilities by highly trained personnel. The Cf-252 produced at ORNL is done at the REDC, which is conveniently located next to the HFIR. Cf-252 is sold as bulk wire, which has been described as palladium (Pd) metal incasing californium oxide (Cf 2 O 3 ). The process was developed by Mosley et al. at Savannah River Laboratory (SRL) where it was modeled after the thorium work done by Fuschillo et al. This process has been used since the 1970s to synthesize this unique wire, but its fundamental chemistry and materials characteristics were never openly reported. Here we aim to better understand the chemistry and the materials characteristics of Cf-252 wire production for process improvements and to better our fundamental understanding of the mid-late actinides. Though there are many challenges in working with radioactive elements such as Cf, the isotope Cf-252 is even more complicated due to its neutron emission. One challenge with neutron emission is the ability of neutrons to penetrate much deeper through materials, causing radiation damage. This makes using instrumentation to characterize the chemistry and materials properties of this process difficult. For this reason, this study will first focus on terbium (Tb) as a surrogate for Cf. Currently Tb is used as a carrier or filler in Cf production when small amounts of Cf are being processed. This, along with their similar size and charge, makes Tb a reasonable surrogate for this study.

36 MATERIALS SCIENCE↗

Chemical Modeling of the Capture of Radioiodine Species

Iodine is a common fission product resulting from the transmutation of uranium fuel in nuclear power reactors. The short-lived radioactive isotope, 131 I, with a half-life of around eight days, would be a particular health concern if released into the environment. Capture materials, such as activated carbon, are used routinely in nuclear power plants and medical isotope production facilities to remove this hazard during normal operations to reduce emissions to acceptable levels. Iodine, unlike other common fission products such as noble gases, is challenging because of the wide range of molecular forms and oxidation states (from +VII in IF 7 to -I in iodide) that it displays, which can interconvert both in the gas phase and in the solution phase for example. The work in this project is focused on three computational tasks. In the first, we consider the binding of iodine-containing molecules of varying oxidation states to the major component of activated carbon – pristine graphene-like sheets. The second task focused on molecular binding and possible chemical transformations resulting from the reaction of molecular iodine with chemical functional groups on the edge of the graphene sheets or surface defects in the sheet itself. The final task was associated with radiolytic breakdown of 131 I to 131 Xe in iodine containing molecules and investigated the resulting molecular fragmentation process both in the gas phase and on the graphene-like surface. For each of the tasks, the intent was to learn about the thermodynamics and kinetics of the chemical transformations and use the calculations to provide parameters for input into kinetic models describing these processes for interpretation of experimental data in future work.

07 ISOTOPE AND RADIATION SOURCES↗

A Technical basis for in-house calibration of 252 Cf neutron source emission rates

10CFR835 stipulates that radiation protection instruments must be calibrated at least annually. Accordingly, calibration of dose rate instruments are reliant on well-known reference fields. The neutron-free-in-air facility (NFIA) located at TA36-0214 provides such a capability for neutron remmeters. One of the reference NFIA sources, 252 Cf, must be replaced every 8-10 years due to its relatively short half-life (2.645 ± 0.008 y). In the past, each newly purchased 252 Cf source has been calibrated at NIST using the Mn-bath technique prior to shipping to LANL. However, because of COVID-19 complications, the most recently acquired 252 Cf source (FTC-CF-7167) has been stored at LANL pending approval to ship to NIST for calibration. Due to the considerable expense in transporting the source to and from NIST, this TBD was written to demonstrate that new sources can be accurately calibrated via intercomparison measurements with older NIST-calibrated 252 Cf sources. It had been previously noted that such measurements yielded emission rates that agreed very well with the official rates established by NIST

252cf↗

Modeling Explosive Dispersal of Radiological Material: A Nonparametric Analysis

The National Atmospheric Release Advisory Center (NARAC) is a Department of Energy (DOE) asset that provides guidance on the potential effects of atmospherically released hazards based on dispersion simulation results. Numerical simulation results are compared to well-characterized experimental measurements whenever possible to validate and refine the model predictions. In 2012, such measurements were obtained by Defence Research and Development Canada (DRDC) and collaborating organizations for the case of explosively released 140 La – a radioactive isotope with a half-life of 1.6781 days.

