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Background identification in cryogenic calorimeters through $\alpha -\alpha$ delayed coincidences

Localization and modeling of radioactive contaminations is a challenge that ultra-low background experiments are constantly facing. These are fundamental steps both to extract scientific results and to further reduce the background of the detectors. Here we present an innovative technique based on the analysis of $\alpha -\alpha$ delayed coincidences in 232 Th and 238 U decay chains, developed to investigate the contaminations of the ZnSe crystals in the CUPID-0 experiment. This method allows to disentangle surface and bulk contaminations of the detectors relying on the different probability to tag delayed coincidences as function of the $\alpha$ decay position.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

MODELING OF THE GROUNDWATER TRANSPORT AROUND A DEEP BOREHOLE NUCLEAR WASTE REPOSITORY

The concept of disposal of high-level nuclear waste in deep boreholes drilled into crystalline bedrock is gaining renewed interest and consideration as a viable mined repository alternative. A large amount of work on conceptual borehole design and preliminary performance assessment has been performed by researchers at MIT, Sandia National Laboratories, SKB (Sweden), and others. Much of this work relied on analytical derivations or, in a few cases, on weakly coupled models of heat, water, and radionuclide transport in the rock. Detailed numerical models are necessary to account for the large heterogeneity of properties (e.g., permeability and salinity vs. depth, diffusion coefficients, etc.) that would be observed at potential borehole disposal sites. A derivation of the FALCON code (Fracturing And Liquid CONvection) was used for the thermal-hydrologic modeling. This code solves the transport equations in porous media in a fully coupled way. The application leverages the flexibility and strengths of the MOOSE framework, developed by Idaho National Laboratory. The current version simulates heat, fluid, and chemical species transport in a fully coupled way allowing the rigorous evaluation of candidate repository site performance. This paper mostly focuses on the modeling of a deep borehole repository under realistic conditions, including modeling of a finite array of boreholes surrounded by undisturbed rock. The decay heat generated by the canisters diffuses into the host rock. Water heating can potentially lead to convection on the scale of thousands of years after the emplacement of the fuel. This convection is tightly coupled to the transport of the dissolved salt, which can suppress convection and reduce the release of the radioactive materials to the aquifer. The purpose of this work has been to evaluate the importance of the borehole array spacing and find the conditions under which convective transport can be ruled out as a radionuclide transport mechanism. Preliminary results show that modeling of the borehole array, including the surrounding rock, predicts convective flow in the system with physical velocities of the order of 10-5 km/yr over 105 years. This results in an escape length on the order of kilometers, which is comparable to the repository depth. However, a correct account of the salinity effects reduces convection velocity and escape length of the radionuclides from the repository.

Modeling↗

Migration and Distribution of Natural Organic Matter Injected into Subsurface Systems - 16523

The Savannah River Site (SRS) was one of the major U.S. Department of Energy facilities that produced large amounts of radioactive and hazardous waste during the Cold War era, a legacy of material production for defense purposes. The unlined F-Area seepage basins received approximately 1.8 billion gallons of acidic waste solutions containing low-level radioactivity from numerous isotopes generated by uranium slug and irradiated fuel processing. Sufficient quantities of uranium isotopes, I-129, Tc-99, and tritium migrated into the groundwater, creating an acidic plume with a pH between 3 and 5.5. Humic substances (HS) are complex heterogeneous mixtures of poly-dispersed materials formed by biochemical and chemical reactions during the decay and transformation of plant and microbial remains. They are known for their excellent binding capacity for metals, making them a strong candidate for remediation efforts to reduce the mobility of uranium (VI) in the subsurface. Studies showed that HS are an important ion exchange and metal-complexing ligand, carrying a large number of functional groups with high complexing capacity that can greatly affect the mobility behavior of actinides in natural systems. Hence, it is a potential in situ amendment for treating groundwater contaminated with these constituents. Column experiments were conducted to address the complexities of HS in flow-through porous media representative of the acidic aquifer at the SRS F-Area Seepage Basins. The humate source used, Huma-K, is high in humic and fulvic compounds. The column studies were done using the soil obtained from SRS's FAW-1 core-hole at a depth interval of 60'-70'. A bromide tracer test was performed to obtain the pore volume (PV), variance and Peclet number. The columns were saturated with an artificial groundwater solution prepared to mimic the groundwater at SRS that was pH adjusted to 3.5 and 5 until the effluent pH reached equilibrium. Approximately one (1) PV of 5000 ppm of Huma-K was injected into the columns at 2 ml/min to study the sorption of Huma-K on the sediment. Desorption of Huma-K was studied by injecting approximately four (4) PVs of the pH adjusted artificial groundwater solution. A faster increase in pH was observed in column 1 (saturated with pH 3.5 AGW) compared to column 2 (saturated with pH 5 AGW). After injection of 2 PV of AGW, the pH of the columns reached 6.5 and 7, respectively, for columns 1 and 2. After injecting an additional PV of AGW, the pH remained relatively stable. With an increase in pH from 3.5 to 5.0, the overall retention of HA increased from 461 mg/kg for the column with pH 3.5 to 642 mg/kg for the column with pH 5. This suggests that retention is not due to adsorption alone, but adsorption coupled with precipitation and re-dissolution of Huma-K as it flows through the columns is a possible explanation for greater retention at pH 5. This negates the use of a simple Langmuir isotherm to explain humate behavior in the acidic environment of column 1. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Progress Toward Fast Decay Energy Spectroscopy for Actinide Analysis

