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DOE OSTI2023

Evaluation of SNOLAB background mitigation procedures through the use of an ICP-MS based dust monitoring methodology

Dust particulate fallout on materials in use for rare-event searches is a concerning source of radioactive backgrounds due to the presence of the naturally occurring radionuclides 40 K, 232 Th, 238 U, and their progeny in dust. Much effort is dedicated to inform radioactive backgrounds from dust and evaluate the efficacy of mitigation procedures. A great portion of such effort relies on fallout models and assumed dust composition. Here, in this work, an ICP-MS based methodology was employed for a direct determination of fallout rates of radionuclides and stable isotopes of interest from dust particulate at the SNOLAB facility. Hosted in an active mine, the SNOLAB underground laboratory strives to maintain experimental areas at class 2000 cleanroom level. This work validates the mitigation procedures in place at SNOLAB and informs dust backgrounds during laboratory activities. Fallout rates of major constituents of the local rock were measured two to three orders of magnitude lower in the clean experimental areas compared to non-clean transition areas from the mine to the laboratory. An increase of approximately two orders of magnitude in the fallout rate of stable Pb isotopes was determined in an experimental area during activities involving handling of Pb bricks. Increased 40 K, 232 Th, and 238 U fallout rates were measured in clean experimental areas during activities generating particulate.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Highly charged ion approach to measure nuclear charge radii of Fr, Ra, and Rn isotopes for precision measurements

Conventional electron scattering and muonic atom spectroscopy techniques are challenging to apply to heavy ions unless the element has at least one stable or extremely long-lived isotope. To overcome this limitation, a recently introduced method for determining nuclear charge radii relies on extreme-ultraviolet (EUV) spectroscopy of the D 1 line in highly charged Na-like ions. In this work, we present an experimental approach to measure the nuclear charge radii of isotopes of radioactive elements such as Fr, Ra, and Rn using this method at TRIUMF’s Ion Trap for Atomic and Nuclear Science (TITAN) instrument, located at the ISAC radioactive beam facility. We also explore the potential of using Na-like D 2 lines in the soft x-ray region for future measurements.

Electron beam ion trap↗

DOE OSTI2024

Ceramic–Metal (Cermet) Composites: A Review of Key Properties and Synthesis Methods Focused on Nuclear Waste Immobilization

Here this paper reviews key properties, applications, and examples of ceramic-metal composites (cermets), and metal matrix composites (MMC) with emphasis on their applicability as waste forms for immobilizing nuclear waste. While the literature is mature for vitrified and cementitious radioactive waste forms, cermet materials have not received adequate attention as potential candidates for immobilizing nuclear waste. To promulgate this effort, this review connects cermet and MMC design, such as hardened tools, with the chemistry of radioactive waste streams. A discussion on certification and qualification standards for cermet waste forms, literature gaps, and “how-to” sections on cermet processing techniques. Key parameters discussed include thermal conductivity, chemical durability, and waste loading, as well as examples for metal-containing waste forms. As cermet waste forms gain momentum within the community, this review paper aims ensure the end-of-life nuclear fuel cycle is addressed from a materials and waste disposition perspective.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Electrical Resistivity Changes During Heating Experiments Unravel Heterogeneous Thermal‐Hydrological‐Mechanical Processes in Salt Formations

Abstract Rock salt is considered a suitable medium for the permanent disposal of heat‐generating radioactive waste due to its isolation properties. However, excavation damage and heating induce complex and heterogeneous thermal‐hydrological‐mechanical (THM) processes across different zones. Quantifying this heterogeneity is crucial for accurate long‐term performance assessment models, but traditional methods lack the necessary resolution. This study employs 4D electrical resistivity tomography (ERT) monitoring during controlled heating experiments in a salt formation to unravel the spatiotemporal dynamics of THM processes. Advanced time‐lapse inversion and clustering analysis quantify subsurface properties and map the heterogeneity of THM dynamics. The ERT results can estimate subsurface properties and delineate the damaged and intact zones, enabling appropriate parameterization and representation of processes for long‐term modeling. This approach may be used in further improving the predictive models and ensuring the safe long‐term disposal of radioactive waste in rock salt.

