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R and D of crystal scintillators from enriched isotopes for high sensitivity double β decay experiments

Experiments to search for neutrinoless double beta decay enters to a new phase when a sensitivity on the level of T{sub 1/2}∼10{sup 26}−10{sup 28} yr is required. Scintillating low temperature detectors possess important properties required for high-sensitivity double beta decay experiments: presence of elements of interest, high energy resolution and detection efficiency, low level of background thanks to excellent particle discrimination ability. High concentration of isotope of interest and as low as possible radioactive contamination are important requirements to crystal scintillators. Other crucial issues are maximal output of detectors and minimal loss of enriched materials. Prospects of several scintillation materials, enriched in isotopes promising for double beta decay experiments, are discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Application of Generic Disposal System Models

This report describes specific GDSA activities in fiscal year 2015 (FY2015) toward the development of the enhanced disposal system modeling and analysis capability for geologic disposal of nuclear waste. The GDSA framework employs the PFLOTRAN thermal-hydrologic-chemical multi-physics code (Hammond et al., 2011) and the Dakota uncertainty sampling and propagation code (Adams et al., 2013). Each code is designed for massively-parallel processing in a high-performance computing (HPC) environment. Multi-physics representations in PFLOTRAN are used to simulate various coupled processes including heat flow, fluid flow, waste dissolution, radionuclide release, radionuclide decay and ingrowth, precipitation and dissolution of secondary phases, and radionuclide transport through the engineered barriers and natural geologic barriers to a well location in an overlying or underlying aquifer. Dakota is used to generate sets of representative realizations and to analyze parameter sensitivity.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

β -delayed neutron emission from Ga 85

Here, decay of 85 Ga was studied by means of β-neutron-γ spectroscopy. A pure beam of 85 Ga was produced at the Holifield Radioactive Ion Beam Facility using a resonance ionization laser ion source and a high-resolution electromagnetic separator. The β-delayed neutron emission probability was measured for the first time, yielding 70(5)%. An upper limit of 0.1% for β-delayed two-neutron emission was also experimentally established for the first time. A detailed decay scheme including absolute γ-ray intensities was obtained. Lastly, results are compared with theoretical β-delayed emission models.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Decontamination and Decommissioning Program of a Radiopharmaceuticals Production Facility - 17103

On May 2012, Best Medical Belgium (BMB) S.A., a manufacturer of pharmaceutical products located on the nuclear site of Fleurus, was declared bankrupt. According to the Belgian law, ONDRAF/NIRAS (Belgian Radioactive Waste Management Agency) was entrusted with the clean-up and the decommissioning operations of the former BMB facilities, nowadays known as 'ONDRAF/NIRAS Site Fleurus' (ONSF). In June 2015, ONSF launched a Decontamination and Decommissioning (D and D) program, for which Tractebel supports the definition of the clean-up and decommissioning strategies; the drafting of the Final Decommissioning Plan (FDP) and License Application for decommissioning; and the follow-up of the clean-up and upcoming D and D works on site. Four nuclear buildings are part of the clean-up and D and D activities. One of them, Building 14 (B14), represents the most challenging task with the clean-up of highly contaminated areas and their further decommissioning up to greenfield. Beside its two cyclotrons successively used for the production of radioisotopes, this building features hot cells and glove boxes used for the purification of radioisotopes and the conditioning of the final pharmaceutical product. The present paper aims at presenting the development of the D and D program in terms of modifications of existing facilities to allow carrying out the clean-up and D and D activities and the management of dismantled radioactive materials in a safe, efficient and cost-effective way as well as in terms of strategic options to be developed for the FDP. To support the clean-up and D and D activities, several workshops have been designed in order to treat radioactive materials removed from the building rooms. Those workshops feature an input buffer storage area, a common output buffer storage area and installations for the treatment of radioactive materials and waste (handling devices, cutting means, decontamination means, free release measurements means, etc.). Some modifications to the existing auxiliary systems will be required in order to dispose of appropriate systems to operate those workshops in a safe way. Activated concrete structures will constitute the most important part of radioactive materials that will arise from the decommissioning activities. To limit the total decommissioning costs, and especially the costs associated to radioactive waste management, two strategies have been developed in order to manage a part of activated concrete as candidate for free release with a certain decay period or as candidate for conventional landfill. Both strategies will have to be further detailed and discussed with the competent Authorities to ensure they can actually be implemented. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Exploration for astromers near 132 Sn with the Canadian Penning Trap

