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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Advances in actinide thin films: synthesis, properties, and future directions

Actinide-based compounds exhibit unique physics due to the presence of 5f electrons, and serve in many cases as important technological materials. Targeted thin film synthesis of actinide materials has been successful in generating high-purity specimens in which to study individual physical phenomena. These films have enabled the study of the unique electron configuration, strong mass renormalization, and nuclear decay in actinide metals and compounds. The growth of these films, as well as their thermophysical, magnetic, and topological properties, have been studied in a range of chemistries, albeit far fewer than most classes of thin film systems. This relative scarcity is the result of limited source material availability and safety constraints associated with the handling of radioactive materials. Here, we review recent work on the synthesis and characterization of actinide-based thin films in detail, describing both synthesis methods and modeling techniques for these materials. Further, we review reports on pyrometallurgical, solution-based, and vapor deposition methods. We highlight the current state-of-the-art in order to construct a path forward to higher quality actinide thin films and heterostructure devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Gallium oxide semiconductor-based large volume ultrafast radiation hard spectroscopic scintillators

We report on the development of the first-ever inorganic radiation-hard moisture-insensitive large volume spectroscopic semiconductor-based scintillator with less than 2 ns decay time and light yields as high as 8000 ph/MeV. Despite extensive research into scintillator materials, the quest for an ideal scintillator combining ultrafast decay times (akin to BaF 2 and Yb-doped scintillators such as Lu 2 O 3 :Yb), high light yields (exceeding 2000 photons per MeV), spectroscopic capabilities, and exceptional radiation hardness remain unfulfilled. In this study, we demonstrate and report for the first time the viability of large-volume (up to 20 mm thickness) gallium oxide (β-Ga 2 O 3 ) semiconductor-based scintillators for applications requiring these properties. These β-Ga 2 O 3 scintillators were grown using the fast turnaround (~2 days) crucible-free optical float zone (FZ) technique. The high light yield and ultrafast decay time of these high-purity n-type semiconductors with free carrier concentration of 6 × 10 17 cm –3 are attributed to native defects, specifically oxygen vacancies (V O ) and gallium–oxygen vacancy pairs (V Ga –V O ), generated during optimized FZ growth. The ultrafast decay, along with high light yield, enables excellent timing resolution and high count rate detection for applications like time-of-flight positron emission tomography, physics experiments, and nuclear safety. The radiation hardness of these devices has been documented in a separate publication.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Cosmogenic production of 37 Ar in the context of the LUX-ZEPLIN experiment

We estimate the amount of 37 Ar produced in natural xenon via cosmic-ray-induced spallation, an inevitable consequence of the transportation and storage of xenon on the Earth’s surface. We then calculate the resulting 37 Ar concentration in a 10-tonne payload (similar to that of the LUX-ZEPLIN experiment) assuming a representative schedule of xenon purification, storage, and delivery to the underground facility. Using the spallation model by Silberberg and Tsao, the sea-level production rate of 37 Ar in natural xenon is estimated to be 0.024 atoms/kg/day. Assuming the xenon is successively purified to remove radioactive contaminants in 1-tonne batches at a rate of 1 tonne/month, the average 37 Ar activity after 10 tons are purified and transported underground is 0.058 − 0.090 𝜇⁢Bq/kg, depending on the degree of argon removal during above-ground purification. Such cosmogenic 37 Ar will appear as a noticeable background in the early science data, while decaying with a 35-day half-life. This newly noticed production mechanism of 37 Ar should be considered when planning for future liquid-xenon-based experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2012

Considerations, measurements and logistics associated with low-energy cyclotron decommissioning

The University of Iowa's 20-year-old 17 MeV Scanditronix cyclotron underwent decommissioning in the summer of 2011. To satisfy local, state and federal regulations defining removal, transportation and long-term safe and environmentally secure disposal of the 22 ton activated cyclotron, a series of nuclear spectroscopic measurements were performed to characterize the nature and extent of proton and neutron activation of the 22-ton cyclotron, its associated targets, and the concrete wall that was demolished to remove the old cyclotron. Neutron activation of the concrete wall was minimal and below exempt concentrations resulting in standard landfill disposal. The cyclotron assessment revealed the expected array of short and medium-lived radionuclides. Subsequent calculations suggest that meaningful levels residual activity will have decayed virtually to background after 15 years, with the total residual activity of the entire cyclotron dropping below 37 MBq (1 mCi).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Current and Projected Future Disposed Inventory Estimate for Trenches 31 and 34 for Performance Assessment and Composite Analysis