Decay energy spectroscopy (DES) is an increasingly popular technique for measuring isotopic composition of actinide samples for nuclear safeguards applications. Current approaches for actinide DES utilize milligram-scale external gold absorbers (> 0.1 nJ/K) that are integrated with actinide samples through mechanical kneading and are thermally connected to microcalorimeters using indium or gold wire bonds. This leads to relatively slow sensor rise time and, consequently, limits counting speed to a few counts per second. We are developing faster metallic magnetic calorimeter-based DES by integrating actinide samples with magnetic sensor materials. This reduces signal rise time and enables high counting speed while maintaining the ability to knead the radioactive source with the absorber. We have measured signal rise time of 0.7 μs with a 1.5 mg external gold absorber using this approach. Here, we also demonstrated online DES operation using an Ortec DSPEC 50, a commercially available data acquisition system developed for semiconductor detectors.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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↗

The Past Informs the Future: An Overview of the Million Worker Study and the Mallinckrodt Chemical Works Cohort

The purpose of this paper is to present an overview of ongoing work on the Million Worker Study (MWS), highlighting some of the key methods and progress so far as exemplified by the study of workers at the Mallinckrodt Chemical Works (MCW). The MWS began nearly 25 y ago and continues in a stepwise fashion, evaluating one study cohort at a time. It includes workers from U.S. Department of Energy (DOE) Manhattan Project facilities, U.S. Nuclear Regulatory Commission (NRC) regulated nuclear power plants, industrial radiographers, U.S. Department of Defense (DoD) nuclear weapons test participants, and physicians and technologists working with medical radiation. The purpose is to fill the major gap in radiation protection and science: What is the risk when exposure is received gradually over time rather than briefly as for the atomic bomb survivors? Studies published or planned in 2018 include leukemia (and dosimetry) among atomic veterans, leukemia among nuclear power plant workers, mortality among workers at the MCW, and a comprehensive National Council on Radiation Protection and Measurements (NCRP) Report on dosimetry for the MWS. MCW has a singular place in history: the 40 tons (T) of uranium oxide produced at MCW were used by Enrico Fermi on 2 December 1942 to produce the first manmade sustained and controlled nuclear reaction, and the atomic age was born. Seventy-six years later, the authors followed the over 2,500 MCW workers for mortality and reconstructed dose from six sources of exposure: external gamma rays from the radioactive elements in pitchblende; medical x rays from occupationally required chest examinations; intakes of pitchblende (uranium, radium, and silica) measured by urine samples; radon breath analyses and dust surveys overseen by Robley Evans and Merril Eisenbud; occupational exposures received before and after employment at MCW; and cumulative radon concentrations and lung dose from the decay of radium in the work environment. The unique exposure reconstructions allow for multiple evaluations, including estimates of silica dust. The study results are relevant today. For example, NASA is interested that radium, deposited in the brain, releases high-LET alpha particles - the only human analogue, though limited, for high energy, high-Z particles (galactic cosmic rays) traveling through space that might affect astronauts on Mars missions. In conclusion, don’t discount the past; it’s the prologue to the future!