58 GEOSCIENCES↗

DOE OSTI2025

Electron correlation and relativistic effects in the excited states of radium monofluoride

Highly accurate and precise electronic structure calculations of heavy radioactive atoms and their molecules are important for several research areas, including chemical, nuclear, and particle physics. Ab initio quantum chemistry can elucidate structural details in these systems that emerge from the interplay of relativistic and electron correlation effects, but the large number of electrons complicates the calculations, and the scarcity of experiments prevents insightful theory-experiment comparisons. Here we report the spectroscopy of the 14 lowest excited electronic states in the radioactive molecule radium monofluoride (RaF), which is proposed as a sensitive probe for searches of new physics. The observed excitation energies are compared with state-of-the-art relativistic Fock-space coupled cluster calculations, which achieve an agreement of ≥99.64% (within ~12 meV) with experiment for all states. Guided by theory, a firm assignment of the angular momentum and term symbol is made for 10 states and a tentative assignment for 4 states. The role of high-order electron correlation and quantum electrodynamics effects in the excitation energies is studied and found to be important for all states.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Urban working groups in the IAEA’s model testing programmes: overview from the MODARIA I and MODARIA II programmes

The IAEA’s model testing programmes have included a series of Working Groups concerned with modelling radioactive contamination in urban environments. These have included the Urban Working Group of Validation of Environmental Model Predictions (1988–1994), the Urban Remediation Working Group of Environmental Modelling for Radiation Safety (EMRAS) (2003–2007), the Urban Areas Working Group of EMRAS II (2009–2011), the Urban Environments Working Group of (Modelling and Data for Radiological Impact Assessments) MODARIA I (2013–2015), and most recently, the Urban Exposures Working Group of MODARIA II (2016–2019). The overarching objective of these Working Groups has been to test and improve the capabilities of computer models used to assess radioactive contamination in urban environments, including dispersion and deposition processes, short-term and long-term redistribution of contaminants following deposition events, and the effectiveness of various countermeasures and other protective actions, including remedial actions, in reducing contamination levels, human exposures, and doses to humans. This paper describes the exercises conducted during the MODARIA I and MODARIA II programmes. These exercises have included short-range and mid-range atmospheric dispersion exercises based on data from field tests or tracer studies, hypothetical urban dispersion exercises, and an exercise based on data collected after the Fukushima Daiichi accident. We report improvement of model capabilities will lead to improvements in assessing various contamination scenarios (real or hypothetical), and in turn, to improved decision-making and communication with the public following a nuclear or radiological emergency.

61 RADIATION PROTECTION AND DOSIMETRY↗

DOE OSTI2025

Development of a military-specific mesh-type computational phantom library and its application to internal dosimetry and in-field radiological triage screening

Estimates of organ-absorbed and committed doses to individuals exposed to radioactive materials via acute inhalation often rely on internal dose coefficients and detector responses from reference human computational models. To achieve more accurate dose assessments to United States Armed Forces service members exposed in-field, computational models with varying morphometric parameters representative of this population are necessary. The International Commission on Radiological Protection (ICRP) Publication 145 provides detailed mesh reference computational phantoms (MRCPs) for adult males and females, with morphometric parameters matched to the 50th percentile. Previously, these phantoms were 2D and 3D scaled to match desired height, mass, and secondary anthropomorphic parameters in the creation of the University of Florida / Memorial Sloan Kettering (UF/MSK) computational phantom library. To achieve body fat percentage targets required for accession into the US Armed Forces, muscle and fat volumes were adjusted accordingly, thus, creating the UF/Department of Defence computational phantom library presented in this study. A comprehensive library of mesh-type computational human phantoms was created, including 57 adult males and 49 adult females with morphometric parameters aligned with United States Armed Forces service members. Phantoms were restricted to a body mass index between 19 and 27.5, with body fat percentages below 26% for males and 36% for females. Specific absorbed fractions were computed for selected source and target combinations, demonstrating how variations in height and body mass influence energy absorption in target regions relative to the ICRP MRCPs. Radiation detector responses were also computed, revealing that higher body masses resulted in decreased registered counts in the detection volume. These findings highlight the importance of incorporating morphometric variability in computational phantoms to achieve more accurate dose assessments and radiation detection responses for United States Armed Forces service members who inhale radioactive materials in-field.

