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At least 775 records · Page 43

Study of radon concentration in wetland Mediterranean water using continuous monitoring - 25416

Radon is a radioactive gas that comes from the uranium and radium decay. It is considered the second cause of lung cancer in nonsmokers by the World Health Organization (WHO). Most studies focus on radon levels in air, which comes mainly from soil. Unfortunately, just some of them focus on radon in water which exposure is mainly due to radon inhalation when it is exhaled from water. In order to develop a methodology for radon measurement in water, this work compares two different techniques. The measurements have been done at Peniscola marsh, a location in the Valencian Community where significant radon concentrations have been measured in previous works. Furthermore, measurements in the Waste-Water-Treatment Plant (WWTP) near the marsh, where high radon concentrations have been found in air, are analyzed to confirm if they can be related to radon presence in water. (authors)

54 ENVIRONMENTAL SCIENCES↗

Buffer Material Degradation in High Level Radioactive Waste Disposal - 18454

The concept of geological disposal for high-level radioactive waste (HLW) is based on a multi-barrier system comprising the natural geological barrier that repository host rock provides and its surroundings, as well as an engineered barrier system (EBS) that includes waste form, waste canisters, buffer materials, and backfill. The multi-barrier system is expected to perform its desired functions to isolate waste from the biosphere and achieve HLW disposal. Because of the interaction processes of radionuclide decay heat with hydraulic and water-mineral reactions in the radioactive waste repository, the bentonite buffer degradation resulting from the external temperature and pressure warrants investigation. However, seldom addressed in Taiwan is the influence of thermo-hydro-chemical (T-H-C) processes on buffer material degradation in the EBS of HLW disposal repositories as related to smectite clay dehydration. Therefore, we adopted the chemical kinetic model of smectite dehydration to calculate the amount of water expelled from smectite clay minerals caused by higher temperatures of waste decay heat. We discovered that smectite clay could cause volume shrinkage because of a loss of interlayer water, which can lead to bentonite buffer compression. The results of this study may be used in advanced research on the evolution of bentonite degradation for both performance assessments and safety analyses of final HLW disposal in Taiwan. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

SUPERNOVA NEUTRINO NUCLEOSYNTHESIS OF THE RADIOACTIVE {sup 92}Nb OBSERVED IN PRIMITIVE METEORITES

The isotope {sup 92}Nb decays to {sup 92}Zr with a half-life of 3.47 × 10{sup 7} yr. Although this isotope does not exist in the current solar system, initial abundance ratios for {sup 92}Nb/{sup 93}Nb at the time of solar system formation have been measured in primitive meteorites. The astrophysical origin of this material, however, has remained unknown. In this Letter, we present new calculations which demonstrate a novel origin for {sup 92}Nb via neutrino-induced reactions in core-collapse supernovae (ν-process). Our calculated result shows that the observed ratio of {sup 92}Nb/{sup 93}Nb ∼ 10{sup –5} can be explained by the ν-process.

79 ASTRONOMY AND ASTROPHYSICS↗

Microstructural Effects of High Dose Helium Implantation in ErD 2

Metal hydrides can store hydrogen isotopes with high volumetric density. In metal tritides, tritium beta decay can result in accumulation of helium within the solid, in some cases exceeding 10 at.% helium after only 4 years of aging. Helium is insoluble in most materials, but often does not readily escape, and instead coalesces to form nanoscale bubbles when helium concentrations are near 1 at.%. Blistering or spallation often occurs at higher concentrations. Radioactive particles shed during this process present a potential safety hazard. This study investigates the effects of high helium concentrations on erbium deuteride (ErD 2 ), a non-radioactive surrogate material for erbium tritide (ErT 2 ). To simulate tritium decay in the surrogate, high doses of 120 keV helium ions were implanted into ErD 2 films at room temperature. Scanning and transmission electron microscopy indicated spherical helium bubble formation at a critical concentration of 1.5 at.% and bubble linkage leading to nanoscale crack formation at a concentration of 7.5 at.%. Additionally, crack propagation occurred through the nanocrack region, resulting in spallation extending from the implantation peak to the surface. Electron energy loss spectroscopy was utilized to confirm the presence of high-pressure helium in the nanocracks, suggesting that helium gas plays a predominant role in deformation. This work improves the overall understanding of helium behavior in ErD 2 by using modern characterization techniques to determine: the critical helium concentration required for bubble formation, the material failure mechanism at high concentration, and the nanoscale mechanisms responsible for material failure in helium implanted ErD 2 .

