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Fluorescence time profile measurement of LAB based liquid scintillator in response to medium relativistic ion particles

Liquid scintillator is widely used in particle physics experiments due to its high light yield, good timing resolution, scalability and low cost. Certain liquid scintillators exhibit pulse shape discrimination capabilities because of difference in fluorescence timing properties induced by different particles. Its fluoresence timing properties have been measured mostly for radioactive decay sources at MeV energies. Here, we present a novel measurement of fluorescence time properties of Linear Alkyl Benzene (LAB) based liquid scintillator in response to high-energy ions of hydrogen (Z = 1), helium (Z = 2) and krypton at around 200–300 MeV/u for the first time. We compared the results to those from radioactive sources and observed a distinct dE / dX dependence, regardless of the particle type. These findings are essential for physics searches such as the diffuse supernova neutrino background in large liquid scintillator detectors like JUNO, and are also critical towards understanding the underlying scintillation timing mechanism.

Ion identification systems↗

SU-C-201-05: Imaging 212Pb-TCMC-Trastuzumab for Alpha Radioimmunotherapy for Ovarian Cancer

Purpose: To support the phase I trial for toxicity, biodistribution and pharmacokinetics of intra-peritoneal (IP) 212Pb-TCMC-trastuzumab in patients with HER-2 expressing malignancy. A whole body gamma camera imaging method was developed for estimating amount of 212Pb-TCMC-trastuzumab left in the peritoneal cavity. Methods: {sup 212}Pb decays to {sup 212}Bi via beta emission. {sup 212}Bi emits an alpha particle at an average of 6.1 MeV. The 238.6 keV gamma ray with a 43.6% yield can be exploited for imaging. Initial phantom was made of saline bags with 212Pb. Images were collected for 238.6 keV with a medium energy general purpose collimator. There are other high energy gamma emissions (e.g. 511keV, 8%; 583 keV, 31%) that penetrate the septae of the collimator and contribute scatter into 238.6 keV. An upper scatter window was used for scatter correction for these high energy gammas. Results: A small source containing 212Pb can be easily visualized. Scatter correction on images of a small 212Pb source resulted in a ∼50% reduction in the full width at tenth maximum (FWTM), while change in full width at half maximum (FWHM) was <10%. For photopeak images, substantial scatter around phantom source extended to > 5 cm outside; scatter correction improved image contrast by removing this scatter around the sources. Patient imaging, in the 1st cohort (n=3) showed little redistribution of 212Pb-TCMC-trastuzumab out of the peritoneal cavity. Compared to the early post-treatment images, the 18-hour post-injection images illustrated the shift to more uniform anterior/posterior abdominal distribution and the loss of intensity due to radioactive decay. Conclusion: Use of medium energy collimator, 15% width of 238.6 keV photopeak, and a 7.5% upper scatter window is adequate for quantification of 212Pb radioactivity inside peritoneal cavity for alpha radioimmunotherapy of ovarian cancer. Research Support: AREVA Med, NIH 1UL1RR025777-01.

60 APPLIED LIFE SCIENCES↗

Half-life of 67 Cu

The half-life of 67 Cu was determined through serial gamma-ray spectrometry measurements of the dominant gamma emission (E γ : 184.6 keV; branching ratio: 48.7%) produced following β- decay. Data were collected consecutively for 1000 s per measurement, with a total of 3063 measurements over the duration of 36 days. The incidence rate for the 184.6 keV gamma-ray was determined from the spectral peak area and duration of each measurement. This rate was then corrected to account for detector dead-time, radioactive decay during each acquisition and drift in the computer clock in comparison to NIST nuclear clock. Least-squares regression analysis was performed to determine the half-life of 67 Cu. The result was 61.761 ± 0.004 h, which is the highest precision measurement to date, and marks a 24-fold precision improvement over the current Nuclear Data Sheets value.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Sci-Thur AM: YIS – 01: New technologies for astatine-211 targeted alpha therapy research