42 ENGINEERING↗

Physical Sciences Vistas Issue 3 2021

In this issue, highlights of our contributions to mission operations include descriptions of the following. • How exact and scrupulous planning in concert with sophisticated science enabled a first-ever direct measurement of a radionuclide with a half-life as short as six days. The work, which included operations at the Los Alamos Neutron Science Centers (LANSCE) Weapons Neutron Research Facility and the Isotope Production Facility’s hot cell facility, is a boon for both astrophysics and weapons science. • An introduction to Christie Davis and her role in ensuring the Lab’s execution of simultaneous excellence. • A look at progress by AOT’s Target and Experimental Support Team in reclaiming long-dormant space in a radiological controlled area for new work improving target systems for the Lujan Center. • A story showcasing a cross-organizational effort to minimize the directorate’s legacy and environmental footprint. Staff from across the Lab joined together to ensure the safe and efficient disposal of Rocky Flats legacy waste stored in a transportainer at the Target Fabrication Facility. • How the Lab’s Utilities and Infrastructure experts collaborated with stakeholders in our directorate to safety execute preventive maintenance on the LANSCE mesa’s large electrical substation. The Safe Conduct of Research principles provided a common framework for the planning and process. • A description of the resources called upon and the procedures undertaken by MPA to inventory the division’s time-sensitive chemicals, including the careful and conscientious response of an alert team member when something seemed amiss.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

225 Ac/ 213 Bi Generator Based on Millifluidics Controlled Electrodeposition

Radioisotopes provide both diagnostic tools and therapeutic treatments for cancer and other diseases. In the US, millions of radioisotope doses are given to patients per year. Radiopharmaceutical generators are widely used to provide such short-lived medical radioisotopes in a clinical setting. These generators work by exploiting chemical differences in a parent/daughter isotope relationship. Actinium-225 (half-life 10 d) is used to provide clinically useful amounts of daughter isotopes 213 Bi (46 m). An integrated millifluidic 225 Ac/ 213 Bi radiopharmaceutical generator device was engineered to produce 213 Bi labeled biomolecules. Using recent LANL successes in additive manufacturing of small-scale fluidic devices, a disposable device was developed that integrates three steps for the production of 213 Bi labeled antibodies: 1) 213 Bi separation from 225 Ac parent, 2) 213 Bi antibody labeling, and 3) purification of the labelled antibody.

213Bi↗

Active Activation Diagnostics for High Energy X-ray and Neutron Measurements

Nuclear activation is a vital tool for diagnosing the properties of high-energy particles and photons. We investigate several potential reactions and suitable activation materials that could be used to simultaneously measure both neutrons and high-energy bremsstrahlung x-rays using one detector. Such a diagnostic would be valuable and practical for several facilities capable of creating such high-energy neutrons and x-rays. Laser-generated sources, such as NIF(-ARC) or Omega(-EP), have been shown to be capable of creating high-energy x-rays via high-intensity laser interactions and neutrons via DT fusion reactions. Furthermore, current laser technology is driving the demand for higher repetition rate diagnostics, hence we further constrain reaction/activation selections to accommodate high-repletion rate experiments. Our investigation will concentrate on identifying potential short half-life activation materials associated with high-energy x-ray reactions that could be incorporated into the existing realtime neutron activation detectors (RTNADs), an array of 48 activation detectors positioned around the NIF target chamber used to measure the DT neutron yield isotropy. We have identified two materials, gold and neodymium, that appear to be the best candidates to complement the RTNADs, by adding a new high-energy x-ray measurement capability.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Basic Radiation Theory and Protection [Slides]

Topics for this presentation include isotopes, alpha and beta radiation, x-rays and gamma-rays, neutrons, ionizing radiation, occupational exposure to radiation (CFR limit), radiation exposure amounts, the half-life, radiation protection, inverse square law (1/r 2 ), fission, fusion, and criticality.