36 MATERIALS SCIENCE↗

Development of bimetallic (Zn@Au) nanoparticles as potential PET-imageable radiosensitizers

Purpose: Gold nanoparticles (GNPs) are being investigated actively for various applications in cancer diagnosis and therapy. As an effort to improve the imaging of GNPs in vivo, the authors developed bimetallic hybrid Zn@Au NPs with zinc cores and gold shells, aiming to render them in vivo visibility through positron emission tomography (PET) after the proton activation of the zinc core as well as capability to induce radiosensitization through the secondary electrons produced from the gold shell when irradiated by various radiation sources. Methods: Nearly spherical zinc NPs (∼5-nm diameter) were synthesized and then coated with a ∼4.25-nm gold layer to make Zn@Au NPs (∼13.5-nm total diameter). 28.6 mg of these Zn@Au NPs was deposited (∼100 μm thick) on a thin cellulose target and placed in an aluminum target holder and subsequently irradiated with 14.15-MeV protons from a GE PETtrace cyclotron with 5-μA current for 5 min. After irradiation, the cellulose matrix with the NPs was placed in a dose calibrator to assess the induced radioactivity. The same procedure was repeated with 8-MeV protons. Gamma ray spectroscopy using an high-purity germanium detector was conducted on a very small fraction (<1 mg) of the irradiated NPs for each proton energy. In addition to experimental measurements, Monte Carlo simulations were also performed with radioactive Zn@Au NPs and solid GNPs of the same size irradiated with 160-MeV protons and 250-kVp x-rays. Results: The authors measured 168 μCi of activity 32 min after the end of bombardment for the 14.15-MeV proton energy sample using the {sup 66}Ga setting on a dose calibrator; activity decreased to 2 μCi over a 24-h period. For the 8-MeV proton energy sample, PET imaging was additionally performed for 5 min after a 12-h delay. A 12-h gamma ray spectrum showed strong peaks at 511 keV (2.05 × 10{sup 6} counts) with several other peaks of smaller magnitude for each proton energy sample. PET imaging showed strong PET signals from mostly decaying {sup 66}Ga. The Monte Carlo results showed that radioactive Zn@Au NPs and solid GNPs provided similar characteristics in terms of their secondary electron spectra when irradiated. Conclusions: The Zn@Au NPs developed in this investigation have the potential to be used as PET-imageable radiosensitizers for radiotherapy applications as well as PET tracers for molecular imaging applications.

60 APPLIED LIFE SCIENCES↗

Advances in Geologic Disposal System Modeling and Application to Crystalline Rock

The Used Fuel Disposition Campaign (UFDC) of the U.S. Department of Energy (DOE) Office of Nuclear Energy (NE), Office of Fuel Cycle Technology (OFCT) is conducting research and development (R&D) on geologic disposal of used nuclear fuel (UNF) and high-level nuclear waste (HLW). Two of the high priorities for UFDC disposal R&D are design concept development and disposal system modeling (DOE 2011). These priorities are directly addressed in the UFDC Generic Disposal Systems Analysis (GDSA) work package, which is charged with developing a disposal system modeling and analysis capability for evaluating disposal system performance for nuclear waste in geologic media (e.g., salt, granite, clay, and deep borehole disposal). This report describes specific GDSA activities in fiscal year 2016 (FY 2016) 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 and the Dakota uncertainty sampling and propagation code. 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 engineered barriers and natural geologic barriers to the biosphere. Dakota is used to generate sets of representative realizations and to analyze parameter sensitivity.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The LSU-Argonne conversion electron spectrometer: A new detector for the X-Array and SATURN decay station

In this study, a new conversion electron detector has been commissioned at the ATLAS/ CARIBU facility at Argonne National Laboratory. The LSU-Argonne Conversion Electron Spectrometer (LACES) is a LN 2 -cooled Si(Li) detector system designed to be incorporated into a decay station that comprises the dedicated HPGe clover array with a box geometry (X -Array) and the Scintillator and Tape Using Radioactive Nuclei (SATURN) device. This integration enables simultaneous measurements of conversion electrons and gamma-rays in decay experiments, yielding novel information on transition multipolarities, electric monopole transitions, and isomeric states that decay mostly via conversion electrons. A measurement of the energy resolution of LACES yielded 2.3-keV FWHM at 975 keV for electrons and 1.3-keV FWHM at 75 keV for X-rays. A detailed study of the absolute detection efficiency (at 5 mm from the source) was performed, where this quantity was determined experimentally in the range of electron transition energies between 25.5 keV and 1047.8 keV and subsequently simulated using the GEANT4 code. Measurement and simulations are found to be in excellent agreement. A precise characterization, for this type of detector system, of the absolute detection efficiency for such a wide energy range is reported for the first time.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Measurement of the 240 Pu/ 239 Pu mass ratio using a transition-edge-sensor microcalorimeter for total decay energy spectroscopy