Purpose: The short-range, densely ionizing α-particles emitted by {sup 211}At (t{sub 1/2}=7.2h) are well suited for the treatment of diffuse microscopic disease, using cancer targeting biomolecules. {sup 211}At availability is limited by the rarity of α-cyclotrons required for standard production. Image-based dosimetry is also limited for {sup 211}At, which emits low intensity X-rays. Our goal was to leverage state-of-the-art infrastructure at TRIUMF to produce and evaluate two related isotopes, {sup 211}Rn (t{sub 1/2}=14.6h, 73% decay to {sup 211}At) as a generator for {sup 211}At, and {sup 209}At (t{sub 1/2}=5.4h, X-ray/gamma-ray emitter) as a novel 211At surrogate for preclinical imaging studies. Methods: Produced by spallation of uranium with 480 MeV protons, mass separated ion beams of short-lived francium isotopes were implanted into NaCl targets where {sup 211}Rn or {sup 209}At were produced by radioactive decay, in situ. {sup 211}Rn was transferred to dodecane from which {sup 211}At was efficiently extracted and evaluated for clinical applicability. High energy SPECT/CT was evaluated for measuring {sup 209}At activity distributions in mice and phantoms. Results: Our small scale {sup 211}Rn/{sup 211}At generator system provided high purity {sup 211}At samples. The methods are immediately scalable to the level of radioactivity required for in vivo experiments with {sup 211}At. {sup 209}At-based high energy SPECT imaging was determined suitable for pursuing image-based dosimetry in mouse tumour models. In the future, we will utilize quantitative {sup 209}At-SPECT for image-based dose calculations. Conclusion: These early studies provided a foundation for future endeavours with {sup 211}At-based α-therapy. Canada is now significantly closer to clinical targeted α-therapy of cancer.

60 APPLIED LIFE SCIENCES↗

Nuclear Structure and Decay Data for A=71 Isobars

Experimental nuclear spectroscopic data are evaluated for 12 known nuclides of mass number=71 (Mn, Fe, Co, Ni, Cu, Zn, Ga, Ge, As, Se, Br, Kr). Detailed compiled and evaluated information is presented for each reaction and decay experiment. The β – n decay of 72 Co to 71 Ni is included in this work, while for β – n decay of 71 Co to 70 Ni, consult Nuclear Data Sheets for A=70 (2016Gu11) or the ENSDF database for 70 Ni. Combining all the available data, recommended values are provided for energies, spins and parities, and half-lives of levels, with energies, branching ratios and multipolarities of γ radiations, and characteristics of β and α radiations in radioactive decays. Excited-states have not yet been identified in 71 Mn, 71 Fe, and 71 Kr, with the ground-state half-life remaining unknown only for 71 Mn; data for excited states in 71 Co and 71 Ni are very limited; 71 Ga, 71 Ge and 71 As are the most extensively studied nuclides via various reactions and decays, followed by 71 Cu, 71 Zn, 71 Se, and 71 Br, however, except for 71 Ge, the decay schemes of all other nuclides are considered as incomplete due to a large gap between the decay Q-value and the highest observed level. Lastly, this work supersedes earlier evaluations of A=71 by 2011Ab01.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

SU-F-T-663: Cerenkov Radiation Enhanced Radiotherapy with Titanium Dioxide Nanoparticle: A Monte Carlo Study

Purpose: A recent publication has shown that by delivering titanium dioxide nanoparticles (titania) as a photosensitizer into tumors, Cerenkov radiation (CR) produced by radionuclides could be used for substantially boosting damage to cancer cells. The present work compares CR production by various clinically relevant radiation sources including internal radionuclides and external beam radiotherapy (EBRT), and provides preliminarily computational results of CR absorption by titania. Methods: 1) Geant4.10.1 was used to simulate ionizing radiation-induced CR production in a 1cm diameter spherical volume using external radiotherapy sources: Varian Clinac IX 6MV and Eldorado {sup 60}Co, both with 10*10 cm{sup 2} field size. In each case the volume was placed at the maximum dose depth (1.5cm for 6MV source and 0.5cm for {sup 60}Co). In addition, {sup 18}F, {sup 192}Ir and {sup 60}Co were simulated using Geant4 radioactive decay models as internal sources. Dose deposition and CR production spectra in 200nm-400nm range were calculated as it is the excitation range of titania. 2) Using 6MV external source, the absorption by titania was calculated via the track length of CR in the spherical volume. The nanoparticle concentration was varied from 0.25 to 5µg/g. Results: Among different radioactive sources, results showed that {sup 18}F induced the highest amount of CR per disintegration, but {sup 60}Co had the highest yield per unit dose. When compared with external sources, 6MV source was shown to be the most efficient for the the same delivered dose. Simulations indicated increased absorption for increasing concentrations, with up to 68% absorption of generated CR for 5µg/g titania concentration. Conclusion: The results demonstrate that 6MV beam is favored with a higher CR yield, compared to radionuclides, and that the use of higher concentrations of titania may increase photosensitization. From the findings, we propose that if sufficiently potent concentrations of titania are delivered to tumors this could substantially boost EBRT.

