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DOE OSTI2021

Development of an Activation Analysis Methodology to Support the Disposal of the High Flux Isotope Reactor Metal Pool Waste

During operation and maintenance of the High Flux Isotope Reactor (HFIR), metal waste from reactor components is generated. Due to space limitations in the pool fuel storage, it is necessary to remove the waste and send it to off-site disposal. Most of this waste was in the reactor and is radioactive through neutron activation. Prior to shipping and disposal at a waste disposal facility, the radiological activity of the waste must be determined. Therefore, a conservative methodology to characterize the radiological activity of the waste must be performed. The methodology used was based on being able to determine a conservative overall activity and radionuclide inventory based on radiological survey data and neutron activation products for the materials present.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Recent 238 Pu Production Activities at Idaho National Laboratory

The Plutonium-238 ( 238 Pu) Production program at Idaho National Laboratory (INL) is actively qualifying irradiation targets containing 237 Np for the Advanced Test Reactor (ATR) to produce 238 Pu for future National Aeronautics and Space Administration missions. INL qualified and loaded seven targets in the ATR’s south flux trap for cycle 169A, which occurred in Spring 2021. The irradiation qualification program has expanded to additional ATR irradiation positions after two baseline production targets in three positions validated significant production of 238 Pu. The validation model was followed by the PFS-1 experimental test in the ATR Critical Facility that verified 238 Pu production cross sections. This paper outlines the progress and status of the 238 Pu production program at INL. The qualification effort, safety analysis, hardware status, and future activities for qualification of an updated target design for use in the ATR are discussed.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2020

Performance Improvements on SNS and HFIR Instrument Data Reduction Workflows Using Mantid

Performance of data reduction workflows at the High Flux Isotope Reactor (HFIR) and the Spallation Neutron Source (SNS) at Oak Ridge National Laboratory (ORNL) is mainly determined by the time spent loading raw measurement events stored in large and sparse datasets. This paper describes: (1) our long-term view to leverage SNS and HFIR data management needs with our experience at ORNL’s world-class high performance computing (HPC) facilities, and (2) our short-term efforts to speed up current workflows using Mantid, a data analysis and reduction community framework used across several neutron scattering facilities. We show that minimally invasive short-term improvements in metadata management have a moderate impact in speeding up current production workflows. We propose a more disruptive domain-specific solution: the No Cost Input Output (NCIO) framework, we provide an overview, the risks and challenges in NCIO’s adoption by HFIR and SNS stakeholders.

Godoy, William↗

DOE OSTI2024

Target development using the method of High-Intensity Vibrational Powder Plating (HIVIPP) at the Center for Accelerator Target Science (CATS) at Argonne National Laboratory (ANL)

One of the primary goals of the Center for Accelerator Target Science (CATS) is to provide targets and foils in support of the ATLAS User Facility and the Low-Energy community at large. While a wide array of target production techniques are available at CATS, new methods that must be explored invariably arise. One such technique, the High-Intensity Vibrational Powder Plating (HIVIPP), was first reported in 1997 by Isao Sugai. It was developed to produce targets and stripper foils that were difficult to make by standard methods. At Argonne National Laboratory (ANL), we have successfully constructed and tested a simple system for this purpose. We have produced targets of carbon and titanium on various metal backings using the HIVIPP method. We are currently in the exciting phase of exploring the production of other elements, including isotopically enriched and radioactive material. This work is in progress and will be further detailed with specific examples.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Cross-Section Comparison for Pu-238 Production in the Advanced Test Reactor at Idaho National Laboratory

Qualification of Advanced Test Reactor (ATR) positions for Pu-238 production has been ongoing at Idaho National Laboratory (INL). The ATR qualifications have stretched over multiple years during which new techniques have been developed and made available for ATR experiment neutronic analysis. As part of the transition to newer codes, new cross-section libraries have been evaluated for use in the Pu-238 production experiment analysis. A comparative study was done using the MCNP ORGIEN Activation Analysis (MOAA) tool between ENDF/B-VII.0 and ENDF/B-VIII.0 cross sections to capture the impact of the change in cross-sections on the analysis needed to qualify Pu-238 production targets. All comparisons were done assuming the ATR GEN-I targets were located in the south flux trap of the ATR. Finally, an overview of how this qualification and potential irradiation fits into Pu-238 is discussed.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2025

Extraction of the non-spin- and spin-transfer isovector responses via the 12 C ⁡( 10 Be, 10 B + 𝛾)⁢ 12 B reaction