Nuclear isomers can have significant impacts on astrophysical nucleosynthesis processes, with recent efforts demonstrating that the population of isomeric states with different half-lives may require separate treatment in reaction networks to accurately capture the differences in heating or in identifiable electromagnetic signals. Several potential so-called “astromers” in tin and antimony isotopes near doubly magic 132 Sn were identified and direct mass measurements of their ground and isomeric states were performed with the Canadian Penning Trap at Argonne National Laboratory's CARIBU facility, and their impact on astrophysical reaction rates and in reaction networks was calculated. Finally, it was found that 129⁢𝑔,𝑚 Sn , with measured mass excesses of −80593.2⁢(25) and −80557.4⁢(25) keV, respectively, and an excitation energy of 35.8(35) keV, behaves as an astromer during neutron capture in the 𝑖-process and in the 𝑟-process.

isomer decays↗

Precision Measurement of Electron Antineutrino Disappearance in the Daya Bay Experiment

The Daya Bay reactor neutrino experiment studies the disappearance of electron antineutrinos from reactor cores at the Daya Bay Power Plant located in China. Daya Bay has made a precision measurement of one of the parameters describing the quantum mechanical mixing between neutrino flavor states and mass states, the mixing angle $\theta_{13}$. One source of systematic uncertainty in the measurement is due to background induced by cosmic ray muons. The detectors are located underground to minimize the cosmic flux, but the residual backgrounds must be measured. This program will focus on the study and measurement of the cosmic muon-induced backgrounds at Daya Bay with a goal of achieving the lowest possible level of background-related systematics on the disappearance measurement. In addition to providing crucial input to the Daya Bay disappearance analysis, measurements of the muon flux and the production of neutrons and radioactive nuclei by cosmic muons will be of general interest to other underground experiments such as double beta decay and dark matter searches.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Production of highly-enriched 134Ba for a reference material for isotope dilution mass spectrometry measurements

Isotope dilution mass spectrometry (IDMS) is an analytical technique capable of providing accurate and precise quantitation of trace isotope abundance and assay providing measurement uncertainties below 1 %. To achieve these low uncertainties, the IDMS method ideally utilizes chemically pure “spike” solutions that consist of a single highly enriched isotope that is well-characterized relating to the abundance of companion isotopes and concentration in solution. To address a current demand for accurate 137Cs/137Ba ratio measurements for “age” determination of radioactive 137Cs sources, Idaho National Laboratory (INL) is producing enriched 134Ba isotopes that are tobe used for IDMS spikes to accurately determine 137Ba accumulation from the decay of 137Cs. The final objective of this work it to provide a homogenous set of reference materials that the National Institute of Standards and Technology can certify as standard reference materials used for IDMS. The process that was developed at INL for the separation and isolation of Ba isotopes, chemical purification of the isotopes in solution, and the encapsulation of the materials will be described.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Stability of {sup 248–254}Cf isotopes against alpha and cluster radioactivity

Stability of {sup 248–254}Cf nuclei against alpha and cluster emissions is studied within our Coulomb and proximity potential model (CPPM). It is found that these nuclei are stable against light clusters (except alpha particles) and unstable against heavy cluster (A{sub 2}≥40) emissions. For heavy cluster emissions the daughter nuclei lead to doubly magic {sup 208}Pb or the neighbouring one. The effects of quadrupole and hexadecapole deformations of parent nuclei, daughter nuclei and emitted cluster on half lives are also studied. The computed alpha decay half life values (including quadrupole deformation β{sub 2}) are in close agreement with experimental data. Inclusion of quadrupole deformation reduces the height and width of the barrier (increases the barrier penetrability) and hence half life decreases. -- Highlights: •{sup 248–254}Cf parents are stable against light clusters (except alpha particles) and are unstable against heavy clusters ({sup 46}Ar, {sup 48,50}Ca etc.). •For the case of heavy cluster emissions the daughter nuclei are doubly magic {sup 208}Pb or neighbouring one. •The alpha decay half lives are in agreement with experimental data. •The cluster decay half lives decrease with the inclusion of quadrupole deformation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Observation of a γ -decaying millisecond isomeric state in 128 Cd 80

A new high-spin isomer in the neutron-rich nucleus 128 Cd was populated in the projectile fission of a 238 U beam at the Radioactive Isotope Beam Factory at RIKEN. A half-life of T1/2 = 6.3(8) ms was measured for the new state which was tentatively assigned a spin/parity of (15-). The experimental results are compared to shell model calculations performed using state-of-the-art realistic effective interactions and to the neighbouring nucleus 129 Cd. In the present experiment no evidence was found for the decay of a 18 + E6 spin-trap isomer, based on the complete alignment of the two-neutron and two-proton holes in the 0h 11/2 and the 0g 9/2 orbit, respectively, which is predicted to exist by the shell model.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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↗