60 APPLIED LIFE SCIENCES↗

SN 1987A - Out on the tail

The expected light curve of Supernova 1987A is calculated for the next 10 yr based solely upon energy input from radioactive decay of Co-56 and Co-57. During the third year, energy input from Co-57 begins to dominate. How the bolometric (ultraviolet-optical-infrared) light curve deviates from that given by 100 percent deposition of the gamma-rays is a measure of the mixing that has gone on in the supernova. Current measurements favor a mixed model. The radioactive light curve decreases beneath 10 to the 39th ergs/s at an age of about 900 days, by which time the neutron star remnant should have made its presence known.

Pinto, Philip A.↗

FISPACT-II: An Advanced Simulation System for Activation, Transmutation and Material Modelling

Fispact-II is a code system and library database for modelling activation-transmutation processes, depletion-burn-up, time dependent inventory and radiation damage source terms caused by nuclear reactions and decays. The Fispact-II code, written in object-style Fortran, follows the evolution of material irradiated by neutrons, alphas, gammas, protons, or deuterons, and provides a wide range of derived radiological output quantities to satisfy most needs for nuclear applications. It can be used with any ENDF-compliant group library data for nuclear reactions, particle-induced and spontaneous fission yields, and radioactive decay (including but not limited to TENDL-2015, ENDF/B-VII.1, JEFF-3.2, JENDL-4.0u, CENDL-3.1 processed into fine-group-structure files, GEFY-5.2 and UKDD-16), as well as resolved and unresolved resonance range probability tables for self-shielding corrections and updated radiological hazard indices. The code has many novel features including: extension of the energy range up to 1 GeV; additional neutron physics including self-shielding effects, temperature dependence, thin and thick target yields; pathway analysis; and sensitivity and uncertainty quantification and propagation using full covariance data. The latest ENDF libraries such as TENDL encompass thousands of target isotopes. Nuclear data libraries for Fispact-II are prepared from these using processing codes PREPRO, NJOY and CALENDF. These data include resonance parameters, cross sections with covariances, probability tables in the resonance ranges, PKA spectra, kerma, dpa, gas and radionuclide production and energy-dependent fission yields, supplemented with all 27 decay types. All such data for the five most important incident particles are provided in evaluated data tables. The Fispact-II simulation software is described in detail in this paper, together with the nuclear data libraries. The Fispact-II system also includes several utility programs for code-use optimisation, visualisation and production of secondary radiological quantities. Included in the paper are summaries of results from the suite of verification and validation reports available with the code.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Spent Nuclear Fuel Disposition

One interdisciplinary field devoted to achieving the end-state of used nuclear fuel (UNF) through reuse and/or permanent disposal. The reuse option aims to make use of the remaining energy content in UNF and reduce the amount of long-lived radioactive materials that require permanent disposal. The planned approach in the U.S., as well as in many other countries worldwide, is direct permanent disposal in a deep geologic repository. Used nuclear fuel is fuel that has been irradiated in a nuclear reactor to the point where it is no longer capable of sustaining operational objectives. The vast majority (by mass) of UNF is from electricity generation in commercial nuclear power reactors. Furthermore, the other main source of UNF in the U.S. is the Department of Energy’s (DOE) and other federal agencies’ operation of reactors in support of federal government missions, such as materials production, nuclear propulsion, research, testing, and training. Upon discharge from a reactor, UNF emits considerable heat from radioactive decay. Some period of active on-site cooling (e.g., 2 or more years) is typically required to facilitate efficient packaging and transportation to a disposition facility. Hence, the field of UNF disposition broadly includes storage, transportation and ultimate disposition. See also: Nuclear Fission (content/nuclear-fission/458400), Nuclear Fuels (/content/nuclear-fuels/458600), Nuclear Fuel Cycle (/content/nuclear-fuel-cycle/458500), Nuclear Fuels Reprocessing (/content/nuclear-fuels-reprocessing/458700), Nuclear Power (/content/nuclear-power/459600), Nuclear Reactor (/content/nuclear-reactor/460100), Radiation (/content/radiation/566300), and Radioactive Waste Management (/content/radioactive-waste-management/568900).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Neutron-star mergers and new opportunities in rare isotope experimental research