The purpose of this environmental calculation file (ECF) is to document and project future disposed radionuclide inventory estimates for the two currently active trenches in burial ground 218-W-5, which are designated as Trenches 31 and 34. This ECF also documents the current disposed radionuclide inventory estimate for the balance of the trenches in burial ground 218-W-5, which consist of 11 inactive trenches. All inventories were derived from disposal records maintained in the Solid Waste Information Tracking System (SWITS) database and are decayed corrected to a common date of January 1, 2070 to facilitate summation. This ECF supports modeling for performance assessment (PA) and composite analysis (CA) of waste facilities on the Hanford Site Central Plateau.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Preconceptual Design of Irradiated Fuel Salt Management System

The National Reactor Innovation Center was established by the U.S. Department of Energy to accelerate the demonstration and deployment of advanced nuclear reactors. To meet this mission, the National Reactor Innovation Center has developed the Laboratory for Operations and Testing in the U.S. (LOTUS) to support the first fast-spectrum molten salt reactor demonstration. The goal of this research is to understand the system requirements that may be applied to a molten salt reactor experiment in the LOTUS test bed and to perform systems analyses and preconceptual development of a storage container for the management of the irradiated molten salt fuel. This study proposes a set of irradiated fuel salt management processes for the molten salt reactor, from defueling to storage or disposal. For that, the historic Molten Salt Reactor Experiment (MSRE) at Oak Ridge National Laboratory has served as a crucial source of data for a mock application. This paper proposes a potential geometry for storing irradiated fuel salt based on MSRE data and the Monte Carlo N-Particle radiation transport code. The geometry was analyzed for criticality safety under abnormal situations, such as water ingress and interaction between containers. Based on the determined configuration of the storage system, the decay heat produced from the irradiated fuel salts was calculated to provide a reasonable time scale of the dormancy period. Using the same geometry assumed above, the neutron and gamma dose rates from the irradiated fuel salt at the end of the dormancy period were estimated, which will be useful for understanding the handling and radiation protection requirements for handling the irradiated fuel salt. Lastly, a reactor in the LOTUS test bed could use chloride-based fuel as opposed to the fluoride-based fuel used in MSRE. Thus, a literature study provided data to understand the similarities and differences between the characteristics of fluoride- and chloride-based salts in terms of salt chemistry, material characteristics, postirradiation behavior, neutronics, thermal hydraulics, and heat removal. This study, together with the proposed irradiated fuel salt management processes, preliminary criticality calculations, decay heat, and dose rate estimates, provides a strong basis for future investigation into the management of irradiated fuel salts generated during molten salt reactor technology demonstrations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Modeling DOE Standard Canister Configurations with Updated Surface Chemistry

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. 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 rate as the total dose applied in increased. A previous study created a small-scale chemical model was built to replicate a mini-canister surrogate system at SRNL as well as for the smaller capsule tests performed at INL. The previous iteration of the model utilized step function for its G-values for the hydrogen generation over a 200-year period. This model makes an update to the surface chemistry to account for theorized surface chemistry reactions allowing for oxygen to remain bounded to the oxyhydroxide layer. As additional experiments continue, the kinetic fits may be adjusted to adapt to new data. Three canister configurations are modeled – the base 18-inch, 15-foot DOR standard canister with 30 ATR fuel elements, an 18-inch, 10-foot DOE standard canister with 32 ATR fuel elements and a 24-inch, 10-foot DOE standard canister with 40 ATR fuel elements. In previous reports, the primary sensitivity of the canister conditions was identified as the decay heat of the fuel and the dried condition of the fuel. Only these parameters are studied in the report. For the nominal case with dried fuel, the hydrogen generation is only about 2%, so it is even less than the flammability limit if it were exposed to oxygen. For the densely packed 18-inch case the total hydrogen concentration is only around 4% with the nominal decay heat. For the densely packed 24-inch case the total hydrogen concentration is only 2.5%, roughly 20% higher than the original packing design, and still under flammability conditions if exposed to oxygen.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Measurements of β -delayed proton emitters in the region of 100 Sn

