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Gamma & Neutron Field-Data Recommendations [Slides]

Summary: The three spectra types desired are: IPC, background, known source; Source-to-detector distance should be stated clearly and photographed if possible; 300 sec is the minimum desired count time; A background spectrum provides a baseline against which to compare the IPC spectrum; Photographs and an event / scenario description can provide situational awareness

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Thorium-uranium fission radiography

Results are described for studies designed to develop routine methods for in-situ measurement of the abundance of Th and U on a microscale in heterogeneous samples, especially rocks, using the secondary high-energy neutron flux developed when the 650 MeV proton beam of an accelerator is stopped in a 42 x 42 cm diam Cu cylinder. Irradiations were performed at three different locations in a rabbit tube in the beam stop area, and thick metal foils of Bi, Th, and natural U as well as polished silicate glasses of known U and Th contents were used as targets and were placed in contact with mica which served as a fission track detector. In many cases both bare and Cd-covered detectors were exposed. The exposed mica samples were etched in 48% HF and the fission tracks counted by conventional transmitted light microscopy. Relative fission cross sections are examined, along with absolute Th track production rates, interaction tracks, and a comparison of measured and calculated fission rates. The practicality of fast neutron radiography revealed by experiments to data is discussed primarily for Th/U measurements, and mixtures of other fissionable nuclei are briefly considered.

Haines, E. L.↗

Prompt Photofission Neutron Detection in Depleted Uranium

The detection of prompt photofission neutrons during active interrogation is a strong indication of the presence of special nuclear materials. However, the high-energy photons used for interrogation create a very challenging radiation environment for the detection of prompt fission signatures. These challenges include detector saturation and pulse pile-up. Additionally, there is an elevated neutron background that further challenges the detection of prompt fission neutrons. This background is produced because of (γ, Xn) photonuclear reactions in the surrounding high-Z materials. Here, we demonstrate the detection of prompt photofission neutrons in these challenging environments. Depleted uranium (DU) and lead targets are interrogated with bremsstrahlung photons produced by a 9-MV electron linear accelerator. Fast neutrons are detected with trans-stilbene organic detectors, and scintillation pulses are analyzed using a previously developed and demonstrated artificial neural network system. We observe a 5 times higher photoneutron count rate when the lead target is replaced with the DU target. Additionally, we observe a difference in the photoneutron light-output distributions of lead and DU. Here, this difference in the measured distributions is due to the difference in the photoneutron-energy spectra; DU photoneutrons are emitted with (γ, n) and watt-energy spectra, whereas lead photoneutrons are emitted with only the (γ, n) spectrum.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fork Experiments in the Hot Cell Using Spent Fuel Rods for International Nuclear Safeguards

This work leveraged the rare availability of 25 full-length pressurized water reactor spent fuel rods and 1 irradiated mixed-oxide rod at an Oak Ridge National Laboratory hot cell. This was done to collect measurement data with two Fork detectors to assess the detectors’ capability of verifying operator declaration data and detecting partial defects in spent fuel, which are the two primary goals of international safeguards on spent nuclear fuel. The data can also be used to benchmark the ORIGEN module, which has been adopted in the International Atomic Energy Agency’s (IAEA’s)/European Atomic Energy Community’s (Euratom’s) Integrated Review and Analysis Program to predict the Fork detector count rates in real time. In this project, the authors first calibrated two Fork detectors—a standard one and a modified one—by using known strong neutron and gamma sources. Then, the authors measured all 26 fuel rods at multiple locations along the length. The fuel rods were then assembled into three arrays—2 × 2, 3 × 3, and 5 × 5—by using specially designed support grids to mimic fuel assemblies and measure the arrays with both detectors. For the 5 × 5 array, 4 and 8 fuel rods of the array were replaced in two separate cases with short stainless-steel rods to mimic two partial defect scenarios, and the arrays were measured before and after the replacements. Polyethylene blocks were used in this experiment to mimic water. The results show that the Fork detectors were able to verify operator declarations and detect partial defects in spent fuel, and the authors were the first to demonstrate this through experiments. A discovery was also made that determined the root cause of the nonlinear response to gamma dose in the ion chambers used in IAEA and Euratom’s Fork detectors. After the experiments, both detectors were retrieved from the hot cell for future use. The data collected in this project will be used in a parallel International Nuclear Safeguards Engagement Program (INSEP) project to enhance the safeguards in the Finnish spent fuel encapsulation plant, and the data will be useful to other projects in the future given the increased safeguards needs due to spent fuel transfer and disposal activities worldwide.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A photon-phreak digs the LDEF happening