61 RADIATION PROTECTION AND DOSIMETRY↗

Flow Measurements in Pressurized Helium Gas Cooling Channels

Production of metastable Technetium-99 (Tc-99m) is vital to the medical imaging community. It is a radioactive tracer that emits gamma rays as it decays and it is these gamma rays that are then detected through imaging. Tc-99m is extracted from the decay of Molybdenum-99 (Mo-99) which has a half-life of about 2-3 days. One method of generating Mo-99 is using accelerator based technology, through the irradiation of Mo-100 using an electron beam. This is part of the NNSA’s mission to produce Mo-99 commercially, within the US, without the use of highly enriched uranium (HEU) in support of nonproliferation and global security. Los Alamos National Laboratory (LANL) is working with NorthStar medical Radioisotopes (NMR) on their efforts to produce Mo-99 from the irradiation of Mo-100 targets. The NMR target consists of an Inconel window that allows the electron beam to penetrate and irradiate a stack of Mo-100 discs. The irradiation process generates large amounts of heat and requires extensive cooling of the Mo-100 targets and target housing using pressurized helium gas. Before beam on target, the design of the target stack and target housing is tested at LANL using laser based diagnostics experiments. We quantify the velocity field of the helium gas around the target housing to estimate whether the cooling provided is sufficient for the design and to validate computational fluid dynamics (CFD) models. Fiber optic imaging is also developed for use during cold testing (without beam on target) as well as during irradiation, to obtain real time information on disc performance.

07 ISOTOPE AND RADIATION SOURCES↗

Extended Modeling of DOE Sealed Canisters with Updated Chemistry Models

Road-ready and final disposition packaging configurations for the advanced test reactor (ATR) fuel currently specifies storage within helium backfilled DOE sealed standard canisters. The aluminum cladding of the ATR fuel contains an oxyhydroxide layer of boehmite/bayerite that generates hydrogen when subjected to irradiation. Understanding the effect of this hydrogen buildup over time to important for long term storage considerations. Previous modeling efforts have built a coupled CFD-chemical model to simulate the temperature gas phase concentrations within the DOE sealed standard canisters. These models have coupled the temperature conditions to both the gas phase radiolysis chemistry and the surface chemistry associated with the oxyhydroxide layer. The previous iteration of the model utilized constant G-values for the hydrogen generation a 50-year period. This new iteration of the model utilizes new experimental data to update the hydrogen generation rate, as well as increase the simulated time to a 200-year period. Given the half-life assumed for the primary Cs-137 isotope responsible for gamma radiation in the ATR spent fuel, the 200-year period decreases the decay heat and dose rate of the spent fuel by a factor of 100, which combined with the updated chemistry substantially decreases new hydrogen generation. Continued experimental work has identified trends for aluminum surrogate samples with oxyhydroxide layers for tests done at higher dose rates. At low initial doses a fast generation rate of hydrogen occurs which starts to roll over to a lower generation as the total dose applied increase. A small-scale chemical model was built to replicate as mini-canister surrogate system at SRNL as well as for the smaller capsule tests performed at INL. A variety of chemical models to capture this effect were tested, and a back reaction of H radical absorbing onto the surface, or inhibition of the reaction by significant H 2 cover gas were both able to fit both the mini-canister and the small capsule test data. Both kinetic fits were used to generate data from the new 200-year simulation. As additional experiments continue, the kinetic fits may be adjusted to adapt to new data. However, updated data shows that hydrogen atmosphere has little effect on actual generation data, so the model was reverted to use a star-stepped G-value for low-dose and high-dose regions. For the undried fuel case, the three models differ significantly with an end concentration of 1% for back reaction, 4.2% for inhibition, and 13.1% for constant G-value for the nominal scenario. For the dried fuel case, the nominal cases showed end concentrations of 0.23% for back reaction, 1.9% for inhibition, and 4.2% for const G-value for the nominal scenario. For the constant G-value case that is less conservative than the other two, the pressure for undried fuel increases to 1.94 atm over 200 years for the nominal case and 2.11 atm for the high decay heat case. The total hydrogen concentration after 200 years is 4.92% for the low decay heat case and 27.4% for the high decay heat case for undried fuel and is 1.4% and 9.6% for low and high decay heat fuel for the dried fuel case. If small amount of residual air is present, the potential for nitric acid formation of 595, 1568, and 2816 ppm for the lower, nominal, and upper fuel decay heat can occur. At long-term timeframes no significant shift in major species present occurs, so no appreciable amount of oxygen is present in the system. The continued rate of hydrogen generation in the canister occurs at an increase of 0.04% by mole over the final 10 years. Increasing the model range out to 1000 years continues to drop the hydrogen generation rate through decreasing dose rate.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Capture of Organic Iodides from Vessel Off-Gas Streams