computational phantoms↗

DOE OSTI2024

Studying microbially induced corrosion on glass using ToF-SIMS

Microbially induced corrosion (MIC) is an emerging topic that has huge environmental impacts, such as long-term evaluation of microbial interactions with radioactive waste glass, environmental cleanup and disposal of radioactive material, and weathering effects of microbes. Time-of-flight secondary ion mass spectrometry (ToF-SIMS), a powerful mass spectral imaging technique with high surface sensitivity, mass resolution, and mass accuracy, can be used to study biofilm effects on different substrates. Understanding how to prepare biofilms on MIC susceptible substrates is critical for proper analysis via ToF-SIMS. We present here a step-by-step protocol for preparing bacterial biofilms for ToF-SIMS analysis, comparing three biofilm preparation techniques: no desalination, centrifugal spinning (CS), and water submersion (WS). Comparisons of two desalinating methods, CS and WS, show a decrease in the media peaks up to 99% using CS and 55% using WS, respectively. Proper desalination methods also can increase biological signals by over four times for fatty acids using WS, for example. ToF-SIMS spectral results show chemical compositional changes of the glass exposed in a Paenibacillus polymyxa SCE2 biofilm, indicating its capability to probe microbiologically induced corrosion of solid surfaces. This represents the proper desalination technique to use without significantly altering biofilm structure and substrate for ToF-SIMS analysis. ToF-SIMS spectral results showed chemical compositional changes of the glass exposed by a Paenibacillus bacterial biofilm over 3-month inoculation. Finally, possible MIC products include various phosphate phase molecules not observed in any control samples with the highest percent increases when experimental samples were compared with biofilm control samples.

36 MATERIALS SCIENCE↗

DOE OSTI2024

EMP, Attachment 2: Data Management Plan

This Data Management Plan (DMP) is an attachment to the Pacific Northwest National Laboratory Environmental Radiological Air Monitoring Plan (EMP). PNNL is a U.S. Department of Energy Office of Science national laboratory. Radioactive effluent monitoring and environmental surveillance for PNNL operations in Washington State are the responsibility of the PNNL Environmental Protection and Regulatory Programs division and are conducted by the Environmental Radiation Task staff. This DMP describes the data management processes for PNNL radioactive air emissions (stack) monitoring and environmental radiological ambient air surveillance activities.

40 CFR 61 Subpart H↗

DOE OSTI2022

Origin of Plutonium-244 in the Early Solar System

We investigate the origin in the early Solar System of the short-lived radionuclide 244 Pu (with a half life of 80 Myr) produced by the rapid (r) neutron-capture process. We consider two large sets of r-process nucleosynthesis models and analyse if the origin of 244 Pu in the ESS is consistent with that of the other r and slow (s) neutron-capture process radioactive nuclei. Uncertainties on the r-process models come from both the nuclear physics input and the astrophysical site. The former strongly affects the ratios of isotopes of close mass ( 129 I/ 127 I, 244 Pu/ 238 U, and 247 Pu/ 235 U). The 129 I/ 247 Cm ratio, instead, which involves isotopes of a very different mass, is much more variable than those listed above and is more affected by the physics of the astrophysical site. We consider possible scenarios for the evolution of the abundances of these radioactive nuclei in the galactic interstellar medium and verify under which scenarios and conditions solutions can be found for the origin of 244 Pu that are consistent with the origin of the other isotopes. Solutions are generally found for all the possible different regimes controlled by the interval (δ) between additions from the source to the parcel of interstellar medium gas that ended up in the Solar System, relative to decay timescales. If r-process ejecta in interstellar medium are mixed within a relatively small area (leading to a long δ), we derive that the last event that explains the 129 I and 247 Cm abundances in the early Solar System can also account for the abundance of 244 Pu. Due to its longer half life, however, 244 Pu may have originated from a few events instead of one only. If r-process ejecta in interstellar medium are mixed within a relatively large area (leading to a short δ), we derive that the time elapsed from the formation of the molecular cloud to the formation of the Sun was 9-16 Myr.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Annual Summary Report for the Remote-Handled Low-Level Waste Disposal Facility—FY 2024

This Fiscal Year (FY) 2024 annual summary report (ASR) documents the continued adequacy of the performance assessment (PA), the composite analysis (CA), and associated operating disposal- authorization statement (ODAS) technical-basis documents for the Remote-Handled (RH) Low-Level Waste (LLW) Disposal Facility at Idaho National Laboratory (INL). Annual review of the adequacy of the PA and CA for the Remote-Handled Low-Level Waste (RHLLW) Disposal Facility ensures that conclusions of the analyses remain valid in accordance with requirements of Department of Energy (DOE) Order 435.1, “Radioactive Waste Management.” In FY 2024, no significant operational changes or other activities occurred that would cause deviation from the assumptions in the PA and CA pertaining to disposal geometry, verification of waste characteristics, tracking disposal inventories against total limits, facility-closure design, or institutional controls. Nineteen waste canister shipments were received at the RHLLW Disposal Facility, and all nineteen waste canisters were emplaced in disposal vaults.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗

DOE OSTI1989

Nuclear Safety [Vol. 30, No. 1, January-March 1989]