Radioactivities of the LDEF onboard experiments induced by gamma emitting rays in both intentional samples and spacecraft parts were examined. The long time greatly enhanced the ability to detect some of the longer lived nuclides, including: 2.6 yr Na-22 in Al and Fe; 5.3 yr Co-60 in Co, Ni, and In; 2.9 yr Rh-102 in In; and 38 yr Bi-207 in Pb. These radionuclides, along with such other as 33 yr Ar-42 in Ti, Fe, or Ni and 47 yr Ti-44 in the same elements, would be appropriate monitors of the high energy space radiation field on long round-trip voyages in the solar system. Additional candidate radionuclides are also discussed. Radiometric analysis of the LDEF samples was a substantial effort among a dedicated group of experts in low level counting, and highlights several important aspects of the procedures needed to achieve success in this kind of endeavor. Target elements should be chosen to differentiate between neutron and proton induced reactions, whenever this is feasible. Reactions should be chosen with a wide range of energy thresholds, to enable calculation of both intensity and energy spectra of the particle fluxes.

Smith, Alan R.↗

A Short-Lived Isotope Counting System (SLICS) to measure reaction cross sections producing light, beta-decaying nuclei on OMEGA

A new activation detector optimized for short-lived isotopes was designed, installed, and tested on OMEGA. The Short-Lived Isotope Counting System (SLICS) can be positioned as close as 35 cm from the OMEGA target chamber center in a ten-inch-manipulator. Stable target samples can be mounted on the front end of the detector assembly to undergo triton-, deuteron-, or neutron-induced reactions that produce short-lived reaction products that beta decay. The emitted betas are detected in a phoswich configuration to eliminate the gamma background. The detector is optimized for isotopes with half-lives from 150 ms to 20 s, filling a gap in OMEGA’s current activation detectors for isotopes with half-lives >5 min. In a pilot study, SLICS achieved an efficiency of 24.5% ± 2.0% for counting 8Li, with a total of 505.8 ± 4.4 qualifying events. Using the existing triton laser-ion acceleration platform on OMEGA, this detector can be used to measure rarely studied tritium-induced reactions on light nuclei with an estimated uncertainty of 12%. As a result, the design of the detector and its performance during a first experiment employing deuterium as a surrogate will be discussed.

Beta spectrometry↗

Altered morphology and diffusivity of water confined in MXenes: Machine learning–accelerated computations combined with experiments

Nanoconfined water exhibits unique properties compared to bulk water due to limited quantities, frustrated hydrogen bonding, and surface interactions, which are fundamental for energy storage and transport applications. We integrate machine learning–accelerated ab initio molecular dynamics with x-ray diffraction (XRD) and inelastic neutron scattering (INS) to systematically analyze the thermodynamic and dynamic behavior of water confined between functionalized (-F, -O, and -OH) two-dimensional (2D) Ti 3 C 2 T x MXene layers. As water intercalates between layers, the interlayer spacing exhibits layer-dependent staging characteristics. The water polarization can be flipped by the count and morphology of intercalated molecules interacting with MXene surface groups, resulting in varying electrostatic potential profiles. On the basis of interfacial electrostatic potential, hydrogen bond lifetime, and molecular orientation, we establish a linear combination of exponential model describing water diffusivity. These computational insights align well with experimental x-ray and neutron measurements, suggesting strategies for tuning water morphology and transport by tailoring MXene surface chemistry and water content for electrochemical energy storage and nanofluidic applications.