In nuclear waste reprocessing, radioactive iodine is released in both organic and inorganic forms into off-gas streams. Due to its properties of long half-life and potential accumulation in human bodies, radioactive iodine is required to be removed from off-gas streams by the Environmental Protection Agency (EPA) and Nuclear Regulatory Commission (NRC). In this study, the removal of organic iodides using two prototype silver (Ag) adsorbents, i.e., reduced Ag functionalized silica aerogel (Ag 0 -aerogel) and reduced Ag exchanged mordenite (Ag 0 Z), is investigated through a combination of experimental and modeling studies.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Enhancing Radionuclide Production Capabilities at the Duke University Medical Center Cyclotron with a Focus on Astatine-211

Radionuclides play an important role in a diverse array of fields including physics, chemistry, agriculture, materials science, national security, medical research and patient care. Establishing a reliable domestic supply of key radionuclides is critical to our national competitiveness in these areas. Regarding medical applications, targeted alpha-particle therapy (TAT) has become of great interest to basic researchers and clinicians alike and is emerging as a valuable and cost-effective approach for cancer treatment. Unfortunately, progress in TAT, particularly with regard to its clinical translation, has been severely hampered by the limited availability of the most promising radionuclides at a reasonable cost, and with appropriate chemical and radiochemical purity. In this project, we have attempted to address this problem by focusing on production of the 7.2-h half-life α-particle emitter, 211 At, which has long been considered to be one of the most promising radionuclides for TAT. We note that he critical importance of improving the supply of 211 At in the United States was noted in the Funding Opportunity Announcement related to this project. At Duke University, we have a CS-30 cyclotron that is one of the few accelerators in the United States that has an alpha-particle beam that has enough energy to make useful quantities of 211 At. With this cyclotron, we have been able to produce more 211 At than anywhere else in the world because of our unique internal cyclotron target system. However, the CS-30 cyclotron is nearly 40 years old and was no longer reliable. In addition, its operation required considerable skill, largely because it had analog control systems, and vital parts including old-fashioned power supplies, were becoming unavailable. For these reasons, the current project was undertaken to evaluate all the subsystems of the CS-30 cyclotron and replace, repair, and update them. With help from our consultant, Ionetix, this has now been accomplished. We believe that because of this work, the CS-30 can reliably supply 211 At for basic research and clinical trials both at Duke and beyond.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

A Fission-like Neutron Spectrum Shaping Assembly based on D-T Generator

For nearly five decades, 252 Cf sources have been used for testing and calibration over a wide range of neutron detection devices used for nuclear safety and radiation protection. However, the vastly increased cost of 252 Cf sources, its short half-life, and concerns about future shortage have prompted nuclear facilities and radiological calibration laboratories that rely on high-intensity neutron sources to seek alternatives. While there appear to be no other radionuclide neutron sources that would match the 252 Cf performance characteristics, all of them, including 252 Cf, present similar concerns in terms of hazards, safety, and security. As a possible solution to this issue, the Pacific Northwest National Laboratory (PNNL) developed a low-risk, cost-efficient alternative to produce fission-like spectra based on commercially available deuterium-tritium (D-T) neutron generators. The alternative of producing a fission-like neutron spectrum without any fissionable materials or beryllium would enable the nuclear facilities across the entire complex to eliminate their reliance on high intensity 252 Cf sources for nuclear safety and radiation protection applications, substantially reducing risks and associated costs. This report describes efforts of designing the spectrum shaping assembly, its construction and characterization of the neutron field produced. Performance of this newly developed D-T generator based neutron field is demonstrated via calibration of a criticality detector, neutron survey instruments, and personal dosimeters verified against current standardized fields produced by 252 Cf spontaneous fission sources.