In this study, we have developed a new category of sensor for measurement of the 240 Pu/ 239 Pu mass ratio from aqueous solution samples with advantages over existing methods. Aqueous solution plutonium samples were evaporated and encapsulated inside of a gold foil absorber, and a superconducting transition-edge-sensor microcalorimeter detector was used to measure the total reaction energy (Q-value) of nuclear decays via heat generated when the energy is thermalized. Since all of the decay energy is contained in the absorber, we measure a single spectral peak for each isotope, resulting in a simple spectral analysis problem with minimal peak overlap. We found that mechanical kneading of the absorber dramatically improves spectral quality by reducing the size of radioactive inclusions within the absorber to scales below 50 nm such that decay products primarily interact with atoms of the host material. Due to the low noise performance of the microcalorimeter detector, energy resolution values of 1 keV fwhm (full width at half-maximum) at 5.5 MeV have been achieved, an order of magnitude improvement over α-spectroscopy with conventional silicon detectors. We measured the 240 Pu/ 239 Pu mass ratio of two samples and confirmed the results by comparison to mass spectrometry values. These results have implications for future measurements of trace samples of nuclear material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Nevada National Security Site Underground Radionuclide Inventory, 1951-1992: Accounting for Radionuclide Decay through September 30, 2012

This report is an update of report LA-13859-MS (Bowen et al., 2001). In that original report, the underground radionuclide inventory at the Nevada National Security Site (NNSS) was decay corrected to September 23, 1992, the date of the last underground nuclear test at the NNSS. In this report, the inventory is updated to account for the decay of radionuclides over two additional decades (1992-2012) and revised tritium, fission product and actinide inventory figures and tables are presented. The maximum contaminant levels for radionuclides were also updated to Safe Drinking Water Act Maximum Contaminant Levels (MCLs) (CFR, 2013). Also, a number of minor errata found in the original publication were corrected. An inventory of radionuclides produced by 828 underground nuclear tests conducted at the NNSS by the Lawrence Livermore National Laboratory, the Los Alamos National Laboratory, and the Department of the Defense from 1951 to 1992 includes tritium, fission products, actinides, and activation products. The inventory presented in this report provides an estimate of radioactivity remaining underground at the NNSS after nuclear testing. The original test inventory is decayed to September 30, 2012, and predictions of inventory decay over the subsequent 1000 years are presented. For the purposes of summary and publication, the Los Alamos National Laboratory and Lawrence Livermore National Laboratory authors of this report subdivided the inventory into five areas corresponding to the principal geographic test centers at the NNSS. The five areas roughly correspond to Underground Test Area “Corrective Action Units” (CAUs) for remediation of groundwater. In addition, the inventory is further subdivided for the Yucca Flat region by tests where the working point depth is more than 328 feet (100 meters) above the water table and tests that were detonated below that level. Water levels used were those from the U. S. Department of Energy, Nevada Operations Office (1997), now called the Nevada Field Office. Curie activities and atoms are reported as of September 30, 2012. This inventory is strictly a compilation of the residual radiologic inventory remaining from the underground nuclear tests conducted by Lawrence Livermore National Laboratory, Los Alamos National Laboratory and the Department of the Defense from 1951 to 1992 and does not include radioactivity from other types of nuclear testing (e.g., atmospheric, reactors, rocket engines). A companion classified report (Miller et al., 2002) contains test-specific data for each test performed at the NNSS. This work has been sponsored by the U. S. Department of Energy, National Nuclear Security Administration Nevada Field Office.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Impact of Modular Total Absorption Spectrometer measurements of β decay of fission products on the decay heat and reactor ν ¯ e flux calculation

Here, we report the results of a β-decay study of fission products 86 Br, 89 Kr, 89 Rb, 90 gs Rb, 90m Rb, 90 Kr, 92 Rb, 139 Xe, and 142 Cs performed with the Modular Total Absorption Spectrometer (MTAS) and on-line mass-separated ion beams. These radioactivities were assessed by the Nuclear Energy Agency as having high priority for decay heat analysis during a nuclear fuel cycle. We observe a substantial increase in β feeding to high excited states in all daughter isotopes in comparison to earlier data. This increases the average γ-ray energy emitted by the decay of fission fragments during the first 10 000 s after fission of 235 U and 239 Pu by approximately 2% and 1%, respectively, improving agreement between results of calculations and direct observations. New MTAS results reduce the reference reactor ¯ν e flux used to analyze reactor ¯ν e interaction with detector matter. The reduction determined by the ab initio method for the four nuclear fuel components, 235 U, 238 U, 239 Pu, and 241 Pu, amounts to 0.976, 0.986, 0.983, and 0.984, respectively.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Exploring isospin symmetry breaking in exotic nuclei: High-precision mass measurement of 23 Si and shell-model calculations of 𝑇 = 5/2 nuclei