The isovector response in 12 B was investigated via the 12 C ⁡( 10 Be, 10 B + 𝛾)⁢ 12 B* reaction at 100⁢𝐴MeV. By utilizing the 𝛾-decay properties of the 1.74 MeV 0 + and 0.718 MeV 1 + states in 10 B, the separate extraction of the non-spin-transfer (Δ⁢𝑆 = 0) and spin-transfer (Δ⁢𝑆 = 1) isovector responses up to an excitation energy of 50 MeV in 12 B in a single measurement is demonstrated. The experimental setup employed the S800 spectrometer to detect and analyze the 10 B ejectiles and the Gamma-Ray Energy Tracking In-beam Nuclear Array (GRETINA) for obtaining the Doppler-reconstructed spectrum for 𝛾 rays emitted in flight by 10 B. A 12 C foil was placed at the pivot point of the spectrograph. Here, the 12 B reaction product was not detected. Contributions from transitions associated with the transfer of different units of angular momentum in the non-spin- and spin-transfer responses were analyzed using a multipole decomposition analysis. The extracted non-spin-dipole (Δ⁢𝑆 = 0, Δ⁢𝐿 = 1) and spin-dipole (Δ⁢𝑆 = 1, Δ⁢𝐿 = 1) responses were found to be consistent with available data from other charge-exchange probes, validating the non-spin- and spin-transfer filters used. While statistical uncertainties and experimental resolutions were relatively large due to the modest intensity of the 10 Be secondary beam, the results show that, with the much higher intensities that will be available at new rare-isotope beam facilities, the ( 10 Be, 10 B + 𝛾) reaction and its Δ⁢𝑇 𝑧 = −1 partner, the ( 10 C, 10 B + 𝛾) reaction, are powerful tools for elucidating the isovector non-spin- and spin-transfer responses in nuclei.

Charge-exchange reactions↗

DOE OSTI2022

First inverse kinematics measurement of resonances in Be 7 ( α , γ ) C 11 relevant to neutrino-driven wind nucleosynthesis using DRAGON

A possible mechanism to explain the origin of the light $\textit{p}$ nuclei in the Galaxy is the nucleosynthesis in the proton-rich neutrino-driven wind ejecta of core-collapse supernovas via the $\textit{νp}$ process. However, this production scenario is very sensitive to the underlying supernova dynamics and the nuclear physics input. As far as the nuclear uncertainties are concerned, the breakout from the $\textit{pp}$ chains via the 7 Be(α,γ) 11 C reaction has been identified as an important link which can influence the nuclear flow and, therefore, the efficiency of the $\textit{νp}$ process. However, its reaction rate is poorly known over the relevant temperature range, $\textit{T}$ = 1.5–3 GK. We report on the first direct measurement of two resonances of the 7 Be(α,γ) 11 C reaction with previously unknown strengths using an intense radioactive 7 Be beam from the Isotope Separator and Accelerator (ISAC-I) Center facility and the DRAGON recoil separator in inverse kinematics. In this work, we have decreased the 7 Be(α,γ) 11 C reaction rate uncertainty to ≈9.4–10.7% over the relevant temperature region.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

NASA NTRS1991

Induced radioactivity in LDEF components

The systematics of induced radioactivity on the Long Duration Exposure Facility (LDEF) were studied in a wide range of materials using low level background facilities for detection of gamma rays. Approx. 400 samples of materials processed from structural parts of the spacecraft, as well as materials from onboard experiments, were analyzed at national facilities. These measurements show the variety of radioisotopes that are produced with half-lives greater than 2 wks, most of which are characteristic of proton induced reactions above 20 MeV. For the higher activity, long lived isotopes, it was possible to map the depth and directional dependences of the activity. Due to the stabilized configuration of the LDEF, the induced radioactivity data clearly show contributions from the anisotropic trapped proton flux in the South Atlantic Anomaly. This effect is discussed, along with evidence for activation by galactic protons and thermal neutrons. The discovery of Be-7 was made on leading side parts of the spacecraft, although this was though not to be related to the in situ production of radioisotopes from external particle fluxes.

Harmon, B. A.↗

DOE OSTI2025

Post-Irradiation Examination on MiniFuel UCO and UO 2 TRISO Particles Irradiated in HFIR at High Power

Post-irradiation examination (PIE) of MiniFuel compacts was conducted at Oak Ridge National Laboratory (ORNL) under the Nuclear Science User Facilities project in collaboration with Kairos Power (KP) to evaluate the performance of tristructural-isotropic (TRISO) particles under high particle power and fluoride-salt-cooled high-temperature reactor (FHR)-relevant conditions. MiniFuel compacts containing low-enriched uranium oxide-uranium carbide (LEUCO), low-enriched uranium dioxide (LEUO2), and natural UCO (NUCO) kernels were irradiated for four cycles at ORNL’s High Flux Isotope Reactor (HFIR) at target temperatures between 500°C and 900°C. Post irradiation, the experiment was disassembled at ORNL to recover the MiniFuel subcapsules, which were subsequently punctured to measure fission gas release. Subcapsule disassembly allowed the recovery of components of interest, such as silicon carbide (SiC) thermometry, fuel specimens, fission product sinks, and SiC spacers. The experimental irradiation temperature was confirmed by analyzing the SiC thermometry via dilatometry. PIE on the fuel specimens included gamma spectrometry and deconsolidation leach burn leach, which were complemented by imaging techniques such as x-ray computed tomography, optical microscopy, and electron microscopy. The PIE results provide insight into TRISO particle integrity, fission product retention, coating performance, and kernel migration, informing fuel qualification for application in KP’s FHR concept.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2026

Mark-18A Target Material Recovery Program: Initial Hot Startup

The Savannah River National Laboratory (SRNL) has been tasked by the National Nuclear Security Administration to recover highly valued isotopes from irradiated Mark-18A (Mk-18A) targets. The Savannah River Site (SRS) has sixty-five Mk-18A targets available for the recovery of the high valued materials. The Mk-18A targets were manufactured with Pu-242 then irradiated under high neutron flux in K-Reactor at the SRS from 1968 to 1978. The sixty-five Mk-18A targets are currently stored in the SRS L-Area Basin and will be removed one at a time and individually transported to SRNL. Upon receipt at SRNL, the Mk-18A target material will be removed from the confinement, dissolved, chemically separated, and calcined to a stable oxide. The flowsheet is designed to recover the plutonium as well as the trivalent actinides. The original targets were manufactured with varying quantities of Pu-242, ranging from 5.2 grams to 121.5 grams. Taking a graded approach to process start up, the lowest loaded target (FT-80-03) was selected as the first target to be received and processed at SRNL. As operational experience and knowledge is gained from processing targets, higher loaded targets will be selected for processing to increase the quantities of valuable isotopes recovered. Due to dose concerns, the receipt and processing of the Mk-18A targets is performed in the SRNL Shielded Cells Facility. The targets are stored in a double J-can confinement in the L-Area Basin. A specially designed cask was procured for transport of the targets from L-Area to SRNL. Once received at SRNL, the targets are loaded into the back of Cell 7 and resized as they enter the cell. The resized targets (1/4 length) are then processed one at a time through the following processes: caustic dissolution and filtration, acidic dissolution and filtration, elutable Reillex anion exchange, diglycolamide (DGA) resin extraction, and DGA calcination. This processing results in two product streams. The first is an aqueous plutonium solution which is removed from the shielded cells and taken to a glovebox for further purification and conversion to an oxide. The second is a calcined oxide product containing the Am and Cm as well as other lanthanide fission products which is removed from the shielded cells using a bagless transfer system. Both materials are packaged for shipment to Oak Ridge National Laboratory (ORNL). This paper will discuss the operating experience, lessons learned, and results from initial process hot startup.

Armstrong, Christopher [Savannah River National La↗

DOE OSTI2021

Measurements of Short-Lived Isomers from Photofission as a Method of Active Interrogation for Special Nuclear Materials

Isomeric fission products, such as 134m Te (T 1/2 = 164 ns) and 136m Xe (T 1/2 = 2.95 μs), are proposed as a signature of special nuclear materials in active interrogation applications. To test this conjecture, monoenergetic 9, 11, and 13 MeV photons from the HIγS facility are used to induce fission of 235 U, 238 U, and 239 Pu targets. The de-excitation γ rays of the isomers are measured using time-gated spectroscopy with high-purity germanium detectors. The 134m Te and 136m Xe isomers are detected and identified by the energy and decay half-life of their characteristic γ-ray transitions. The ratio of yields for these two signature γ rays, corresponding to 134m Te/( 136m Xe + 136 I), is found to be strongly correlated with the identity of the fissioning nuclei. These results show that fission-product isomers may be used in active interrogation to detect and identify special nuclear materials, even providing information on the isotopic enrichment. In conclusion, the feasibility of an active interrogation scenario using a bremsstrahlung beam is discussed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Post-Irradiation Examination on MiniFuel UCO and UO 2 TRISO Particles Irradiated in HFIR at High Power

Post-irradiation examination (PIE) of MiniFuel compacts was conducted at Oak Ridge National Laboratory (ORNL) under the Nuclear Science User Facilities project in collaboration with Kairos Power (KP) to evaluate the performance of tristructural-isotropic (TRISO) particles under high particle power and fluoride-salt-cooled high-temperature reactor (FHR)-relevant conditions. MiniFuel compacts containing low-enriched uranium oxide-uranium carbide (LEUCO), low-enriched uranium dioxide (LEUO 2 ), and natural UCO (NUCO) kernels were irradiated for four cycles at ORNL’s High Flux Isotope Reactor (HFIR) at target temperatures between 500°C and 900°C. Post irradiation, the experiment was disassembled at ORNL to recover the MiniFuel subcapsules, which were subsequently punctured to measure fission gas release. Subcapsule disassembly allowed the recovery of components of interest, such as silicon carbide (SiC) thermometry, fuel specimens, fission product sinks, and SiC spacers. The experimental irradiation temperature was confirmed by analyzing the SiC thermometry via dilatometry. PIE on the fuel specimens included gamma spectrometry and deconsolidation leach burn leach, which were complemented by imaging techniques such as x-ray computed tomography, optical microscopy, and electron microscopy. The PIE results provide insight into TRISO particle integrity, fission product retention, coating performance, and kernel migration, informing fuel qualification for application in KP’s FHR concept.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS1992

Gamma radiation survey of the LDEF spacecraft

The retrieval of the Long Duration Exposure Facility spacecraft in January 1990 after nearly six years in orbit offered a unique opportunity to study the long term buildup of induced radioactivity in the variety of materials on board. We conducted the first complete gamma-ray survey of a large spacecraft on LDEF shortly after its return to earth. A surprising observation was the Be-7 activity which was seen primarily on the leading edge of the satellite, implying that it was picked up by LDEF in orbit. This is the first known evidence for accretion of a radioactive isotope onto an orbiting spacecraft. Other isotopes observed during the survey, the strongest being Na-22, are all attributed to activation of spacecraft components. Be-7 is a spallation product of cosmic rays on nitrogen and oxygen in the upper atmosphere. However, the observed density is much greater than expected due to cosmic-ray production in situ. This implies transport of Be-7 from much lower altitudes up to the LDEF orbit.

Phillips, G. W.↗

DOE OSTI2026

The sweeper spectrometer for neutron invariant-mass spectroscopy at FRIB

Neutron invariant-mass spectroscopy (NIMS) is a key technique for studying unbound and weakly bound nuclei at the limits of stability. At the Facility for Rare Isotope Beams (FRIB), such measurements are performed using the Sweeper spectrometer, a large-gap, high-rigidity dipole system coupled to the MoNA-LISA neutron detector arrays. To meet the demands imposed by higher beam energies (>130 MeV/u) and the broad cocktail-beam selection available at FRIB, the spectrometer has recently been upgraded to improve particle-identification and detection performance. Upstream of the reaction target, a plastic scintillator with Silicon photomultiplier (SiPM) readout provides the global trigger and time reference, two parallel plate avalanche counters (PPACs) track the trajectories of incoming beam particles, and a silicon PIN detector measures the energy loss, ΔE, for charge (Z) identification. After the Sweeper magnet, the trajectories of the reaction products are tracked by two micro-pattern drift chambers (MPDCs), their charge (Z) is identified by a Frisch-grid ionization chamber (FG-IC), and their mass-to-charge ratio (A/Q) is deduced by time-of-flight measurement using a fast plastic scintillator read out by an array of photomultiplier tubes (PMTs). The detection system also incorporates the Modular Neutron Array (MoNA) for neutron detection and the CAESium-iodide scintillator ARray (CAESAR) for high-efficiency γ-ray measurements to enable full kinematic reconstruction. Performance was evaluated using a cocktail beam around 37 Al accelerated at E ≈ 130 MeV/u during the first FRIB campaign, demonstrating the readiness of the upgraded system for future studies of nuclei at and beyond the neutron drip line.

Particle identification methods↗

NASA NTRS1991

Gamma radiation survey of the LDEF spacecraft

The retrieval of the Long Duration Exposure Facility (LDEF) spacecraft after nearly 6 years in orbit offered a unique opportunity to study the long term buildup of induced radioactivity in the variety of materials on board. The first complete gamma ray survey was conducted of a large spacecraft on LDEF shortly after its return to Earth. A surprising observation was the large Be-7 activity which was seen primarily on the leading edge of the satellite, implying that it was picked up by LDEF in orbit. This is the first known evidence for accretion of a radioactive isotope onto an orbiting spacecraft. Other isotopes seen during the survey, the strongest being Na-22 and Mn-54, are all attributed to activation of spacecraft components in orbit. Be-7 is a spallation product of cosmic rays on nitrogen and oxygen in the upper atmosphere. However, the observed density is much greater than expected due to cosmic ray production in situ. This implies transport of Be-7 from much lower altitudes up to the LDEF orbit.

Phillips, G. W.↗

NASA NTRS1993

Radioactivities induced in some LDEF samples

Radioactivities induced in several Long Duration Exposure Facilities (LDEF) samples were measured by low-level counting at Los Alamos and elsewhere. These radionuclides have activities similar to those observed in meteorites and lunar samples. Some trends were observed in these measurements in terms of profiles in trunnion layers and as a function of radionuclide half-life. Several existing computer codes were used to model the production by the protons trapped in the Earth's radiation belts and by the galactic cosmic rays of some of these radionuclides, Mn-54 and Co-57 in steel, Sc-46 in titanium, and Na-22 in alloys of titanium and aluminum. Production rates were also calculated for radionuclides possibly implanted in LDEF, Be-7, Be-10, and C-14. Enhanced concentrations of induced isotopes in the surfaces of trunnion sections relative to their concentrations in the center are caused by the lower-energy protons in the trapped radiation. Secondary neutrons made by high-energy trapped protons and by galactic cosmic rays produce much of the observed radioactivities, especially deep in an object. Comparisons of the observed to calculated activities of several radionuclides with different half-lives indicate that the flux of trapped protons at LDEF decreased significantly at the end of the mission.

Reedy, Robert C.↗

DOE OSTI2020

Understanding the Structure and Dynamics of Complex Biomembrane Interactions by Neutron Scattering Techniques

The membrane is one of the key structural materials of biology at the cellular level. Composed predominantly of a bilayer of lipids with embedded and bound proteins, it defines the boundaries of the cell and many organelles essential to life and therefore is involved in almost all biological processes. Membrane-specific interactions, such as drug binding to a membrane receptor or the interactions of an antimicrobial compound with the lipid matrix of a pathogen membrane, are of interest across the scientific disciplines. Herein we present a review, aimed at nonexperts, of the major neutron scattering techniques used in membrane studies: small-angle neutron scattering, neutron membrane diffraction, neutron reflectometry, quasielastic neutron scattering, and neutron spin echo. Neutron scattering techniques are well suited to studying biological membranes. The nondestructive nature of cold neutrons means that samples can be measured for long periods without fear of beam damage from ultraviolet, electron, or X-ray radiation, and neutron beams are highly penetrating, thus offering flexibility in samples and sample environments. Most important is the strong difference in neutron scattering lengths between the two most abundant forms of hydrogen, protium and deuterium. Changing the relative amounts of protium/deuterium in a sample allows the production of a series of neutron scattering data sets, enabling the observation of differing components within complex membrane architectures. This approach can be as simple as using the naturally occurring neutron contrast between different biomolecules to study components in a complex by changing the solution H 2 O/D 2 O ratio or as complex as selectively labeling individual components with hydrogen isotopes. This review presents an overview of each experimental technique with the neutron instrument configuration, related sample preparation and sample environment, and data analysis, highlighted by a special emphasis on using prominent neutron contrast to understand structure and dynamics. This review gives researchers a practical introduction to the often enigmatic suite of neutron beamlines, thereby lowering the barrier to taking advantage of these large-facility techniques to achieve new understandings of membranes and their interactions with other molecules.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Efficient loading of reduced data ensembles produced at ORNL SNS/HFIR neutron time-of-flight facilities

We present algorithmic improvements to the loading operations of certain reduced data ensembles produced from neutron scattering experiments at Oak Ridge National Laboratory (ORNL) facilities. Ensembles from multiple measurements are required to cover a wide range of the phase space of a sample material of interest. They are stored using the standard NeXus schema on individual HDF5 files. This makes it a scalability challenge, as the number of experiments stored increases in a single ensemble file. The present work follows up on our previous efforts on data management algorithms, to address identified input output (I/O) bottlenecks in Mantid, an open-source data analysis framework used across several neutron science facilities around the world. We reuse an in-memory binary-tree metadata index that resembles data access patterns, to provide a scalable search and extraction mechanism. In addition, several memory operations are refactored and optimized for the current common use cases, ranging most frequently from 10 to 180, and up to 360 separate measurement configurations. Results from this work show consistent speed ups in wall-clock time on the Mantid LoadMD routine, ranging from 19% to 23% on average, on ORNL production computing systems. The latter depends on the complexity of the targeted instrument-specific data and the system I/O and compute variability for the shared computational resources available to users of ORNL’s Spallation Neutron Source (SNS) and the High Flux Isotope Reactor (HFIR) instruments. Nevertheless, we continue to highlight the need for more research to address reduction challenges as experimental data volumes, user time and processing costs increase.

Godoy, William↗