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Electromagnetic backgrounds and potassium-42 activity in the DEAP-3600 dark matter detector

The DEAP-3600 experiment is searching for weakly interacting massive particles dark matter with a 3.3 × 10 3 kg single phase liquid argon (LAr) target, located 2.1 km underground at SNOLAB. The experimental signature of dark matter interactions is kilo electron volt–scale 40 Ar nuclear recoils producing 128 nm LAr scintillation photons observed by photomultiplier tubes. The largest backgrounds in DEAP-3600 are electronic recoils (ERs) induced by β and γ rays originating from internal and external radioactivity in the detector material. A background model of the ER interactions in DEAP-3600 was developed and is described in this work. The model is based on several components which are expected from radioisotopes in the LAr, from ex situ material assay measurements, and from dedicated independent in situ analyses. This prior information is used in a Bayesian fit of the ER components to a 247.2 d dataset to model the radioactivity in the surrounding detector materials. Pulse-shape discrimination separates ER and NR events. However, detailed knowledge of the ER background and activity of detector components sets valuable constraints on NR backgrounds including neutrons and alphas. In addition, the activity of 42 Ar in LAr in DEAP-3600 is determined by measuring the daughter decay of 42 K. Finally, this cosmogenically activated trace isotope is a relevant background at higher energies for other rare event searches using atmospheric argon, e.g., DarkSide-20k, GERDA, or LEGEND. The specific activity of 42 Ar in the atmosphere is found to be 40.4 ± 5.9 μ Bq/kg of argon.

79 ASTRONOMY AND ASTROPHYSICS↗

MCNP Intrinsic Source Constructor (MISC): A User’s Guide

The MCNP Intrinsic Source Constructor (MISC) facilitates the construction of MCNP source definition cards for radioactive materials. Given a material nuclide specification, either weight or atom fractions of those nuclides, and either a weight or atom density of the material, MISC will construct the source spectrum distribution of a specified particle type. MISC also calculates the absolute number of particles emitted per second per unit mass or volume. Furthermore, if decay chain information is available in the data sets selected by the user, the initial isotopes specified by the user can be approximately decayed to the resulting isotopes after a specified amount of time.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Improving Fission Products at CARIBU (NA-22 Final Report)

Detailed knowledge of fission-product (FP) decay properties is needed for a variety of applications of nuclear science such as nuclear-energy production, nuclear-nonproliferation efforts, nuclear-forensics assessments, and stockpile stewardship, as well as for establishing a comprehensive understanding of the fission process, r-process nucleo-synthesis, and fundamental neutrino science. Although nearly a thousand radioactive isotopes are produced in fission, in many cases key pieces of nuclear data on only a handful of isotopes are needed to make a significant impact.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Hadronic nuclear energy: An approach towards green energy

Nuclear energy is undoubtedly the largest energy source capable of meeting the total energy requirements to a large extent in long terms. However the conventional nuclear energy involves production of high level of radioactive wastes which possesses threat, both to the environment and mankind. The modern day demand of clean, cheap and abundant energy gets fulfilled by the novel fuels that have been developed through hadronic mechanics/chemistry. In the present paper, a short review of Hadronic nuclear energy by intermediate controlled nuclear synthesis and particle type like stimulated neutron decay and double beta decay has been presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Development of an underground HPGe array facility for ultra low radioactivity measurements

Low Level Counting techniques using low background facilities are continuously under development to increase the possible sensitivity needed for rare physics events experiments. The CUP (Center for Underground Physics) group of IBS is developing, in collaboration with Canberra, a ultra low background instrument composed of two arrays facing each other with 7 HPGe detectors each. The low radioactive background of each detector has been evaluated and improved by the material selection of the detector components. Samples of all the building materials have been provided by the manufacturer and the contaminations had been measured using an optimized low background 100% HPGe with a dedicated shielding. The evaluation of the intrinsic background has been performed using MonteCarlo simulations and considering the contribution of each material with the measured contamination. To further reduce the background, the instrument will be placed in the new underground laboratory at YangYang exploiting the 700m mountain coverage and radon-free air supplying system. The array has been designed to perform various Ultra Low background measurements; the sensitivity we are expecting will allow not only low level measurements of Ra and Th contaminations in Copper or other usually pure materials, but also the search for rare decays. In particular some possible candidates and configurations to detect the 0νECEC (for example {sup 106}Cd and {sup 156}Dy) and rare β decays ({sup 96}Zr, {sup 180m}Ta , etc ) are under study.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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↗

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↗

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 ↗

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↗

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↗

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↗

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↗