Nuclear Safety is a review journal that covers significant developments in the field of nuclear safety. Its scope includes the analysis and control of hazards associated with nuclear energy, operations involving fissionable materials, and the products of nuclear fission and their effects on the environment. Primary emphasis is on safety in reactor design, construction, and operation; however, the safety aspects of the entire fuel cycle, including fuel fabrication, spent-fuel processing, nuclear waste disposal, handling of radioisotopes, and environmental effects of these operations, are also treated. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 1 International Conference on Thermal Reactor Safety: NUCSAFE 88 by A. P. Malinauskas and J. G. Pruett; ACCIDENT ANALYSIS: 18 Chernobyl Today: State of Research by A. Yu. Gagarinskii; CONTROL AND INSTRUMENTATION: 23 Problems Associated with Routine In-Plant Radioactive Effluent Monitoring Systems at U.S. Light-Water Reactors by Barry G. Wahlig, David M. Walker, Mahmoud R. Ghavi, and John M. Palms; DESIGN FEATURES: 34 Twentieth DOE/NRC Nuclear Air-Cleaning Conference by R. R. Bellamy, D. W. Moeller, and M. W. First, 46 Design Options for the Core Support Structure for Liquid-Metal-Cooled Reactor Plants by J. P. Burelbach, W. J. Kann, J. G. Saiveau, and R. W. Seidensticker; ENVIRONMENTAL EFFECTS: 53 The Radiological Consequences of the Chernobyl Accident by L. V. Konstantinov and A. J. González; WASTE AND SPENT FUEL MANAGEMENT: 70 Activities Related to Waste Management Compiled by E. G. Silver; OPERATING EXPERIENCES: 80 Fuel Performance Annual Report for 1986 by W. J. Bailey, 103 Safety Considerations Related to 12-Hour Shift Schedules by S. Gould, 105 Reactor Shutdown Experience Compiled by J. W. Cletcher, 108 Operating U.S. Power Reactors Compiled by E. G. Silver; RECENT DEVELOPMENTS: 130 General Administrative Activities Compiled by E. G. Silver, 140 Reports, Standards, and Safety Guides by D. S. Queener, 145 Status of Power-Reactor Licensing Activities Compiled by E. G. Silver, 153 Proposed Rule Changes as of Sept. 30, 1988; ANNOUNCEMENTS: 69 Northwestern University Short Course on Radiation Safety, 79 International Seminar on Fission Product Transport Processes in Reactor Accidents, 129 Harvard School of Public Health Offers Short Courses, 152 MIT Offers Summer Short Courses on Reactor Safety and Nodal Analysis, 152 Seminar on Use of PCs in Probabilistic Safety Analysis, 157 The Authors, 160 Indexes to Nuclear Safety, Volume 29.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Review of the Safety Analyses of the Konrad Repository - 20530

The Bundesgesellschaft fuer Endlagerung (BGE) is the license holder of all geological repository sites in Germany since 2017. Besides the construction of the Konrad repository for the emplacement of low- and intermediate-level waste (LILW), the operation of the Asse II mine including the retrieval of the emplaced waste, and the preparation for the closure of the Morsleben repository, BGE is responsible to carry out the operative tasks of selecting a site for a high-level waste (HLW) repository. The Konrad repository is Germany's first repository for radioactive waste with negligible heat generation, which was fully licensed under atomic law within the scope of a plan approval procedure from the original application in 1982 until the license was granted in 2002 and finally confirmed by the Federal Administrative Court in 2007. The emplacement of LILW was licensed up to a volume of 303,000 m{sup 3} with a total β/γ-activity of 5 x 10{sup 18} Bq and a total α-activity of 1.5 x 10{sup 17} Bq. Currently, the former iron ore mine Konrad is being converted to a repository and is expected to come into operation in 2027. But what if there is no safety case in place nor a regulatory framework tailored for a change of documents in order to ensure the safety according to the state-of-the-art of science and technology during the evolution of a long-term project such as a geological repository? In this presentation, a review procedure of the safety analyses, that have been the basis of the plan approval decision for the Konrad repository at that time, will be described. Furthermore, the first results of this graduated review procedure for updating the safety analyses will be presented. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Heavy Elements and Electromagnetic Transients from Neutron Star Mergers