The recent observation of the first neutron-star merger event GW170817 had major impact on our understanding of stellar nucleosynthesis. It was identified for the first time as one of the sites for the astrophysical r process, a process that is responsible for the synthesis of roughly half of the isotopes of the heavy elements. The observed kilonova afterglow from the neutronstar merger event was interpreted as the result of the radioactive decays of r-process isotopes as they decay back to the valley of stability. The observed kilonova light curve is however broad due to its complex composition and the Doppler-shift due to fast moving matter, and is therefore impossible to interpret without accurate knowledge of the nuclear properties of the nuclei involved. This work focuses on the current experimental efforts to measure the relevant nuclear properties, together with plans for the next generation radioactive beam facilities, and in particular the Facility for Rare Isotope Beams (FRIB).

79 ASTRONOMY AND ASTROPHYSICS↗

Retrospective Imaging and Characterization of Nuclear Material

Modern techniques for detection of covert nuclear ma-terial requires some combination of real time measurement and/or sampling of the material. More common is real time measure-ment of the ionizing emission caused by radioactive decay or through the materials measured in response to external interroga-tion radiation. One can expose the suspect material with various radiation types, including high energy photons such as x rays or with larger particles such as neutrons and muons, to obtain images or measure nuclear reactions induced in the material. Stand-off detection using imaging modalities similar to those in the medical field can be accomplished, or simple collimated detec-tors can be used to localize radioactive materials. In all such cases, the common feature is that some or all of the nuclear materials have to be present for the measurement, which makes sense; as one might ask, “How you can measure something that is not there?” The current work and results show how to do exactly that: characterize nuclear materials after they have been removed from an area leaving no chemical trace. This new approach is demon-strated to be fully capable of providing both previous source spa-tial distribution and emission energy grouping. The technique uses magnetic resonance for organic insulators and/or lumines-cence techniques on ubiquitous refractory materials similar in theory to the way the nuclear industry carries out worker person-nel dosimetry. Spatial information is obtained by acquiring gridded samples for dosimetric measurements, while energy infor-mation comes through dose depth profile results that are func-tions of the incident radiation energies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Issue Resolution During the Development of the Performance Assessment for the Savannah River Site Saltstone Disposal Facility - 20125