Here, we present a high-precision mass measurement of the proton-rich nucleus 23 Si, performed with the LEBIT Penning trap at the Facility for Rare Isotope Beams (FRIB) utilizing the time-of-flight ion cyclotron resonance (TOF-ICR) technique. We determined a mass excess of 23362.9(5.8) keV, which agrees with a recent storage-ring measurement from the experimental Cooler-Storage Ring (CSRe) in Lanzhou but has a factor of 20 improved precision 23 Si is hence the nucleus with the most precisely known mass among all nuclei with an isospin projection of 𝑇 𝑧 = −5/2. We performed shell-model calculations with the USDC and USDCm Hamiltonians to study binding energy differences and Thomas-Ehrmann shifts in mirror systems with an isospin up to 𝑇 = 5/2. Our experimental result and other recently reported masses of neutron-deficient sd-shell nuclei agree well with the theoretical predictions, demonstrating that isospin symmetry breaking in sd-shell nuclei—even at high isospin values—is well described by modern shell-model calculations.

20 ≤ A ≤ 38↗

$β$-delayed neutron emission studies of 137,138 I and 144,145 Cs performed with trapped ions

A detailed study of the β-delayed neutron emission properties of 137,138 I and 144,145 Cs has been performed by confining ions in the Beta-decay Paul Trap. The daughter ions following β decay emerge from the trapped-ion cloud with negligible scattering allowing reconstruction of the recoil-ion energy from the time of flight. From this information, the neutron-emission branching ratios and neutron-energy spectra were deduced. The results for the 137 I and 144,145 Cs decays are in agreement with previous results performed using direct neutron-detection techniques. In the case of 138 I, a branching ratio of 6.18(50)% is obtained, yielding a value consistent with the more recent results, which are a factor of two larger than measurements made prior to 1978.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Two-proton decay from α-cluster states in 10 C and 11 N

Two-proton decay from excited states in 10 C and 11 N has been characterized from an analysis of the 2p + 2α and 3p + 2α exit channels. Data from four previously published invariant-mass studies associated with inelastic excitation, multinucleon knockout, and neutron pickup reactions have been considered. A rotational band in 10 C was identified built on the second 0 + state which has strong α-cluster molecular structure. The members of this band were tentatively identified up to J π = 4 + and all identified states have a prompt 2p decay branch. The spins of the 0 + and 2 + members were deduced from comparisons of the momentum correlations in their 2p branches to those from known 2p emitters. The 2 + and the tentative 4 + members are both above the α threshold and exhibit large reduced decay widths for α emission. This band exhibits a similar moment of inertia to its analog in the mirror nucleus 10 Be. Evidence is also presented for a molecular band in 11 N built on the second 3/2 – state which 2p decays. Furthermore, tentative members of this band have been assigned up to J π = 9/2 – and their excitation energies also match their likely analogs in the mirror nucleus 11 Be.

6 ≤ A ≤ 19↗

High-precision mass measurement of 103 Sn restores smoothness of the mass surface

As a step towards the ultimate goal of a high-precision mass measurement of doubly magic 100 Sn, the mass of 103 Sn was measured at the Low Energy Beam and Ion Trap (LEBIT) located at the Facility for Rare Isotope Beams (FRIB). Utilizing the time-of-flight ion cyclotron resonance technique, a mass uncertainty of 3.7 keV was achieved, an improvement by more than an order of magnitude compared to a recent measurement performed in 2023 at the Cooler Storage Ring (CSRe) in Lanzhou. Although the LEBIT and CSRe mass measurements of 103 Sn are in agreement, they diverge from the experimental mass value reported in the 2016 version of the Atomic Mass Evaluation (AME2016), which was derived from the measured 𝑄 𝛽 + value and the mass of 103 In. In AME2020, this indirectly measured 103 Sn mass was classified as a “seriously irregular mass” and replaced with an extrapolated value, which aligns with the most recent measured values from CSRe and LEBIT. As such, the smoothness of the mass surface is confidently reestablished for 103 Sn. Here, LEBIT's mass measurement of 103 Sn enabled a significant reduction in the mass uncertainties of five parent isotopes which are now dominated by uncertainties in their respective 𝑄 values.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Enhanced sensitivity to trace 238 U impurity of sapphire via coincidence neutron activation analysis