An experiment on neutron-deficient nuclei in the region of doubly magic 100 Sn was carried out at the Radioactive Ion Beam Factory (RIBF) at the RIKEN Nishina Center in Japan. 𝑁 ≈ 𝑍 ≈ 50 nuclei were produced following fragmentation of an intense primary 124 Xe beam and implanted in the Advanced Implantation Detector Array silicon setup for the first study of proton-rich nuclei with this system at RIKEN. Measurements of the 𝛽-delayed proton emitter decay half-lives, branching ratios and proton energy spectra of nuclei in the region of 100 Sn were performed, with improved precision in many cases. New results for the energy spectrum of 101 Sn are presented, where a 2.03(5)-MeV peak was observed. In conclusion, these results are compared to shell-model calculations, using the recent precise measurement of the 101 In proton separation energy are presented.

Appleton, C. J. [Univ. of Edinburgh, Scotland (Uni↗
DOE OSTI2022

Half-life measurement of the 199-keV isomeric state in Ga 76

Background: Isomeric states in atomic nuclei are a sensitive probe of their underlying microscopic structure and can be used to study the evolution of shell structure far from stability. Recent studies have identified and provided detailed spectroscopy of isomers in neutron-rich nuclei with Z = 28-50. Isomeric states in the odd-odd gallium isotopes have been reported for all gallium isotopes from A = 72 to A = 80 with the exception of 76 Ga. Purpose: The purpose of this experiment was to observe short-lived isomeric states in the vicinity of 78 Ni. Methods: In-beam fragmentation of a 86 Kr primary beam at the National Superconducting Cyclotron Laboratory produced radioactive ions which were delivered to and deposited in a Ce Br 3 scintillator coupled to a position-sensitive photomultiplier tube. Beta-delayed γ rays were measured by ancillary HPGe clover and LaBr 3 detectors which surrounded the implantation detector. Results: The previously observed J π = 1 + , 199-keV level in 76 Ga, populated following the β decay of 76 Zn, was identified as isomeric with a half-life of 34(1) stat. (8) sys. ns. Shell-model calculations suggest this state is formed by the coupling of protons in negative-parity configurations to 1/2 - neutron configurations. Transition strengths assuming a ground-state spin of J = 2 and J = 3 were determined from the experimental data.

59 ≤ A ≤ 89↗
DOE OSTI2015

Annual Continuation And Progress Report For Low-Energy Nuclear Physics Research At Lawrence Livermore National Laboratory

(I)In this project, the Beta-­decay Paul Trap, an open-­geometry RFQ ion trap that can be instrumented with sophisticated radiation detection arrays, is used for precision β-­decay studies. Measurements of β-­decay angular correlations, which are sensitive to exotic particles and other phenomena beyond the Standard Model (SM) of particle physics that may occur at the TeV-­energy scale, are being performed by taking advantage of the favorable properties of the mirror 8 Li and 8 B β ± decays and the benefits afforded by using trapped ions. By detecting the β and two α particles emitted in these decays, the complete kinematics can be reconstructed. This allows a simultaneous measurement of the β-­n, β-­n-­α, and β-α correlations and a determination of the neutrino energy and momentum event by event. In addition, the 8 B neutrino spectrum, of great interest in solar neutrino oscillation studies, can be determined in a new way. Beta-­delayed neutron spectroscopy is also being performed on neutron-­rich isotopes by studying the β-­decay recoil ions that emerge from the trap with high efficiency, good energy resolution, and practically no backgrounds. This novel technique is being used to study isotopes of mass-­number A~130 in the vicinity of the N=82 neutron magic number to help understand the rapid neutron-­capture process (r-­process) that creates many of the heavy isotopes observed in the cosmos. (II)A year-long CHICO2 campaign at ANL/ATLAS together with GRETINA included a total of 10 experiments, seven with the radioactive beams from CARIBU and three with stable beams, with 82 researchers involved from 27 institutions worldwide. CHICO2 performed flawlessly during this long campaign with achieved position resolution matching to that of GRETINA, which greatly enhances the sensitivity in the study of nuclear γ-­ray spectroscopy. This can be demonstrated in our results on 144 Ba and 146 Ba where the octupole deformation is evident from the measured B(E3; 3 - →0 + ) strengths that significantly greater than the theoretical predictions. We anticipate that CHICO2 will continue to be a viable charged-­particle detector for the research need of the low-­energy nuclear physics community.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2012

