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Deuteron-induced reactions on natural Zr from threshold to 50 MeV: production of 86g Y

Two stacks of thin Zr foils were irradiated with 30 and 50 MeV deuterons, respectively, using the Lawrence Berkeley National Laboratory 88-Inch Cyclotron, and 19 excitation functions for nat Zr(d,x) reactions were measured over a beam energy range of 6.3–47.64 MeV, where the independent cross sections for nat Zr(d,x) 88 Nb and nat Zr(d,x) 86m,g Y were measured for the first time. The well-characterized nat Fe(d,x) 56 Co, nat Ni(d,x) 56 Co, nat Ni(d,x) 58 Co, nat Ni(d,x) 61 Cu, nat Ti(d,x) 46 Sc and nat Ti(d,x) 48 V monitor reactions were used to determine the deuteron beam current throughout the stacks. All cross sections were determined using High Purity Germanium (HPGe) detector γ-ray spectroscopy. A variance minimization technique was employed to simultaneously constrain the deuteron beam currents with multiple monitor reactions, thus reducing systematic uncertainties. An additional 16 channels are reported for reactions on the nickel, titanium, and iron monitor foils, leading to a total of 35 excitation functions, with seven reaction channels reported for the first time in this work. The measured excitation functions are compared to calculations provided by the reaction modeling codes TALYS – 2.0, ALICE – 2020, CoH – 3.5.3 and EMPIRE – 3.2.3, as well as the TENDL – 2023 data library. The degree of agreement between theory and experiments is discussed. The possible production of the important PET radionuclide 86g Y via the nat Zr(d,x) route was critically examined. The physical yields for nat Zr(d,x) 86 Y and other yttrium isotopes produced were calculated and compared to other production pathways. Due to high-level of associated radionuclide impurities, this route cannot deliver 86g Y suitable for medical applications.

86gY

Analysis of Radioactive Waste and Contamination using 3D Position-Sensitive CdZnTe Detectors

INTRODUCTION The US has surplus plutonium. This material will be diluted in gloveboxes at SRS [Ref 1 and 2]. This process will create holdup. Holdup is material in an unexpected or unwanted location. Because this holdup material is primarily PuO2, it must be accounted for (measured). This measurement is typically done using a liquid-nitrogen cooled, HPGe detector. To enable more rapid processing, advanced holdup technologies are being explored [Ref 3 and 4]. METHODS For the surplus plutonium dilute and dispose program, the traditional detector system could slow down the optimal operational tempo of the program. A multiple-detector system, providing complete glovebox coverage, based on CdZnTe crystals, 3D-positioning electronics, and a coded aperture mask, is in the process of being developed by ORNL and SRNL [Ref 4].

Whiteside, Tad [Savannah River National Laboratory

FRAM v.7.1

Fixed-energy Response-function Analysis with Multiple efficiency (FRAM) is a software code designed primarily for plutonium and uranium isotopic analysis. It is widely used in both the domestic and international safeguards community. FRAM can quickly and accurately determine the isotopic compositions of plutonium, uranium, and mixed oxides (MOX) when measuring with a high-purity germanium (HPGe), cadmium zinc telluride (CZT), or lanthanum bromide (LaBr3) detector. The capabilities of FRAM have been enhanced to analyze the data of the pixelated CZT detector (made by H3D) and to measure the mass of plutonium, uranium, and MOX. Both the isotopic composition and mass of the item can be quickly determined with one measurement using a gamma detector with FRAM v.7.1.

07 ISOTOPE AND RADIATION SOURCES

Assessment of Naturally Occurring Radioactive Material (NORM) in Illicit Drugs Using High-Resolution Gamma Spectroscopy

This report documents results assessing the presence of Naturally Occurring Radioactive Material (NORM) in illicit drugs using high-resolution gamma spectroscopy. Specifically, high-purity germanium (HPGe) measurements were conducted at the Drug Enforcement Administration (DEA) South Central Laboratory on 11 samples (referred to as exhibits) including cocaine, fentanyl, heroin, ketamine, LSD, marijuana, methamphetamines, psilocybin mushrooms, and synthetic cannabinoids.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA

GADRAS-DRF Validation for Safeguards and Custom Peak Fit Enhancements

In previous years, SGTech funded enhancements to the isotopics routine in the software called Gamma Detector Response and Analysis Software-Detector Response Function (GADRAS-DRF), including the addition of peak fit customization capabilities. A project was also funded that focused on implementing a peak-based model fitting routine, allowing model fitting to be performed without dependence on export-controlled cross-sections. In FY25 significant improvements were made to the custom peak fitting interface, accompanied by several validation studies within GADRAS-DRF. These studies encompassed IsotopeID performance, distributed source analysis, isotopics validation, and activity estimation. Additionally, the peak-only model fitting option was validated using an HPGe measurement of a rotating drum with line sources.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Detector Response and Battery Reliability