In 2019, Savannah River Remediation developed a revision to the performance assessment (PA) on behalf of the U.S. Department of Energy (DOE) Savannah River Operations Office (SR) for the near-surface disposal of low-level waste at the Savannah River Site (SRS) Saltstone Disposal Facility (SDF). Soluble waste from SRS Tank Farms undergoes salt processing to remove cesium and other high-activity constituents. The low-activity decontaminated salt solution (DSS) is then immobilized by mixing it into a cementitious waste form known as saltstone. After mixing, the saltstone is poured into leak-tight concrete vaults, known as saltstone disposal units (SDUs), where the waste form cures. By the time of facility closure, the SDF is expected to consist of 15 SDUs with a combined capacity of 1.06 E+09 L (280 Mgal) of cured saltstone. The facility operates under a Disposal Authorization Statement from DOE and a permit from the South Carolina Department of Health and Environmental Control (SCDHEC). Since the start of operations in 1990, the SDF has received almost 6.7 E+07 L (18 Mgal) of DSS, resulting in the safe disposal of 2.7 E+16 Bq (7.3 E+05 Ci) of activity. Due to the radioactive decay of short-lived contaminants, the total remaining activity in the disposed waste is estimated to be approximately 1.4 E+16 Bq (3.9 E+05 Ci), as of September 2018. The Disposal Authorization Statement requires a demonstration that the system of engineered and natural features of the disposal facility will limit releases from the facility and be protective of human health and the environment for at least the next 1,000 years. The long-term performance of the facility was evaluated under the requirements of the DoE's Radioactive Waste Management Manual (US DOE Manual 435.1-1). Simulations were performed to demonstrate that the disposal facility would meet performance objectives specified in the manual. The evaluation was based on numerical models that simulate the releases of contaminants from the saltstone waste form. Contaminants were transported through groundwater and air pathways to points of assessment to evaluate compliance (i.e., 100 m from the SDUs). In addition, the potential consequences of an inadvertent human intrusion (IHI) were also evaluated. A number of issues were overcome during the development of these simulations. These issues were identified as part of internal technical reviews. Simulations are developed by people and people make mistakes, so the internal technical review process is a vital step in PA development. Specific examples of resolved issues include a unit-conversion error, an inappropriate definition for a model boundary condition, a model time-stepping issue, and an error in the calculation for the buildup of contaminants in soil. Actions taken to address these issues resulted in an improved product with a better supported technical basis and more defensible results. The identification and correction of these issues are discussed. By understanding these issues, model developers and technical reviewers working on PAs in the future may avoid repeating these types of mistakes. Transparency with respect to these mistakes builds trust between waste management sites, regulators, and stakeholders. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Decay Curve Correction Analysis Report

The decay curve analysis that is done on the short-lived radionuclide gas samples is used to differentiate between gaseous radionuclides that have the same characteristic gamma decay energy, 511 kiloelectron-volts (keV). A sample of stack gas is isolated and the total counts in the 511 keV peak are counted repeatedly in 10-second intervals to evaluate the decay rate of the sample over time. Analysis of this decay data required a series of steps. First, a raw data report is generated by the gamma acquisition system, based on an analysis template within the acquisition software. The data report file was then loaded into Microsoft Word, and a macro was used to perform minor formatting (remove colons and insert tabs between data columns) to allow analysis within Excel. The file is then saved as a text file at this point. The text file is then uploaded into Excel and a series of macros are used to add labels, calculate radioactive decay constants, and analyze the gamma decay data using linear regression techniques. The analysis template has been used since 1998 for stack 53000303 (TA-53, building 0003, exhaust stack 03) and 2000 for stack 53000702. The overall process, including the gamma report format and the macros used in Word and Excel for processing the report, had remained unchanged until 2015. In October of 2015, staff made a change to the report template in the gamma acquisition software which resulted in an error in the calculations later performed by the Excel macro. This error was not caught until a more in-depth review of the analysis took place regarding 2020 data. This report covers a much more complete review of the issue that occurred regarding the decay curve analysis, a review of the calculations completed to correct the issue, a review of the updated decay curve analysis process, and recommendations for moving forward.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Cassini Power Subsystem

The electrical output of Cassini’s power system has been decaying consistently as predicted during its 20-year mission between October 1997 and September 2017. The power telemetry data is presented for the entire Cassini mission, including launch, cruise, and Saturn tour, up to the most recent available data. The spacecraft has been powered by three independent Radioisotope Thermoelectric Generators (RTGs) connected in parallel, which were able to generate 882 W at the beginning of the mission shortly after launch. The decrease in power energy output has mainly been driven by the heat reduction of the hot side of the RTGs due to the natural radioactive decay of its heat source plutonium (mostly plutonium-238 [238Pu]), degradation of thermoelectric material performance, and interface degradation.