From the Lost Radium Files: Misadventures in the Absence of Training, Regulation, and Accountability

Purpose: Radium was the foundation of brachytherapy in the early decades of the 20th century. Despite being a most precious and perilous substance, it was mislaid with surprising frequency. This essay explores how it was lost, the efforts taken to recover it, and measures instituted to prevent mishandling. Methods and Materials: Review of contemporary literature, government publications, archives, and lay press. Results: Radium is a particularly dangerous substance because of its long half-life, its gaseous daughter (radon), and the high-energy emissions of its decay products. Despite the hazard, it was unregulated for most of the century. Any physician could obtain and administer it, and protocols for safe handling were generally lacking. Change came with appreciation of the danger, regulation, mandated training, and the institution of a culture of accountability. Unfortunately, careless management of medical radionuclides remains a global hazard. Conclusion: Responsible stewardship of radioactive material was not a high priority, for practitioners or the federal government, for much of the 20{sup th} century. As a result, large quantities of radium had gone astray, possibly subjecting the general public to continued radiation exposure. Lessons from the radium era remain relevant, as medical radionuclides are still mishandled.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2019

Observation of a $μs$ isomer in ${134\atop{49}}$ In $_{85}$: Proton-neutron coupling "southeast" of ${132\atop{50}}$ Sn $_{82}$

In this paper, we report on the observation of a microsecond isomeric state in the single-proton-hole, three-neutron-particle nucleus 134 In . The nuclei of interest were produced by in-flight fission of a 238 U beam at the Radioactive Isotope Beam Factory at RIKEN. The isomer depopulates through a γ ray of energy 56.7(1) keV and with a half-life of $T_{1/2}$ = 3.5 (4) $μs$. Based on the comparison with shell-model calculations, we interpret the isomer as the $I^π$ = 5 - member of the $π0g{-1\atop{9/2}}Ⓧv1f{3\atop{7/2}}$ multiplet, decaying to the $I^π$ = 7 - ground state with a reduced-transition probability of $B (E$ 2; 5 - $\rightarrow$ 7 - = 0.53 (6) W. u. Observation of this isomer, and lack of evidence in the current work for a $I^π$ = 5 - isomer decay in 132 In , provides a benchmark of the proton-neutron interaction in the region of the nuclear chart “southeast” of 132 Sn , where experimental information on excited states is sparse.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2016

Overview of PGSFR Project

The long-term plan for advanced SFR development was authorized by Korean Atomic Energy Commission (KAEC) in 2008 and updated in 2011, which will be carried out toward the construction of a SFR prototype plant called PGSFR (Prototype Gen-IV Sodium-cooled Fast Reactor) by 2028. The primary purpose of PGSFR is to demonstrate the technology reducing radioactive waste of spent nuclear fuel from nuclear power plants (NPP) in Korea. There are 24 NPPs in operation nationwide covering 30% of domestic electricity demand. The spent nuclear fuel is currently stored in the on-site storage pool of NPPs. Then, it has become a critical issue to ensure technical options to handle spent nuclear fuel in the long term basis to secure the sustainable operation of NPPs. PGSFR is a pool type sodium-cooled fast reactor with the power of 150 MWe or 400 MWth. PGSFR uses metallic fuel to make use of inherent safety characteristics of metallic fuel. The spent nuclear fuel will be processed using pyro-process to produce U-TRU-Zr fuel for PGSFR. But the initial core shall be loaded by low enriched U-Zr fuels. PGSFR has two intermediate loops with two intermediate heat exchangers (IHX) for each loop to deliver the generated heat from the core to power conversion system. There a steam generators producing super-heated steam in each loop. There are four decay heat removal circuits; two passive and two active ones. The reactor building is built on a seismic isolation base mat which can significantly mitigate seismic vibration of major components in the reactor building. The reactor building has a containment structure to isolate the reactor building under specific accident conditions and also provide structural integrity at the time of aircraft impact accident. PGSFR project is the national development program of Korea to construct the first SFR in Korea by 2028. The primary goal of PGSFR is the demonstration of reduction of radioactive waste from spent nuclear fuel by incineration in PGSFR. SFRA will flexibly cope with the licensing environment to minimize the uncertainty in licensing and safety concerns. The successful construction of PGSFR will bring Korean nuclear industry a step closer to guarantee the sustainable operation of NPPs nationwide and finally most importantly will solve the spent nuclear fuel issue of Korea. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2019