The Sandia National Laboratories (SNL) Material Control and Accountability (MC&A) measurements team performs confirmation measurements of Special Nuclear Material (SNM) at different locations around Sandia. The measurement team has access to two High purity Germanium (HPGe) detectors, the AEGIS (Model: AEGIS-BEGE5030), and the ORTEC (Model: trans-SPEC-DX-100). These two can operate purely on battery power, but the response of the detectors while on battery power is not well documented. To enhance our knowledge with these detectors the team wants to investigate the detectors response to changes in battery range, wall charging, and mid operation battery swaps (Hot Swaps).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

24.1.3.4 Upgraded Fixed Energy Response Function Analysis with Multiple Efficiencies (FRAM) Software for U/Pu/MOX Mass Measurements

Fixed-energy Response-function Analysis with Multiple efficiency (FRAM) is a software code designed primarily for plutonium and uranium isotopic analysis. It is widely used in both the domestic and international safeguards community. FRAM can quickly and accurately determine the isotopic compositions of plutonium, uranium, and mixed oxides (MOX) when measuring with a high-purity germanium (HPGe), cadmium zinc telluride (CZT), or lanthanum bromide (LaBr 3 ) detector. The capabilities of FRAM have been enhanced to analyze the data of the pixelated CZT detector (made by H3D) and to measure the mass of plutonium, uranium, and MOX. Both the isotopic composition and mass of the item can be quickly determined with one measurement using a gamma detector with FRAM v.7.1.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND

Radioactivity-in-materials lead for nEXO (Final Scientific Report)

Abstract, introduction, and summary of work completed and products produced by DOE award SC002466. Primary products were six peer-reviewed publications and two PhD theses. This award also supported the operation of an underground HPGe detector and several radioassay measurements: one in a stand alone publication in Phys. Rev. C and the others in an upcoming nEXO radioassay summary paper. The nEXO collaboration aims to demonstrate the Majorana nature of the neutrino by observing the neutrinoless double-beta decay of 136 Xe with a next-generation experiment. The University of Kentucky nEXO group (UKY) operates a world-leading ultra-low-background γ-ray spectrometer as part of the nEXO radioactive background control R&D effort. The nEXO project is a proposed ton-scale neutrinoless double-beta decay experiment. The UKY PI is leading the radioactivity content assessment for all materials required by the nEXO project. As a subset of this task, UKY is also responsible for project-wide management of all low-background γ-ray spectrometry measurements; material assays with these types of instruments, together with ICP-MS, neutron-activation-analysis, and α-spectrometry, are critical to ensuring that the nEXO project can achieve its design sensitivity

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

Accelerated 133 Xe Quantification in Samples Containing Significant 133 mXe

The quantification of 133 Xe in the presence of its mother radionuclide 133 mXe requires the full quantification of both to perform the ingrowth correction for 133 Xe. Due to the nature of both of these radionuclides, the 133 mXe requires significantly more time to quantify by High Purity Germanium (HPGe) detectors due to lower production yields, lower gamma emission probabilities, and lower detection efficiencies. This work shows that 133 Xe and 133 mXe quantification can be accelerated by measuring the 133m:133 activity ratio for a large batch of material and applying this activity ratio to assays of lower activity subsamples of the same batch of material. Included in this report are derivations of the required decay correction equations, and experiments using actual samples to validate the performance of these equations. A detector calibration method is also shown that leverages this method as an alternative to existing calibration methods for 133 mXe quantification.

133mXe

High-spatial resolution and high-spectral resolution detector for use in the measurement of solar flare hard X-rays

In the areas of high spatial resolution, the evaluation of a hard X-ray detector with 65 micron spatial resolution for operation in the energy range from 30 to 400 keV is proposed. The basic detector is a thick large-area scintillator faceplate, composed of a matrix of high-density scintillating glass fibers, attached to a proximity type image intensifier tube with a resistive-anode digital readout system. Such a detector, combined with a coded-aperture mask, would be ideal for use as a modest-sized hard X-ray imaging instrument up to X-ray energies as high as several hundred keV. As an integral part of this study it was also proposed that several techniques be critically evaluated for X-ray image coding which could be used with this detector. In the area of high spectral resolution, it is proposed to evaluate two different types of detectors for use as X-ray spectrometers for solar flares: planar silicon detectors and high-purity germanium detectors (HPGe). Instruments utilizing these high-spatial-resolution detectors for hard X-ray imaging measurements from 30 to 400 keV and high-spectral-resolution detectors for measurements over a similar energy range would be ideally suited for making crucial solar flare observations during the upcoming maximum in the solar cycle.