Window Cooling Studies and Disk Vibration Testing on a Subset of Mo-100 Disks

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, with a smaller percentage adding up to 2.2 kW of heat deposited on the Inconel window. During irradiation, pressurized helium gas flows through 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. LANL has previously also tested NMR’s Inconel beam window by heating the window, while flowing pressurized helium, using the average heat deposited on the window. However, the NMR beam is pulsed with a duty cycle of 12.5%, which introduces oscillation in temperature around the nominal 600 °C steady state value with each pulse. Available fatigue curves for Inconel are few, established for room temperature, and they are based on mechanical strain cycles not thermally induced strain as in the NMR target. The effect of pulsed beam heating on the Inconel window therefore needs to be quantified. This report details the experiments conducted to assess the factors that lead to mass loss in the NMR target disks as well as to understand the effect of a pulsed beam on NMR’s Inconel window. This work describes LANL’s experimental characterization of the flow induced vibrations and disk mass loss in a reduced scale set-up containing 5 to 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. Improved target holders significantly reduce disk mass loss to almost negligible quantities. This work finds that the larger window to first disk gap and improved target holder geometry should allow NMR to successfully conduct irradiations with minimal mass loss. The window tests were conducted to understand the effect of a pulsed beam on both the window longevity and to estimate the window temperature and displacement during pulsing. The experiments presented here were performed at significantly low power, due to the limitations of the induction heating system. The window temperature rose to approximately 73 °C with a significantly reduced power of 45 W without beam pulsing. With a 5 Hz pulse rate, 12.5% duty cycle, the window temperature remained constant at 26 °C. These experiments will be repeated with improved coil geometry and reported in upcoming journal papers.

42 ENGINEERING↗

New transitions and levels for 163 Tb obtained from β-decay studies

Transitions in 163 Tb following β decay of 163 Gd were obtained as part of investigations of γ rays emitted following 163 Euβ decay to 163 Gd. In this work, detailed analysis of the low-energy structure of 163 Tb has been carried out with these data to expand previous β-decay studies and reactions studies of levels in 163 Tb. Data were collected at the LeRIBSS station of the Holifield Radioactive Ion Beam Facility at Oak Ridge National Laboratory with an array of four Clover HPGe detectors for γ rays and two plastic scintillators for β detection. The γ rays were identified as belonging to 163 Gd and 163 Tb via mass selection and γ-γ-β, γ-γ, or γ-x-ray coincidence. In total, 38 new γ-ray transitions were observed in 163 Tb from 15 newly identified levels and 12 previously identified levels. Potential energy surface calculations were performed which support a rigid prolate deformation. Previously identified unplaced transitions in 163 Tb have been placed within the level scheme of 163 Tb and additional states and transitions have been identified.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Properties of γ-decaying isomers in the 100 Sn region populated in fragmentation of a 124 Xe beam

A systematic study was performed of microsecond γ-decaying isomers around 100 Sn produced in a fragmentation reaction of a 124 Xe beam at 345 MeV/u at the Radioactive Ion Beam Factory of the RIKEN Nishina Center in Saitama, Japan. Half-lives of isomeric states in that region were remeasured allowing us to improve the currently available experimental information. Reduced transition probabilities were deduced and compared to shell-model calculations in various model spaces. Furthermore, the recently reported low-energy transitions in 92 Rh and 96 Ag were remeasured with improved precision. Additionally, experimental information on isomeric ratios, including five new ones, were extracted and compared to a previous experimental study and the sharp cutoff model of fragmentation reaction.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Decommissioning for the containment vessel of HTR-PM: Monte Carlo simulation and long-time predictions

A high temperature gas cooled reactor-pebble bed module (HTR-PM) is currently under design and construction in China. Calculations of induced radioactivity in the concrete containment vessel of HTR-PM were performed in order to predict the decommissioning problems. The main activation products and the ambient dose equivalent rate corresponding to 40 years of operations followed by 30 days/1 year/10 years of decay, were calculated by using the Monte Carlo particle transport code FLUKA. Finally, according to the Chinese National Standard and on the basis of the knowledge gained from this study, the classifications of the radioactive solid wastes were discussed, and some suggestions for the working duration of the employees were given. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Chromatographic separation of radioactive noble gases from xenon

The Large Underground Xenon (LUX) experiment operates at the Sanford Underground Research Facility to detect nuclear recoils from the hypothetical Weakly Interacting Massive Particles (WIMPs) on a liquid xenon target. Liquid xenon typically contains trace amounts of the noble radioactive isotopes 85 Kr and 39 Ar that are not removed by the in situ gas purification system. The decays of these isotopes at concentrations typical of research-grade xenon would be a dominant background for a WIMP search exmperiment. To remove these impurities from the liquid xenon, a chromatographic separation system based on adsorption on activated charcoal was built. 400 kg of xenon was processed, reducing the average concentration of krypton from 130 ppb to 3.5 ppt as measured by a cold-trap assisted mass spectroscopy system. Finally, a 50 kg batch spiked to 0.001 g/g of krypton was processed twice and reduced to an upper limit of 0.2 ppt.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Bayesian uncertainty quantification of tristructural isotropic particle fuel silver release: Decomposing model inadequacy plus experimental noise and parametric uncertainties