Radiological Performance Modeling: Platform Comparison

Zapadnoe Uranium Mill Tailings Site, Pridneprovsky Chemical Plant Ukraine: Two exposure scenarios were utilized to develop performance assessment models in GoldSim and NORMALYSA. The first scenario is an onsite worker exposed to radioactivity through external ground irradiation as well as radon and radioactive dust inhalation. The second being an offsite Resident 300 years after institutional control exposed through the ingestion of garden vegetables irrigated by contaminated ground water, ingestion of fish from Konoplyanka River, and agricultural activities in contaminated garden. NORMALYSA utilizes a modular interface to connect extensive pre-created modules to develop contaminant transport and risk assessment models for safety assessments and performance assessments at NORM and legacy sites. Developed by Facilia AB, the program was tested with the creation of the Zapadnoe model under the International Atomic Energy Agency MODARIA Il Working Group 1 (WG1). Default values are provided for input parameters where site specific data and distributions lack. Probabilistic simulations and inputs are limited to parameters with assigned Gaussian probability functions. Similar results for transient worker inhalation dose were found in comparison with the Zapadnoe GoldSim model. However, the NORMALYSA model has results larger by an order of magnitude for external radiation in the transient worker and for aquatic food ingestion, inhalation, and garden food ingestion to the resident. Performance Assessment Modeling: Radiological performance models promote good management and support in remediation and environmental decision making by optimizing radioactive waste disposal site performance. a performance assessment model of the Zapadnoe uranium mill tailings site and a model for calculating authorized limits at Los Alamos National Laboratory are created to demonstrate and highlight the respective capabilities of three modeling platforms: GoldSim, NORMALYSA, and RESRAD-Onsite. GoldSim is a general-purpose modeling platform with the ability to simulate site-specific FT radionuclide transport and risk assessment using a graphical interface to create and link elements that act as indivisible building blocks of the model. The Zapadnoe performance assessment model created in GoldSim is composed of input parameters collected from site specific parameters from WG1 as well as standard assumptions seen in the Generic PA Model from Neptune and Company. The multivariate Zapadnoe simulation contains both deterministic and probabilistic simulation capabilities with the ability to quantitatively represent the uncertainty and associated risks of the site via the Monte Carlo simulation method. Model parameters, documentation, and assumptions are built directly into the model creating a transparent, reproducible, and more purposeful site specific model. To demonstrate this, an ingestion of water pathway was included in addition to the exposure pathways included in the NORMALYSA model. GoldSim offers a wide variety of probability distributions to choose from as well as many tools to visualize the uncertainty of the models and explore which pathways and radionuclides dominate dose. In contrast to the NORMALYSA model, the GoldSim model uses dynamic simulation to calculate tritium concentrations. Authorized limits support the evaluation of radiological health effects from radionuclides present in bulk contaminated soil in order to assist in the process of clearing land for release under different uses. Calculations of authorized limits in RESRAD-Onsite and GoldSim models support the evaluation for 15 radionuclides using a residential exposure scenario, indoor and outdoor inhalation of dust and vapor phase radionuclides (tritium), incidental soil ingestion, and ingestion grown fruits and Vegetables. RESRAD-Onsite, developed by Argonne National Laboratory is a dedicated computer code for calculating radiation doses and cancer risks to an individual located on top of radioactively contaminated soils. It can also be used to provide guidelines for deriving radionuclide soil levels corresponding to a specific dose criterion. The menu driven user interface facilitates selection of radionuclides and soil concentrations, as well as defines parameter values related to materials, environmental factors, and exposure pathways. The program contains radionuclide-specific data such as dose conversion factors and risk coefficients, as well as soil-water partition coefficients and transfer factors for biotic media. The GoldSim model successfully emulates the RESRAD-Onsite code using identical radiological decay and ingrowth factors, radiation dose conversion factors, and other input parameters. DE EEDE ETS Each model supports dynamic modeling of radionuclide ingrowth and decay over time, and integrate this capability with the transport of radionuclides in the environment via processes such as advection and/or diffusion in fluids, or within porous solid media, The applicability of each program is heavily dependent on project context. In the context of developing Authorized Limits, RESRAD-Onsite may be a more desirable option as it was developed for this particular application. For simple disposal or legacy sites or sites that do not need site-specific model structure, NORMALYSA may be a desirable modeling platform, GoldSim can be used to model any problem for which RESRAD or NORMALYSA is applicable, but its strength lies in its flexibility, analytical, and probabilistic capabilities.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Effectiveness of actinide management in fast reactors over a finite recycling period - 15123