Desai, U. D.

Gamma-ray observations of SN 1987A with an array of high-purity germanium detectors

A balloonborne gamma-ray spectrometer comprising an array of high-purity n-type germanium (HPGe) detectors surrounded by an active NaI(T1) collimator and Compton suppressing anticoincidence shield was flown on May 29-30, 1987. The average column depth of residual atmosphere in the direction of SN 1987A at float altitude was 6.3 g/sq cm during the observation. The 3-sigma upper limit obtained for the 1238-keV line from Co-56 is 0.0013 photons/sq cm s. The corresponding limit for the 847-keV line is 0.0017 photons/sq cm s.

Sandie, W. G.

Gamma ray spectrometry of LDEF samples at SRS

A total of 31 samples from Long Duration Exposure Facility (LDEF), including materials of Al, V, and steel trunnions were analyzed by ultralow level gamma spectrometry. The study quantified particle induced activations of Na-22, Sc-46, Cr-51, Mn-54, Co-56, Co-57, Co-58, and Co-60. The samples of trunnion sections exhibited increasing activity toward the outer end of the trunnion and decreasing activity toward its radial center. The trunnion sections did not include an end piece that collects noticeable Be-7 on its leading surface. No significant Be-7 was detected in the samples analyzed. The most sensitive analyses were performed with a 90 pct. efficient HPGe gamma ray detector, which is enclosed in a purged active/passive active shield.

Winn, Willard G.

Continuum Background in Space-Borne Gamma-Ray Detectors

The background measured with space-borne gamma-ray spectrometers (GRS) in the 100 keV-10 MeV energy region consists of both discrete lines and continuum. The discrete lines originate in the decay of radioactive species. The continuum originates from a number of different processes and can be an important factor in the detection, for example, of weak gamma-ray lines from a planetary surface. Measurements of the gamma-ray background have been made during the cruise portion of a number of planetary missions. The three missions described here are the Apollo 15 and 16 missions each of which carried a 7 cm x 7 cm NaI scintillation detector, the Mars Observer (MO) mission which used a 5.5 cm X 5.5 cm high-purity germanium (HPGe) detector, and the Near Earth Rendezvous Asteroid (NEAR) mission that has a 2.54 cm x 7.6 cm NaI detector. A comparison of the intensity and spectral shape of these background spectra can be useful to help understand how these backgrounds vary with spacecraft size, detector position, and detector size. The use of shields to reduce the background components on these three missions is a test of the effectiveness of different shield designs.

Larry G. Evans

Induced radioactivity of LDEF materials and structural components

We present an overview of the Long Duration Exposure Facility (LDEF) induced activation measurements. The LDEF, which was gravity-gradient stabilized, was exposed to the low Earth orbit (LEO) radiation environment over a 5.8 year period. Retrieved activation samples and structural components from the spacecraft were analyzed with low and ultra-low background HPGe gamma spectrometry at several national facilities. This allowed a very sensitive measurement of long-lived radionuclides produced by proton- and neutron-induced reactions in the time-dependent, non-isotropic LEO environment. A summary of major findings from this study is given that consists of directionally dependent activation, depth profiles, thermal neutron activation, and surface beryllium-7 deposition from the upper atmosphere. We also describe a database of these measurements that has been prepared for use in testing radiation environmental models and spacecraft design.

NASA Discipline Radiation Health

Development of a Quasi-monoenergetic 6 MeV Gamma Facility at NASA Goddard Space Flight Center

The 6 MeV Gamma Facility has been developed at NASA Goddard Space Flight Center (GSFC) to allow in-house characterization and testing of a wide range of gamma-ray instruments such as pixelated CdZnTe detectors for planetary science and Compton and pair-production imaging telescopes for astrophysics. The 6 MeV Gamma Facility utilizes a circulating flow of water irradiated by 14 MeV neutrons to produce gamma rays via neutron capture on oxygen (O-16(n,p)N-16 yields O-16* yields O-16 + gamma). The facility provides a low cost, in-house source of 2.742, 6.129 and 7.117 MeV gamma rays, near the lower energy range of most accelerators and well above the 2.614 MeV line from the Th-228 decay chain, the highest energy gamma ray available from a natural radionuclide. The 7.13 s half-life of the N-16 decay allows the water to be irradiated on one side of a large granite block and pumped to the opposite side to decay. Separating the irradiation and decay regions allows for shielding material, the granite block, to be placed between them, thus reducing the low-energy gamma-ray continuum. Comparison between high purity germanium (HPGe) spectra from the facility and a manufactured source, Pu-238/C-13, shows that the low-energy continuum from the facility is reduced by a factor approx. 30 and the gamma-ray rate is approx.100 times higher at 6.129 MeV.