Tristructural isotropic (TRISO) particle fuel is one of the most promising fuel concepts enabling high temperature and high burnup reactor operation. One dominant source of radioactivity released from the TRISO particles is silver (Ag), which is subject to a high release fraction and long decay life compared to other fission products. Previous modeling efforts using the fuel performance code BISON indicated nonnegligible uncertainties in modeling the diffusion process of fission products in TRISO compared to the Advanced Gas Reactor experiments. The overall uncertainties observed when modeling the fission product diffusion can result from uncertainties in model parameters, noisy experimental measurements, and deficiencies in the developed models. The three types of underlying uncertainties have not yet been properly quantified in open literature. Here, this paper presents the Bayesian uncertainty quantification (UQ) using massively parallelizable Markov chain Monte Carlo samplers. The uncertainties due to model parameters, model inadequacy, and experimental measurement noise are quantified, with the σ term used to represent the sum of the model inadequacy and measurement noise uncertainties. It is worth noting that this is the first time the σ term is inferred for nuclear fuel experiments, as compared to using prescribed values for uncertainty quantification in previous work. The parallelizable Markov chain Monte Carlo samplers efficiently infer the model parameters and the σ term, giving insight into physical parameters like diffusion coefficients and the combined model discrepancy and measurement noise. A subsequent forward uncertainty quantification (UQ) is also performed based on the calibration results to generate more accurate predictions of the Ag release. The model inadequacy plus experimental noise is the most dominant source of uncertainty compared to the parametric uncertainty. All the UQ analyses presented in this work are based on the second series of the irradiation experiments in the Advanced Gas Reactor program.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Measurement of neutron dose equivalent outside and inside of the treatment vault of GRID therapy

Purpose: To evaluate the neutron and photon dose equivalent rates at the treatment vault entrance (H{sub n,D} and H{sub G}), and to study the secondary radiation to the patient in GRID therapy. The radiation activation on the grid was studied.Methods: A Varian Clinac 23EX accelerator was working at 18 MV mode with a grid manufactured by .decimal, Inc. The H{sub n,D} and H{sub G} were measured using an Andersson–Braun neutron REM meter, and a Geiger Müller counter. The radiation activation on the grid was measured after the irradiation with an ion chamber γ-ray survey meter. The secondary radiation dose equivalent to patient was evaluated by etched track detectors and OSL detectors on a RANDO{sup ®} phantom.Results: Within the measurement uncertainty, there is no significant difference between the H{sub n,D} and H{sub G} with and without a grid. However, the neutron dose equivalent to the patient with the grid is, on average, 35.3% lower than that without the grid when using the same field size and the same amount of monitor unit. The photon dose equivalent to the patient with the grid is, on average, 44.9% lower. The measured average half-life of the radiation activation in the grid is 12.0 (±0.9) min. The activation can be categorized into a fast decay component and a slow decay component with half-lives of 3.4 (±1.6) min and 15.3 (±4.0) min, respectively. There was no detectable radioactive contamination found on the surface of the grid through a wipe test.Conclusions: This work indicates that there is no significant change of the H{sub n,D} and H{sub G} in GRID therapy, compared with a conventional external beam therapy. However, the neutron and scattered photon dose equivalent to the patient decrease dramatically with the grid and can be clinical irrelevant. Meanwhile, the users of a grid should be aware of the possible high dose to the radiation worker from the radiation activation on the surface of the grid. A delay in handling the grid after the beam delivery is suggested.

61 RADIATION PROTECTION AND DOSIMETRY↗

Automation of experiments at Dubna Gas-Filled Recoil Separator

Approaches to solving the problems of automation of basic processes in long-term experiments in heavy ion beams of the Dubna Gas-Filled Recoil Separator (DGFRS) facility are considered. Approaches in the field of spectrometry, both of rare α decays of superheavy nuclei and those for constructing monitoring systems to provide accident-free experiment running with highly radioactive targets and recording basic parameters of experiment, are described. The specific features of Double Side Silicon Strip Detectors (DSSSDs) are considered, special attention is paid to the role of boundary effects of neighboring p–n transitions in the “active correlations” method. An example of an off–beam experiment attempting to observe Zeno effect is briefly considered. Basic examples for nuclear reactions of complete fusion at {sup 48}Ca ion beams of U-400 cyclotron (LNR, JINR) are given. A scenario of development of the “active correlations” method for the case of very high intensity beams of heavy ions at promising accelerators of LNR, JINR, is presented.

43 PARTICLE ACCELERATORS↗