Long-lived nuclear waste primarily consists of transuranic (TRU) isotopes. Full recycling of TRU isotopes can, in theory, lead to a reduction in repository radiotoxicity to reference levels in as little as ∼500 years provided reprocessing and fuel fabrication losses are limited. However, over a limited time frame, the radiotoxicity of the 'final' core can dominate over reprocessing losses, leading to a much lower reduction in radiotoxicity compared to that achievable at equilibrium. In this paper, the fuel cycle code ORION is used to model the recycle of light water reactor (LWR)-produced TRUs in sodium-cooled fast reactors (SFRs). With full actinide recycling, at least 6 generations of SFRs are required in a gradual phase-out of nuclear power to achieve transmutation performance approaching the theoretical equilibrium performance. Break-even SFRs are much less effective from a point of view of reducing waste radiotoxicity. Thorium (Th)-burner fuel cycles are found to result in slightly lower radiotoxicity than U-burner fuel cycles for the same number of generations. Closed break-even Th fuel cycles require ∼3 generations of operation before their waste radiotoxicity benefits result in decay to the reference level in ∼1000 years, provided that Pa is recycled. While this is a very long time frame, it is substantially better than the time frame required by other strategies. The integrated decay heat over the scenario time frame is substantially higher for break-even Th-SFRs than break-even U-SFRs as a result of much higher {sup 90}Sr production. As decay heat affects repository sizing, this weakens the argument for the Th cycle. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Intrinsic electric quadrupole moment of the K π = 8 - isomeric state in Hf 178

The lifetime of the 9 - state in the rotational band based on the 4.0 s, K π = 8 - , isomeric state ( 178 Hf m 1 ) from the decay of the 31-yr isomer ( 178 Hf m 2 ) was determined to be 99(2) ps by means of the fast-timing technique using two LaBr 3 (Ce) scintillators. The δ (E2/M1) mixing ratios of the ΔI = 1 γ rays depopulating levels in this band were deduced from γ-γ angular correlations by using a 178 Hf m 2 radioactive source located at the center of the Gammasphere HPGe detector array. The new results, together with previous spectroscopic information, provide a different way to extract the intrinsic quadrupole moment of Q 0 = 6.45 (14) eb for the 178 Hf m 1 band. A possible explanation for the reduction of the 178 Hf m 1 nuclear charge radius is presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2019

Nuclear Considerations for the Application of Lanthanum Telluride in Future Radioisotope Power Systems