Carr, Gregory A.↗

Building surrogate models of nuclear density functional theory with Gaussian processes and autoencoders

From the lightest Hydrogen isotopes up to the recently synthesized Oganesson (Z = 118), it is estimated that as many as about 8,000 atomic nuclei could exist in nature. Most of these nuclei are too short-lived to be occurring on Earth, but they play an essential role in astrophysical events such as supernova explosions or neutron star mergers that are presumed to be at the origin of most heavy elements in the Universe. Understanding the structure, reactions, and decays of nuclei across the entire chart of nuclides is an enormous challenge because of the experimental difficulties in measuring properties of interest in such fleeting objects and the theoretical and computational issues of simulating strongly-interacting quantum many-body systems. Nuclear density functional theory (DFT) is a fully microscopic theoretical framework which has the potential of providing such a quantitatively accurate description of nuclear properties for every nucleus in the chart of nuclides. Thanks to high-performance computing facilities, it has already been successfully applied to predict nuclear masses, global patterns of radioactive decay like β or γ decay, and several aspects of the nuclear fission process such as, e.g., spontaneous fission half-lives. Yet, predictive simulations of nuclear spectroscopy—the low-lying excited states and transitions between them—or of nuclear fission, or the quantification of theoretical uncertainties and their propagation to basic or applied nuclear science applications, would require several orders of magnitude more calculations than currently possible. However, most of this computational effort would be spent into generating a suitable basis of DFT wavefunctions. Such a task could potentially be considerably accelerated by borrowing tools from the field of machine learning and artificial intelligence. In this paper, we review different approaches to applying supervised and unsupervised learning techniques to nuclear DFT.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Long Term Assessment of Radiocesium in Deer, Fish, Soil, and Vegetation at the Savannah River Site

Throughout the Savannah River Site's (SRS) operational history, many radionuclides have been released into the environment. However, due to fallout from weapons testing, the amount released from SRS, its persistence in the environment, and the seclusion of the Site, radiocesium (Cs-137) is one of the most critical radionuclides in the SRS environment. The Effective half-life (Te) is the time it takes for a radionuclide in the environment to decrease by 50% of its initial amount. There are three means of radionuclide removal: Physical: Radioactive decay, sedimentation, and washout; Chemical: Changes in pH, oxidation state or adsorption; Biological: Changes in the food web or translocation. Effective half-life (T{sub e}) = log{sub e}2/λ{sub e} Where λ{sub e} is estimated from the slopes of loge-transformed Cs-137 activity concentrations regressed on year. The objective of this work was to calculate the effective half-life of Cs-137 in various biota at SRS and to perform an assessment of the changes in the effective half life over time. Compared to 2013 data, there is a slight increase in the effective half-lives for fish at most sampling locations. This effective half-life increase is an indication that the rate of Cs-137 loss is starting to plateau. The effective half-life of Cs-137 in SRS fish ranges from 4-11 years. The effective half-life of Cs-137 in soil at the Creek plantation is about 15 years. The effective half-life of Cs-137 in grassy vegetation at the Creek Plantation is about 14 years. The effective half-life of deer hunted on the SRS is about 15.5 years. After termination of all reactor activity by 1980, the Cs-137 activity began to drop drastically.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Thermal Desorption of Tritium from Fluoride Salt-Cooled Reactor Materials