NASA

Investigation of Deuterium Loaded Materials Subject to X-Ray Exposure

Results are presented from an exploratory study involving x-ray irradiation of select deuterated materials. Titanium deuteride plus deuterated polyethylene, deuterated polyethylene alone, and for control, hydrogen-based polyethylene samples and nondeuterated titanium samples were exposed to x-ray irradiation. These samples were exposed to various energy levels from 65 to 280 kV with prescribed electron flux from 500 to 9000 μA impinging on a tungsten braking target, with total exposure times ranging from 55 to 280 min. Gamma activity was measured using a high-purity germanium (HPGe) detector, and for all samples no gamma activity above background was detected. Alpha and beta activities were measured using a gas proportional counter, and for select samples beta activity was measured with a liquid scintillator spectrometer. The majority of the deuterated materials subjected to the microfocus x-ray irradiation exhibited postexposure beta activity above background and several showed short-lived alpha activity. The HPE and nondeuterated titanium control samples exposed to the x-ray irradiation showed no postexposure alpha or beta activities above background. Several of the samples (SL10A, SL16, SL17A) showed beta activity above background with a greater than 4σ confidence level, months after exposure. Portions of SL10A, SL16, and SL17A samples were also scanned using a beta scintillator and found to have beta activity in the tritium energy band, continuing without noticeable decay for over 12 months. Beta scintillation investigation of as-received materials (before x-ray exposure) showed no beta activity in the tritium energy band, indicating the beta emitters were not in the starting materials.

x-ray irradiation

Contamination, Transportation or Transmutation in LENR Material Analyses

LENR experiments using various loading and triggering mechanisms rely on a variety of elemental and isotopic assays to determine LENR effects. These assays include optical microscopy, Scanning Electron Microscopy with Energy Dispersive X-Ray Analysis (SEM/EDX), X-Ray Photoelectron Spectroscopy (XPS) and Transmission Electron Microscopy (TEM). All of these methods observe the surface of a material. By dissolving or vaporizing the sample, Inductively Coupled Plasma Optical Element Spectroscopy (ICP-OES) can determine elemental composition (ppb) or with mass spectroscopy, isotopes (ICP/MS). One can use a focused ion beam (FIB) to cut open a sample and observe the “cut” with either SEM/EDX, or Time-of-Flight Secondary Ion Mass Spectroscopy (TOF-SIMS). High Purity Gamma Ray Spectroscopy (HPGe) and alpha/ beta Liquid Scintillator spectroscopy can be used. We’ve employed these assay methods in our NASA GRC research under both the Advanced Energy Conversion and Lattice Confinement Fusion Projects. However, there are limitations associated with each of these methods ranging from handling contamination, instrumental limitations including sensitivity and field of view, and sample preparation.

Low Energy Nuclear Reactions

Results of South-East Flux Trap Dosimetry Measurements for the Advanced Test Reactor Critical Facility in support of Advanced Sensors and Instrumentation Development

Reactor dosimetry measurements are commonly used to validate simulation and modeling in nuclear reactor tests. Numerous standard dosimeter materials exist which are commonly utilized with sensitivities to different energy ranges of neutrons. At the Advanced Test Reactor (ATR), cobalt alloy and pure nickel wires are installed every cycle to monitor thermal- and fast-neutron fluence rates. However, there is growing interest in exploring less commonly used materials which are either more sensitive to different parts of the neutron energy spectrum or which can incorporate multiple activation paths in a single material. Epithermal and fast-neutron energies beyond the typical 1-MeV threshold are of particular interest. Two ATR-C Flux Runs took place during 2024; each flux run included supplemental dosimetry packages in the South-East Flux Trap (SEFT) Filler. The focus of the dosimetry package for flux run 23-4 was to test two novel dosimetry methods that can provide simultaneous thermal and threshold (fast) sensitivity in a single dosimeter wire. A selection of 3% Au in Cu alloyed wires were available that provided sensitivity to fast and thermal neutrons through 5 different reactions. Likewise, Fe offers multiple interaction pathways with sensitivity to both thermal and fast neutrons. The main question to be answered by these irradiations was if sufficient radioactivation would take place in the ATR-C SEFT during a nominal 20-minute irradiation at typical power levels (near 600Wth) to observe the threshold reactions that have smaller activation cross-sections than the thermal reactions without being saturated by interfering interactions and Compton continuum during the High-Purity Germanium (HPGe) measurements. The results from comparing the measurement results to anticipated activity levels provide confidence in our ability to activate both traditional and novel dosimetry materials in ATR-C, however not all the measured values matched with the predicted activities. This leaves further room for investigation both on the experimental and computational approaches for future irradiation experiments.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN