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DOE OSTI2025

FRAM Version 7.1’s Bias

The Fixed-Energy Response-Function Analysis with Multiple Efficiency (FRAM) code was developed at Los Alamos National Laboratory to measure the gamma-ray spectrometry of the isotopic composition of plutonium, uranium, and other actinides. For FRAM versions 4 and earlier, the reported uncertainties of the results come from the propagation of the statistics in the peak areas only. No systematic error components are included in the reported uncertainties. For FRAM versions 5 and 6, we examined the FRAM analytical results of both the archival plutonium data and the data specifically acquired for the isotopic uncertainty analysis project and found the relationship between the bias and other parameters. We worked out the equations representing the biases of the measured isotopes from each measurement using internal spectral parameters, such as peak resolution and shape, region of analysis, and burnup (for plutonium) or enrichment (for uranium). The resulting biases were included in the reported uncertainties of FRAM v.5 and v.6.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

VARI3D & PERSENT: Perturbation and Sensitivity Analysis

The nodal diffusion method is one of the most widely used approaches in modern reactor analysis. In the nodal diffusion method, a coarse multi-group set of “homogenized” parameters is constructed such that the complex geometry of a reactor core along with the energy dependence of neutron and gamma ray cross sections in a nuclear reactor are conserved in the simpler geometry. The homogenization is typically done on a fuel assembly level as is the case in the DIF3D code developed at Argonne National Laboratory. The nodal methodology is used primarily to predict fuel cycle behavior of nuclear systems of which there is a substantial amount of validation in the literature. Another use of the nodal method is to obtain reactivity coefficients and kinetics parameters for use in a safety analysis of a given nuclear reactor. While there are many ways to obtain reactivity worth and kinetics parameters, the work presented in this manuscript is unique as it provides the user with the ability to compute reactivity worths, kinetics parameters, and cross section sensitivities with a Cartesian and hexagonal geometry based transport code. This manuscript serves as a single manual for two separate codes: VARI3D and PERSENT. The VARI3D code (VARIational 3D) is based upon the classic finite difference diffusion theory solver available in DIF3D. The PERSENT code (PERturbation and SENitivity for Transport) is based upon the variational nodal method employed in DIF3D termed VARIANT. The VARIANT solver was added to DIF3D in 1995 and has seen continued development and use for the last 18 years. Because VARI3D primarily uses deprecated coding practices, rather than incorporating the perturbation and sensitivity treatments for transport within VARI3D, a new coding development was built using modern Fortran coding. The primary purpose of this manual is to describe the theory behind PERSENT (and by convenience, that of VARI3D) and discuss the input and output of PERSENT along with giving potential users an idea of how to use it. While this manuscript does describe the input and output of VARI3D, the PERSENT code is intended to be the replacement capability of VARI3D as PERSENT can generate nearly identical (if not superior) diffusion theory results. In this manuscript, the relevant aspects of generalized perturbation theory and exact perturbation theory that apply to both VARI3D and PERSENT are covered. The input and output of VARI3D is displayed by excerpting several of the example problems. Similarly, the input and output of PERSENT is displayed along with tips on how best to use the code. Note that the input and output of the inhomogeneous solver wrapped around DIF3D (DIF3D_IFS) is also discussed as it is needed to carry out some of the sensitivities in PERSENT such as reaction rate ratios. This manuscript describes several perturbation and sensitivity problems, and the results computed using PERSENT. From these sections, potential users should find that PERSENT provides not only the typical tables of numbers desired in perturbation and sensitivity analysis work, but also can visually plot the result for a more thorough understanding of the space and energy distribution (Section 5). Overall, PERSENT is observed to produce accurate reactivity worths and sensitivities for the displayed set of test problems and clearly demonstrates the need to have a transport-based sensitivity capability as evident from the thousands of percent errors observed in the 21-group hexagonal fast reactor problem (covered in Section 7). The uncertainty calculation capability is described in Section 3 and demonstrated in Section 7.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2025

Window Cooling Studies and Disk Vibration Testing on a Subset of Mo-100 Disks

Production of metastable Technetium-99 (Tc-99m), a radioactive tracer that emits gamma rays, is vital to the medical imaging community. Tc-99m is extracted from the decay of Molybdenum-99 (Mo-99) which has a half-life of about 2-3 days. The work presented in this report is part of the NNSA’s mission to produce Mo-99 commercially, within the US, without the use of highly enriched uranium (HEU) in support of nonproliferation and global security. Los Alamos National Laboratory (LANL) is working with NorthStar Medical Radioisotopes (NMR) on their efforts to produce Mo-99 through the irradiation of Mo-100 targets using an electron beam. The NMR target comprises a stack of approximately 60-70 Mo-100 disks with diameter 24 mm and thickness 0.74 mm held in stainless steel laminations, each separated using 0.25 mm thick stainless-steel spacers. The symmetric target stack is housed in an Inconel vessel with two Inconel windows on either side. Two electron accelerators are used to produce 40 MeV, 3.16 µA electron beams each that penetrate the Inconel windows and irradiate the Mo-100 disks. Approximately 90% of the total 250 kW beam power is deposited in the NMR target during the irradiation process, with a smaller percentage adding up to 2.2 kW of heat deposited on the Inconel window. During irradiation, pressurized helium gas flows through thin gaps between the disks cooling the beam window, target disks, disk laminations and spacers. Both NMR and LANL have found during cold testing of the target system (no heat deposition) that the Mo 100 disks undergo significant mass loss and disk breakage due to vibrations induced by the flowing helium gas. The mass loss is not only undesirable due to monetary loss from reduced final quantities of Mo-99, but also due to the hazards associated with radioactive material trapped in the cooling lines and particle filters. The effect of flow rate and target geometry on the flow induced vibrations need to be quantified, and recommendations provided to minimize this mass loss. LANL has previously also tested NMR’s Inconel beam window by heating the window, while flowing pressurized helium, using the average heat deposited on the window. However, the NMR beam is pulsed with a duty cycle of 12.5%, which introduces oscillation in temperature around the nominal 600 °C steady state value with each pulse. Available fatigue curves for Inconel are few, established for room temperature, and they are based on mechanical strain cycles not thermally induced strain as in the NMR target. The effect of pulsed beam heating on the Inconel window therefore needs to be quantified. This report details the experiments conducted to assess the factors that lead to mass loss in the NMR target disks as well as to understand the effect of a pulsed beam on NMR’s Inconel window. This work describes LANL’s experimental characterization of the flow induced vibrations and disk mass loss in a reduced scale set-up containing 5 to 10 Mo-100 disks. We use high speed imaging, displacement measurements and microphone measurements combined with signal processing to estimate the vibration frequency of each disk. The effect of disk thickness, target fit and duration of testing on the mass loss is described. We find that in the current configuration of NMR targets, the vibrations and mass loss on the first disk are minimized, while those in the adjacent disks are highest. The microphone and high-speed image data show that increased flow rates and increased duration of testing increases vibration frequency and mass loss. The mass loss is due to both disk rotation and back and forth motion. There are visible wear marks on the disks with the highest mass loss. We also note that the current NMR window gap reduces flow induced vibrations compared to the previous smaller gaps. Improved target holders significantly reduce disk mass loss to almost negligible quantities. This work finds that the larger window to first disk gap and improved target holder geometry should allow NMR to successfully conduct irradiations with minimal mass loss. The window tests were conducted to understand the effect of a pulsed beam on both the window longevity and to estimate the window temperature and displacement during pulsing. The experiments presented here were performed at significantly low power, due to the limitations of the induction heating system. The window temperature rose to approximately 73 °C with a significantly reduced power of 45 W without beam pulsing. With a 5 Hz pulse rate, 12.5% duty cycle, the window temperature remained constant at 26 °C. These experiments will be repeated with improved coil geometry and reported in upcoming journal papers.

42 ENGINEERING↗

DOE OSTI2021

ARC Software Validation Work for the FFTF Reactor

Extensive efforts have been carried out at ANL for the verification and validation of the Argonne Reactor Codes (ARC) software package currently used for the design of Versatile Test Reactor (VTR). The ARC software package consists of steady state neutronics and thermal hydraulics modeling capabilities which are being used by the VTR program to develop most of the VTR reactor design details which will be part of the licensing application. It is anticipated that this software will continue to be used for the design work and for initial operations although additional software may be introduced at a later time. The validation work was focused primarily on obtaining validation data consistent with VTR and usable for the ARC software. Because no critical facilities or operating fast spectrum reactors are available to do experiments for the VTR, the next best option is to identify historical experimental data that can be used as validation data. Early on in VTR, the ZPPR-15 set of experiments was identified as good validation data because of 1) the availability and quality of the data, 2) existing staff that are already familiar with the experimental machine and measurements, 3) most of the ZPPR-15 loadings of interest have already been processed into ARC models, and 4) a full uncertainty quantification has already been done for several loadings of ZPPR-15. The FFTF startup and operations data was identified as the most consistent reactor type that has validation data usable for VTR. Finally, the EBR-II fuel depletion measurements were identified as the best available validation data for VTR. It is important to note that both the FFTF and EBR-II reactors typically come with higher uncertainties than the ZPPR. In the frame of the discussed verification and validation efforts, the present document discusses the analysis of selected FFTF measurements included in the benchmark specifications of the International Reactor Physics Experiment (IRPhE) handbook. The FFTF reactor core configurations from the benchmark specification are presented in Section 2. The analysis is performed with the use of the ARC code suite available at ANL for fast reactor studies and is discussed in Section 3. The reactor parameters from the benchmark include criticality, neutron spectra, effective delayed neutron spectra, control rod worth, isothermal temperature coefficient and low energy gamma-ray spectra. The calculated values and the comparison with the experimental data is discussed in Sections 4 to 9 for each considered reactor parameter. Finally, conclusions are presented in Section 10.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2023

Gamma Spectrometry Code Rodeo for Uranium Enrichment—FY 2022 Report

In the first two quarters of FY22, data acquisition continued at ORNL and LLNL using uranium sources of known enrichments. This was an FY21 task which could not be completed in FY21 because of problems encountered with the ORNL M400 CZT in Q4 of FY21, and the subsequent repairs. The detector was received back from H3D in the first of September 2021 , and the measurements resumed . Measurements using the repaired detector were completed in Q1 of FY22. The spectra were distributed by ORNL to the analyzing labs. Analysis results were received in Q2 of FY2022. The results from the various codes were intercompared and an ANOVA analysis was performed. Random and systematic uncertainties were established for each code. The ANOVA results and discussions were included in a revised version of FY21Annual Report issued in March 2022. A paper was presented at the INMM 2022Annual Conference, with the analysis results from the various isotopic codes, and the ANOVA table with random and systematic uncertainties. The Project Work Plan (PWP) for FY22 included a task to perform field testing of the M400 CZT and the analysis codes using UF 6 cylinder measurements at the Framatome Fuel Fabrication Facility in Richland, WA. PNNL was the lead for the field testing task. PNNL drafted a Field Test Plan, and refined it based on comments received from the team. PNNL coordinated with Framatome facility, the logistics of carrying out the field testing . A collimator and shield made out of TFlex (tungsten impregnated polymer) was designed and professionally manufactured. The collimators were used in the field test measurements. The measurements at Framatome were completed on April 21, 2022. A total of 34 Type 30B cylinders were measured using three M400 detectors (PNNL, LLNL, and ORNL detectors). Measurements using M400 were taken at two locations on the side of each cylinder and from the end-on bottom location. Additionally, HPGe measurements were taken at the end-on location to establish ground truth. Cylinder wall thickness measurements were also made at all three locations. To gain a better understanding of the effect of background from surrounding cylinders, the same five cylinders measured individually in low background locations were measured again in the cylinder storage yards. Due to inclement weather, manufacturer delays, shipping delays, and equipment failure, the measurement campaign spanned twice as long compared to the original timeline. Gamma-ray spectra from M400 and HPGe detectors, along with the cylinder data and photographs were organized and shared with the collaborators for further analysis. Spectra were analyzed by the participating laboratories. FY22 PWP also consists of tasks related to plutonium source measurements, adapting the codes to analyze plutonium spectra, and inter-comparison of the results from various codes. Plutonium spectra are being acquired at LANL, ORNL, and LLNL. LANL, SNL and LLNL are in the process of modifying FRAM, GADRAS, and CZTU, respectively. The plutonium related tasks will be completed in Q2 of FY23.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Nuclear Material Accounting and Control (NMAC) for a Commercial Fuel Debundling Facility in the United States

The concept of fuel debundling proposes that all non-fuel components of a fuel assembly be removed prior to beginning the recycling process. It was introduced to reduce the quantity of and cost of disposing high level radioactive waste during recycling in the United States. However, nuclear material accountancy and control programs could also benefit from fuel debundling due to a reduction in self-shielding material for individual fuel rods compared to a fuel assembly. Current NRC regulations and guidance point to an independent fuel debundling facility with a material-possession-only license as the best option for implementing this concept into a used fuel recycling scheme in the United States. This allows the facility to comply only with simple NMAC requirements under Subpart B of 10 CFR Part 74 without the need to submit an NMAC plan to the NRC, exempting it from more tedious and complex NMAC requirements. However, a recycling facility may desire a Pu mass estimate from measurements of each individual fuel rod to improve accountancy into the dissolver. Many technologies and methodologies were considered for performing NMAC in an independent fuel debundling facility in the United States. Few were able to meet anticipated throughput demands of up to 3,300 rods/day and achieve measurement uncertainties suitable for input accountancy for a recycling facility. The best option was a combination of passive gamma-ray spectroscopy and neutron coincidence counting to meet all requirements for the proposed Fuel Debundling Detector (FUDD). Follow-on work will include a full uncertainty analysis to inform what assumptions can be made to meet input accountancy objectives before beginning experimental activities.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

SpecFIDLER User Manual: Software Version 2.4.0

The Spectroscopic Field Instrument for Detection of Low Energy Radiation (SpecFIDLER) allows response teams to detect and quantify plutonium contamination on the ground. Notional scenarios include dispersion from a weapon accident, or the launch failure of a space probe containing a radioisotope thermoelectric generator. Unlike other instruments, the thin-window sodium iodide detector is sensitive to the low-energy gamma rays emitted by plutonium isotopes. The system supports both mobile survey as well as stationary sampling. This manual provides information about installing, maintaining, and troubleshooting the SpecFIDLER. The scope of this document includes the physical hardware, software for data acquisition, and algorithms for data analysis. Recent changes to the software and algorithms aim to streamline the operation of the system.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

SpecFIDLER User Manual (Software V.2.5.0)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

SpecFIDLER User Manual (Software V.2.6.0)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

SpecFIDLER User Manual (Software V.2.3.0)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2026

Quantum enabled precision measurements of the 229Th nuclear isomer transition (final report)

The existence of the nuclear isomer transition in thorium-229 was first inferred from keV lines in the gamma spectrum of uranium-233 decay more than 40 years ago. Over the years, the value of the transition energy has been refined with indirect measurements using nuclear physics techniques, and the current evidence points to transition energy in the laser-accessible vacuum ultra-violet region of the spectrum. At the start of this project, the two best measurements of the transition energy were 7.8±0.5 eV and 8.28±0.17 eV from high precision gamma ray spectroscopy and kinetic energy of internal conversion electrons, respectively. This project aimed to reduce the uncertainty in the transition energy to 10 meV using direct calorimetric measurements of the decay energy with superconducting nanowire single photon detectors (SNSPDs). Specifically, the method that was pursued was to generate thorium-229 in the excited isomer state by the alpha decay of uranium-233, embed the excited state thorium into an SNSPD, then detect the energy released when the isomer deexcites.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

New MeV-Scale Capabilities in Large Neutrino LArTPCs Using Ambient Radiogenic and Cosmogenic Activity in MicroBooNE

Large neutrino liquid argon time projection chamber (LArTPC) experiments can broaden their physics reach by reconstructing and interpreting MeV-scale energy depositions present in their data. We use data from MicroBooNE, an 85 tonnes LArTPC exposed to Fermilab neutrino beams from 2015 until 2021, to demonstrate new calorimetric and particle discrimination capabilities for isolated $\sim \mathrm{O}(1 \mathrm{MeV})$ energy depositions referred to as blips. We observe a concentration of low energy ( $<3$ MeV ) blips around fiberglass mechanical support struts along the TPC edges with energy spectrum features consistent with the Compton edge of 2.614 MeV Tl-208 decay gamma rays. These features are used to verify proper calibration of electron energy scales in MicroBooNE's data to few percent precision and to measure the specific activity of Tl-208 in the fiberglass composing these struts. Cosmogenicallyproduced blips above 3 MeV in reconstructed energy are used to showcase the ability of large LArTPCs to distinguish between low-energy proton and electron energy depositions.

Andrade Aldana, Diego Armando↗

DOE OSTI2026

Prairie State Generating Company Static and Dynamic Modeling

A reservoir modeling study was conducted to assess the feasibility of storing 162.5 million tonnes (8.125 million tonnes annually) of industrially sourced carbon dioxide (CO 2 ) in the St. Peter – Everton and Knox storage complexes at the Prairie State Generating Company’s (PSGC) site near Marissa, Washington County, Illinois (PSGC site). Two separate models were constructed for the St. Peter – Everton and the Knox storage complexes. The St. Peter and Everton sandstones are the target storage units for the St. Peter – Everton storage complex. The Knox Group formations are the target storage units for the Knox storage complex. The Maquoketa Shale is the primary confining unit for both storage complexes. The static reservoir models used as input to the dynamic reservoir models of the storage complexes were developed from interpretations of logs (e.g., gamma ray, resistivity, porosity, photoelectric, and sonic), structure surfaces using data from 36 wells, thickness maps, well test data, seismic data, and permeability data in PetrelTM.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2026

PARTICULATE STUDY OF NEG PUMPS IRRADIATED IN THE CEBAF TUNNEL

Non-evaporable getter (NEG) pumps are being used to maintain ultra-high vacuum in the beamline of superconducting radio-frequency (SRF) accelerators, such as the Continuous Electron Beam Accelerator Facility (CEBAF) at Jefferson Lab. Because of the sensitivity of the performance of SRF cavities to particulate contamination, it is important to evaluate the integrity of the NEG material after exposure to high radiation during beam operation. The particulate from two NEG pumps based on ZAO® getter alloy was measured with a particle counter in a clean-room. The pumps were assembled onto a hermetically sealed setup which was placed in the CEBAF tunnel. The setup was exposed to 24 h beam operation for ~ 230 days. The total gamma-rays dose measured on the test setup was ~ 1.6 Mrad. The total neutron dose measured at ~ 75 cm of the test setup was ~ 11 krad. The particulate count from the two pumps was measured again in the clean-room after irradiation. Whereas an increase of particulate counts was measured, compared to before irradiation, subsequent measurements indicate the absence of systematically loose particulate. The pumping speed of one of the irradiated pumps was also measured to be consistent with that of a non-irradiated one, corroborating the absence of significant damage to the ZAO® NEG material due to irradiation.

Ciovati, Gianluigi [Thomas Jefferson National Acce↗

DOE OSTI2026

Characterizing the energy resolution of the MicroBooNE LArTPC at the MeV scale using monoenergetic features of 208-Tl decays

A proper understanding of the capabilities and fidelity of low-energy reconstruction is crucial for taking advantage of MeV-scale neutrino physics opportunities in LArTPCs. This poster will present an analysis resulting in the first-ever demonstration of LArTPC energy resolution in the MeV regime. A measurement of the resolution of energy reconstruction in the MicroBooNE LArTPC at ~1.5 MeV was performed using monoenergetic signals generated by 208Tl decay gamma-rays pair-producing in the detector. This study provides a pathway for MeV-scale monoenergetic energy calibrations in future LArTPC experiments.

Manuel Alves, Maria Gabriela [IIT, Chicago] (ORCID↗

DOE OSTI2026

Toward Trustworthy Detectors Detector Characterization for SuperCDMS SNOLAB Commissioning

SuperCDMS SNOLAB is a next generation direct detection experiment searching for low mass dark matter using cryogenic germanium and silicon detectors operated at millikelvin temperatures. As commissioning begins, establishing stable, predictable detector response to energy deposits is a prerequisite for future physics analysis. This work studies detector stability and calibration for four SuperCDMS SNOLAB detectors, det 7 and det 15 (germanium) and det 11 and det 14 (silicon), using Barium-133 calibration data (356 keV gamma ray reference) and low background data (ambient radiation, no external source). The Ba-133 data show no distinct line at the expected energy, and the low background data show a baseline that drifts and oscillates rather than remaining flat, consistently across multiple channels, suggesting a shared, detector wide cause. These observations point to the cryogenic support system as the likely source, since small temperature fluctuations could couple into the temperature sensitive detectors, informing the ongoing commissioning effort.

O'Hanlon, Vika [Skidmore Coll.]↗

DOE OSTI2020

Where do $AMS-02$ anti-helium events come from?

We discuss the origin of the anti-helium-3 and -4 events possibly detected by AMS-02. Using up-to-date semi-analytical tools, we show that spallation from primary hydrogen and helium nuclei onto the ISM predicts a anti-helium-3 flux typically one to two orders of magnitude below the sensitivity of AMS-02 after 5 years, and a anti-helium-4 flux roughly 5 orders of magnitude below the AMS-02 sensitivity. We argue that dark matter annihilations face similar difficulties in explaining this event. We then entertain the possibility that these events originate from anti-matter-dominated regions in the form of anti-clouds or anti-stars. In the case of anti-clouds, we show how the isotopic ratio of anti-helium nuclei might suggest that BBN has happened in an inhomogeneous manner, resulting in anti-regions with a anti-baryon-to-photon ratio of one in a thousand of the baryon-to-photon ratio. We discuss properties of these regions, as well as relevant constraints on the presence of anti-clouds in our Galaxy. We present constraints from the survival of anti-clouds in the Milky-Way and in the early Universe, as well as from gamma-ray observations. In particular, these require the anti-clouds to be almost free of normal matter. We also discuss an alternative where anti-domains are dominated by surviving anti-stars. We suggest that part of the unindentified sources in the 3FGL catalog can originate from anti-clouds or anti-stars. AMS-02 and GAPS data could further probe this scenario.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

The Ultra-High-Energy Source MGRO J1908+06

The TeV gamma-ray source MGRO J1908+06 is one of the highest-energy sources known, with observed emission by the High Altitude Water Cherenkov (HAWC) Observatory extending well past 100 TeV. The source exhibits both energy-dependent morphology and a spatially-dependent spectral index. The emission is likely to be dominantly leptonic, and associated with the radio-quiet PSR J1907+0602. However, one-population models do not describe the data well; a second particle population is needed to explain the shape of the spectral energy distribution at the highest energies. This component can be well-described by either leptonic or hadronic hypotheses. We discuss this feature and implications for detection by multi-wavelength and multi-messenger experiments.

79 ASTRONOMY AND ASTROPHYSICS↗