The fluoride-salt-cooled high-temperature reactor (FHR) is a high-temperature fission reactor concept involving a liquid fluoride salt coolant, coated particle fuel, and enhanced passive safety mechanisms. Utilizing a low-pressure coolant and high temperature fuel allows for smaller reactor buildings and use of gas Brayton power cycles for higher efficiency in electricity production. One of the fluoride salts being considered for the FHR coolant is 2LiF - BeF{sub 2} (flibe). Tritium is generated frequently in flibe from thermal neutron transmutation of Li-6 and Be-9. Tritium retention in irradiated structural materials presents a challenge to the design of the FHR; high neutron fluence can induce significant material damage and alteration of microstructures to trap tritium in the structure, particularly in carbon-based materials (such as steels). Investigation of tritium transport in flibe salt and structural materials is also critical to evaluating mass balance of tritium in a system for quantifying leakage of tritium to the environment. It is important to understand the uptake of tritium in these proposed core materials since the transport of tritium within an FHR is of critical concern for operational safety due to corrosion, and to prevent tritium release into the environment. The presence of TF corrodes stainless steel by oxidizing chromium. Tritium gas (T{sub 2}) easily diffuses through reactor materials and can be released into the environment through the primary piping and heat exchangers. There is great interest in identifying materials that are compatible with the FHR environment that can be used to getter tritium from the salt, or to inhibit the diffusion of tritium to prevent its release into the environment. As part of the FHR Integrated Research Project (IRP), capsules containing proposed core materials immersed in flibe salt were irradiated at 700 deg. C for 1000 hours (FS-1) and 300 hours (FS-2) in the MIT Research Reactor (MITR). During irradiation, tritium is produced in the salt, and then interacts with the other materials in the capsule. Measurements of the effluent gas during the FHR IRP irradiation experiments indicated that less than 1% of the tritium generated in the salt escaped in the gas phase. It is assumed that most of the tritium was captured, either via diffusion or surface adsorption, on the materials inside the capsule. Tritium frequently adsorbs to sample surfaces in the form of HTO, which requires relatively low temperatures to release (on the order of 100 deg. C). In certain cases, tritium can be bound in the bulk of materials from diffusion or neutron transmutation of lithium and beryllium in the structural materials. Accurate measurement of very small concentrations of hydrogen is difficult; by taking advantage of the radioactive decay of tritium (which emits low-energy beta radiation), several methods become available to detect and quantitatively measure the tritium. The most sensitive method is liquid scintillation counting (LSC), which requires the tritium to be suspended in optically-transparent liquid media that is compatible with scintillating solution, such as water. This measurement technique requires the tritium to be extracted from the material, which can be achieved through leaching into water, thermal desorption, or complete destruction of the sample by acid digestion or pyrolysis. A less destructive method is preferred in order to preserve the specimens, reduce the generation of radioactive mixed wastes, and minimize the carryover of other activation products. For total thermal desorption of tritium from the materials, the tritiated materials must be heated to temperatures in excess of 300 deg. C. Heating the specimens above the irradiation temperature will re-mobilize the tritium and allow it to be captured from the gas stream directly into LSC media. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

First experimental determination of the ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar reaction cross section and ³⁹Ar production in Earth’s atmosphere

The cosmogenic ³⁹Ar(t1∕2 = 268 years) isotope of argon is used for geophysical dating and tracing of underground and ocean water, as well as ice owing to its appropriate half-life and chemical inertness as a noble gas; ³⁹Ar serves also in nuclear weapon test monitoring. We measured for the first time the total cross section of the main ³⁹Ar cosmogenic production reaction in the atmosphere, namely ⁴⁰Ar(𝑛, 2𝑛)39 Ar, using 14.8 ± 0.3 MeV neutrons. The neutrons, produced by a deuterium-tritium generator, impinged on a stainless steel sphere filled with Ar gas highly enriched in the ⁴⁰Ar isotope and were monitored by a stack of fast-neutron activation foils. The reaction yield was measured by atom counting of long-lived ³⁹Ar with noble gas accelerator mass spectrometry and, independently, by decay counting relative to atmospheric argon (³⁹Ar/Ar= 8.12 × 10−16 ). A total ⁴⁰Ar(𝑛, 2𝑛)39 Ar cross section of 610 ± 100 mb was determined at 14.8 ± 0.3 MeV incident neutron energy. This result serves as a benchmark for recent theoretical calculations and evaluations, found to reproduce well the experimental total cross section. We use these energy-dependent theoretical cross sections together with experimental spectra of cosmogenic neutrons at different altitudes to calculate the global average rate of neutron-induced ³⁹Ar atmospheric production, resulting in 770 ± 240 39 Ar atoms/cm²/day. The secular equilibrium between the ³⁹Ar calculated production rate and radioactive decay rate leads to a partial isotopic abundance ³⁹Ar/Ar = (5.9 ± 1.8) × 10−16 , showing that ≈73% of atmospheric ³⁹Ar is produced by cosmogenic neutrons, the remaining part believed to be induced by muons and high-energy 𝛾 rays. The ⁴⁰Ar(𝑛, 2𝑛)³⁹Ar cross section at 14 MeV is also a key parameter for quantifying the anthropogenic contribution to atmospheric 39 Ar produced during the thermonuclear tests of the 1960s. We estimate that anthropogenic ³⁹Ar accounts for roughly 20% of the present atmospheric inventory.

39 Ar atmospheric production↗