Thermoelectric-based radioisotope power systems (RPSs) produced in the United States convert the heat generated by the radioactive emission of alpha particles from plutonium dioxide ( 238 puO 2 ) into electricity by means of the Seebeck effect [1]. Certain designs for thermoelectric convertors propose the use of lanthanum telluride (La 3 Te 4 ) materials due to their significant conversion capabilities [2]. The generation of neutrons from spontaneous fission and alpha-neutron (α,n) reactions is also associated with the decay of 238 PuO 2 . A portion of these neutrons will interact with the thermoelectric materials and induce trace amounts of transmutation reactions in various lanthanum and tellurium isotopes. While very small quantities of several transmutation products are predicted, the most significant reaction channels are expected to produce trace amounts of iodine which will accumulate over time. Although iodine is classified as a halogen, it is the least reactive of the halogens, and as such, it is the most likely to be able to chemically convert back into the molecule I 2 . Since I 2 is a gas at RPS temperatures, it may be possible for iodine to attack other components in the thermoelectric cavity of an RPS system. Iodine reacts easily with metals to produce a wide variety of salts. This behavior could affect the performance of La 3 Te 4 thermoelectric devices, particularly the segmented architectures that include multiple sets of bonding and metallization layers. In this type of architecture, several segments of different thermoelectric materials are joined to increase the average thermoelectric figure of merit over a relatively large temperature gradient. It is plausible that sophisticated bonding/metallization layers could be required to join the segment interfaces to each other and to the cold- and hot-shoe materials. The long-term stability and performance of these segmented material combinations could degrade as a result of the potential formation and reactions of metal-iodide compounds at the segment interfaces. This paper (1) investigates the degree to which, if any, this process may threaten potential La 3 Te 4 thermoelectric technologies, (2) presents calculations of the amount of iodine generated over the operational life of a radioisotope thermoelectric generator design, and (3) discusses the potential effects of the resulting material's chemical reactions in a segmented couple-level architecture containing La 3 Te 4 . Conclusions drawn from combined particle transport, transmutation, and thermochemical calculations for La 3 Te 4 thermoelectric materials undergoing a notional 20-year mission scenario suggest that there is no significant potential for transmutation-induced thermoelectric (TE) performance degradation.

Smith, Michael↗
DOE OSTI2016

Gaseous time projection chambers for rare event detection: results from the T-REX project. I. Double beta decay

As part of the T-REX project, a number of R and D and prototyping activities have been carried out during the last years to explore the applicability of gaseous Time Projection Chambers (TPCs) with Micromesh Gas Structures (Micromegas) in rare event searches like double beta decay, axion research and low-mass WIMP searches. In both this and its companion paper, we compile the main results of the project and give an outlook of application prospects for this detection technique. While in the companion paper we focus on axions and WIMPs, in this paper we focus on the results regarding the measurement of the double beta decay (DBD) of {sup 136}Xe in a high pressure Xe (HPXe) TPC. Micromegas of the microbulk type have been extensively studied in high pressure Xe and Xe mixtures. Particularly relevant are the results obtained in Xe + trimethylamine (TMA) mixtures, showing very promising results in terms of gain, stability of operation, and energy resolution at high pressures up to 10 bar. The addition of TMA at levels of ∼ 1% reduces electron diffusion by up to a factor of 10 with respect to pure Xe, improving the quality of the topological pattern, with a positive impact on the discrimination capability. Operation with a medium size prototype of 30 cm diameter and 38 cm of drift (holding about 1 kg of Xe at 10 bar in the fiducial volume, enough to contain high energy electron tracks in the detector volume) has allowed to test the detection concept in realistic experimental conditions. Microbulk Micromegas are able to image the DBD ionization signature with high quality while, at the same time, measuring its energy deposition with a resolution of at least a ∼ 3% FWHM @ Q{sub ββ}. This value was experimentally demonstrated for high-energy extended tracks at 10 bar, and is probably improvable down to the ∼ 1% FWHM levels as extrapolated from low energy events. In addition, first results on the topological signature information (one straggling track ending in two blobs) show promising background discrimination capabilities out of reach of other experimental implementations. Moreover, microbulk Micromegas have very low levels of intrinsic radioactivity, and offer cost-effective scaling-up options. All these results demonstrate that Micromegas-read HPXe TPC remains a very competitive technique for the next generation DBD experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