42 ENGINEERING↗

β- and γ-Counting for Pre-detonation Nuclear Forensics on Eu-155

Post-detonation nuclear forensics was performed at Los Alamos National Laboratory (LANL) on 155Eu, a fission product on the wing of the fission product production curve whose yield is sensitive to fission fuel and neutron energy. With a half-life of 4.753 years, 155Eu provides a longer-lived option for these measurements than other fission products with similar mass numbers. The Chemistry Division Group - Nuclear and Radiochemistry, at LANL routinely measures a suite of fission products from 235U fissions in thermal neutron flux experiments known as thermal calibration exercises, using a mixture of gas proportional β-decay counting and γ-spectrometry on HPGe detectors. The fission products of interest are reported relative to a high-yield reference fission product from the same sample to create a running average ratio specific to neutron energy and fuel type; Equation 1 below shows the ratio-of-ratios R-value measured fission products are reported in: R i x = [A( i X)/A( 99 Mo)] unknown [A( i X)/A( 99 Mo)] 235 U n,th where A denotes activity, i X is the nuclide of interest, and 235 U n,th denotes irradiations of 235 U with thermal neutrons. Measurements of unknown fission spectra are ratioed to a running-average of thermal calibration results, and the resulting R-value can be referred to as against a library of irradiation conditions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The Wavelength Shifting Plate on the LEGEND Experiment

Majorana-type neutrinos lead to a neutrinoless double beta decay with the emission of only two electrons. (Lepton Number Violation). LEGEND experiment is proposed to search for this transition from ⁷⁶Ge to ⁷⁶Se. The goal is to reach the half-life sensitivity of about 10²⁸ years in a 5 kton٠year exposure of a detector with 1 ton of isotopic ⁷⁶Ge mass.

Bae, Wonseok↗

Flow Induced Vibration Studies in Pressurized Helium Gas Cooling Channels

Production of metastable Technetium-99 (Tc-99m), a radioactive tracer that emits gamma rays, is vital to the medical imaging community. Tc-99m is extracted from the decay of Molybdenum-99 (Mo-99) which has a half-life of about 2-3 days. The work presented in this report is part of the NNSA’s mission to produce Mo-99 commercially, within the US, without the use of highly enriched uranium (HEU) in support of nonproliferation and global security. Los Alamos National Laboratory (LANL) is working with NorthStar Medical Radioisotopes (NMR) on their efforts to produce Mo-99 through the irradiation of Mo-100 targets using an electron beam. The NMR target comprises a stack of approximately 60-70 Mo-100 disks with diameter 24 mm and thickness 0.74 mm held in stainless steel laminations, each separated using 0.25 mm thick stainless steel spacers. The symmetric target stack is housed in an Inconel vessel with two Inconel windows on either side. Two electron accelerators are used to produce 40 MeV, 3.16 µA electron beams each that penetrate the Inconel windows and irradiate the Mo-100 disks. Approximately 90% of the total 250 kW beam power is deposited in the NMR target during the irradiation process. During irradiation, pressurized helium gas flows through 0.25 mm thin gaps between the disks cooling the beam window, target disks, disk laminations and spacers. Both NMR and LANL have found during cold testing of the target system (no heat deposition) that the Mo-100 disks undergo significant mass loss and disk breakage due to vibrations induced by the flowing helium gas. The mass loss is not only undesirable due to monetary loss from reduced final quantities of Mo-99, but also due to the hazards associated with radioactive material trapped in the cooling lines and particle filters. The effect of flow rate and target geometry on the flow induced vibrations need to be quantified, and recommendations provided to minimize this mass loss. This work describes LANL’s experimental characterization of the flow induced vibrations and disk mass loss in a reduced scale set-up containing 10 Mo-100 disks. We use high speed imaging, displacement measurements and microphone measurements combined with signal processing to estimate the vibration frequency of each disk. The effect of disk thickness, target fit and duration of testing on the mass loss is described. We find that in the current configuration of NMR targets, the vibrations and mass loss on the first disk are minimized, while those in the adjacent disks are highest. The microphone and high-speed image data show that increased flow rates and increased duration of testing increases vibration frequency and mass loss. The mass loss is due to both disk rotation and back and forth motion. There are visible wear marks on the disks with the highest mass loss. We also note that the current NMR window gap reduces flow induced vibrations compared to the previous smaller gaps. Longer duration testing will provide more data and verification for the findings presented in this report. The work will be continued in FY 24.

43 PARTICLE ACCELERATORS↗