Sapphire has mechanical and electrical properties that are advantageous for the construction of internal components of radiation detectors such as time projection chambers and bolometers. However, it has proved difficult to assess its 232 Th and 238 U content down to the picogram per gram level. Here, this work reports an experimental verification of a computational study that demonstrates 𝛾⁢𝛾 coincidence counting, coupled with neutron activation analysis (NAA), can reach ppt sensitivities. Combining results from 𝛾⁢𝛾 coincidence counting with those of earlier single-𝛾 counting based NAA shows that a sample of Saint Gobain sapphire has 232 Th and 238 U concentrations of <0.26 ppt and <2.3 ppt, respectively; the best constraints on the radiopurity of sapphire.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

On the Age of Cosmic Rays as Derived from the Abundance of Be-10

The isotopic composition of cosmic ray Be, B, C, and N was studied using a new range versus total light technique. Special emphasis was placed on the Be isotopes and in particular, on the radioactive isotope Be-10 due to its mean lifetime against decay. The experiment consisted of a thin trigger scintillator, an acrylic plastic Cerenkov detector and a spark chamber, followed by a totally active stack of 14 scintillation detectors. This stack of scintillators made possible the measurement of range, and also permitted the removal of interacting events by continuously monitoring their identities along their trajectories. The experiment was carried by balloon to atmospheric depths ranging from 3.5 to 5.0 g sq cm residual atmosphere for a total exposure time of 23 hr. Results indicate the survival of ( 55 + or -21) % of the Be-10 in the arriving cosmic rays; the data were interpreted using the leaky box model of cosmic ray propagation.

Hagen, F. A.↗

Development of Microwave Technology for TENORM Waste Treatment - 17377

The sludge and scales generated by the oil and gas industry usually contain radionuclides of the thorium and uranium decay chains, the so-called technologically enhanced, naturally occurring radioactive materials (TENORM) waste. The handling of this waste must consider both the radiation risks presented by those radionuclides and its chemical toxicity, due to the decomposition of oil residues, which may generate hydrogen sulfide and other hazardous compounds. In the case of Brazil, Public Law 10.308 limits the management options for radioactive waste generated by offshore oil production rigs to drumming and storage; it prohibits disposal of any radioactive waste in sea-waters, seabed or oceanic islands. This paper describes the results of the work to develop a treatment process using a specially designed microwave oven, which removes simultaneously water and hydrocarbons from the sludge, thus reducing the volume, the chemical toxicity and the chemical reactivity of the waste. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

SU-F-T-368: Improved HPGe Detector Precise Efficiency Calibration with Monte Carlo Simulations and Radioactive Sources

Purpose: To obtain an improved precise gamma efficiency calibration curve of HPGe (High Purity Germanium) detector with a new comprehensive approach. Methods: Both of radioactive sources and Monte Carlo simulation (CYLTRAN) are used to determine HPGe gamma efficiency for energy range of 0–8 MeV. The HPGe is a GMX coaxial 280 cm{sup 3} N-type 70% gamma detector. Using Momentum Achromat Recoil Spectrometer (MARS) at the K500 superconducting cyclotron of Texas A&M University, the radioactive nucleus {sup 24} Al was produced and separated. This nucleus has positron decays followed by gamma transitions up to 8 MeV from {sup 24} Mg excited states which is used to do HPGe efficiency calibration. Results: With {sup 24} Al gamma energy spectrum up to 8MeV, the efficiency for γ ray 7.07 MeV at 4.9 cm distance away from the radioactive source {sup 24} Al was obtained at a value of 0.194(4)%, by carefully considering various factors such as positron annihilation, peak summing effect, beta detector efficiency and internal conversion effect. The Monte Carlo simulation (CYLTRAN) gave a value of 0.189%, which was in agreement with the experimental measurements. Applying to different energy points, then a precise efficiency calibration curve of HPGe detector up to 7.07 MeV at 4.9 cm distance away from the source {sup 24} Al was obtained. Using the same data analysis procedure, the efficiency for the 7.07 MeV gamma ray at 15.1 cm from the source {sup 24} Al was obtained at a value of 0.0387(6)%. MC simulation got a similar value of 0.0395%. This discrepancy led us to assign an uncertainty of 3% to the efficiency at 15.1 cm up to 7.07 MeV. The MC calculations also reproduced the intensity of observed single-and double-escape peaks, providing that the effects of positron annihilation-in-flight were incorporated. Conclusion: The precision improved gamma efficiency calibration curve provides more accurate radiation detection and dose calculation for cancer radiotherapy treatment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