Compact binary mergers involving neutron stars can eject a fraction of their mass to space. Being extremely neutron rich, this material undergoes rapid neutron capture nucleosynthesis, and the resulting radioactivity powers fast, short-lived electromagnetic transients known as kilonova or macronova. Such transients are exciting probes of the most extreme physical conditions and their observation signals the enrichment of the Universe with heavy elements. Here the current understanding of the mass ejection mechanisms, the properties of the ejecta, and the resulting radioactive transients are reviewed. The first well-observed event in the aftermath of GW170817 delivered a wealth of insights, but much of today's picture of such events is still based on a patchwork of theoretical studies. Apart from summarizing the current understanding, questions where no consensus has been reached yet are also pointed out, and possible directions for the future research are sketched. In an appendix, a publicly available heating rate library based on the WinNet nuclear reaction network is described, and a simple fit formula to alleviate the implementation in hydrodynamic simulations is provided.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

A History of Hanford Tank Waste, Implications for Waste Treatment and Disposal

More than 40 years of plutonium processing have left almost 56 million gallons of mixed radioactive waste sequestered in 177 underground tanks on the Hanford Site. Three different processing technologies were employed for plutonium purification in addition to uranium scavenging and fission product removal from the tank waste. All of these chemical processes have contributed to a complex waste stream that varies from tank to tank that presents downstream processing challenges to render the waste into a safe form for long-term storage. The current disposition pathway for Hanford tank waste is vitrification. To maximize waste loading and minimize the number of high-level waste canisters stored in a geologic repository, pretreatment of the waste is required. Both pretreatment and vitrification operations are impacted by the waste composition.

Separations, filtration, ion exchange↗

DOE OSTI2022

Implications of Underground Nuclear Explosion Cavity Evolution for Radioxenon Isotopic Composition

Abstract Isotopic ratios of radioxenons sampled in the atmosphere or subsurface can be used to verify the occurrence of an underground nuclear explosion (UNE). Differences in the half-lives of radioactive xenon precursors and their decay-chain networks produce different time-dependent concentration profiles of xenon isotopes allowing isotopic ratios to be used for tracking UNE histories including estimating the time of detonation. In this study, we explore the potential effects of post-detonation cavity processes: precipitation of iodine precursors, gas seepage, and prompt venting on radioxenon isotopic evolution which influences UNE histories. Simplified analytical models and closed-form solutions yielding a potentially idealized radioactive decay/ingrowth chain in a closed and well-mixed system typically have limited application by not including the partitioning of the radionuclide inventory between a gas phase and rock melt created by the detonation and by ignoring gas transport from the cavity to host rock or ground surface. In reality, either subsurface transport or prompt release that is principally responsible for gas signatures violates the closed-system (or batch-mode) assumption. A closed-form solution representing time-dependent source-term activities is extended by considering the cavity partitioning process, slow seepage, and/or prompt release of gases from the cavity and applied to realistic systems.

Sun, Yunwei (ORCID:0000000194801439)↗

DOE OSTI2023

Impact of environmental backgrounds on atmospheric monitoring of nuclear explosions

Radionuclide monitoring for nuclear explosions includes measuring radioactive aerosol and noble gas concentrations in the atmosphere. The International Monitoring System (IMS) of the Comprehensive Nuclear Test Ban Treaty (CTBT) has made such measurements for decades, revealing much about how atmospheric radioactivity impacts the sensitivity of the network. For example, civilian emissions of radioiodine make a substantial regional impact, but a minor global impact, while civilian radioxenon emissions create major regional and complex global impacts. This example statement is strongly influenced by the minimum signal level anticipated to be interesting. The original design of the IMS anticipated relatively large signal levels, and the accomplished IMS network substantially meets or exceeds the sensitivity needed to detect those signal levels. Much lower signal levels can be motivated, which could require reconsideration of station sensitivity. Using measured and simulated background concentrations, various possible desired signal levels, and an innovative anomaly threshold, maps of sensitivity and a station ranking are developed for current and future stations. These provide a strong motivation for additional experimentation to learn about sources and the potential plusses of new technology.

Eslinger, Paul W.↗

DOE OSTI2025

Comparison of microprecipitation methods for polonium source preparation for alpha spectrometry

Detection of radioactive isotopes of polonium is important for understanding natural processes, management and assessment of radioactive waste, and nuclear forensics applications. Further, the most common methods for preparation of polonium samples for alpha spectrometry are electrodeposition and spontaneous deposition which are time consuming. Here, we compare three approaches utilizing rapid microprecipitation from bismuth phosphate, copper sulfide, or tellurium alongside traditional spontaneous deposition methods. From these experiments, results show that copper sulfide microprecipitation recoveries are similar to spontaneous deposition on silver and less time consuming with an approximate five-fold decrease in preparation time, including in the presence of complex matrices like seawater.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