Tang, Jiawei [Southeast Univ., Nanjing (China)] (O↗

Thermal Cross Section Measurements At The RPI LINAC

Recently, a cold moderator was designed and developed for use at the Rensselaer Polytechnic Institute Linear Accelerator (RPI LINAC). This cold moderator proved to easily and safely couple to an existing neutron producing target, while enhancing neutron flux below 0.02 eV by up to a factor of 8 by cooling polyethylene down to 29 K. This cold moderator capability allowed for significantly improved counting statistics below 0.02 eV not previously possible due to a poor signal to background ratio. Additionally, testing was performed to characterize the energy resolution of the new cold moderator system and found the system easily capable of resolving resonances in Ta-181 at 4 and 10 eV, while also clearly resolving the Bragg edges found in Be metal below 0.01 eV. Furthermore, following the design and development of a cold polyethylene moderator, a series of thermal total cross section measurements were performed for polyethylene, polystyrene, Plexiglas and yttrium hydride in the thermal region. These measurements serve to help validate thermal scattering law (TSL) evaluations in the 0.0005 – 1 eV energy range. For polyethylene and polystyrene, two sets of experiments were performed – one with the Enhanced Thermal Target (ETT) and another with the ETT plus the new cold moderator capability (ETTC). The yttrium hydride and Plexiglas measurements were only performed with the ETTC. The measurements for polyethylene help to validate the data processing methodology when using the ETTC, while extending the measured range of polyethylene down to 0.0005 eV. Two different Plexiglas, Plexiglas G and Plexiglas G-UVT, and two different concentrations of yttrium hydride, H/Y = 1.85 and 1.68, were measured. Overall, all materials had generally good agreement with their ENDF/B-VIII.0 TSL evaluations, though some discrepancies were noticed. In the case of the yttrium hydride, the high energy oscillations in the hydrogen cross section and the low energy Bragg edges in the yttrium cross section were clearly seen. These measurements represent the first total cross section measurements that encompass the entire thermal region from 0.0005 – 1 eV for polystyrene and yttrium hydride.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Verification of Arms Control Treaties with Resonance Phenomena

Nuclear disarmament treaties remain insufficient to neutralize the existential threat of the nuclear weapons. Technologies are necessary for verifying the authenticity of the nuclear warheads undergoing dismantlement before counting them toward a treaty partner’s obligation. Here we present a review of concepts involving isotope-specific resonance processes, Nuclear Resonance Fluorescence (NRF) [1] and Neutron Resonance Transmission Analysis (NRTA) [2, 3], used to authenticate a warhead’s fissile components by comparing them to a previously authenticated template. All information is encrypted in the physical domain by the addition of an encrypting filter to the target, leading to measurements with an outcome similar to an equation with two unknowns. Using Monte Carlo simulations and experiments we show that the measurements readily detect hoaxing attempt, while no vital isotopic or geometric information about the weapon is released. These nuclear techniques can be used to dramatically increase the reach and trustworthiness of future nuclear disarmament treaties.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Pulse profile modelling of thermonuclear burst oscillations – II. Handling variability

ABSTRACT Pulse profile modelling is a relativistic ray-tracing technique that can be used to infer masses, radii, and geometric parameters of neutron stars. In a previous study, we looked at the performance of this technique when applied to thermonuclear burst oscillations from accreting neutron stars. That study showed that ignoring the variability associated with burst oscillation sources resulted in significant biases in the inferred mass and radius, particularly for the high count rates that are nominally required to obtain meaningful constraints. In this follow-on study, we show that the bias can be mitigated by slicing the bursts into shorter segments where variability can be neglected, and jointly fitting the segments. Using this approach, the systematic uncertainties on the mass and radius are brought within the range of the statistical uncertainty. With about 106 source counts, this yields uncertainties of approximately 10 per cent for both the mass and radius. However, this modelling strategy requires substantial computational resources. We also confirm that the posterior distributions of the mass and radius obtained from multiple bursts of the same source can be merged to produce outcomes comparable to that of a single burst with an equivalent total number of counts.

Astronomy & Astrophysics↗

Study of activation of metal samples from LDEF-1 and Spacelab-2

The activation of metal samples and other material orbited onboard the Long Duration Exposure Facility (LDEF) and Spacelab-2 were studied. Measurements of the radioactivities of spacecraft materials were made, and corrections for self-absorption and efficiency were calculated. Activation cross sections for specific metal samples were updated while cross sections for other materials were tabulated from the scientific literature. Activation cross sections for 200 MeV neutrons were experimentally determined. Linear absorption coefficients, half lives, branching ratios and other pertinent technical data needed for LDEF sample analyses were tabulated. The status of the sample counting at low background facilities at national laboratories is reported.

Laird, C. E.↗

Gamma Spectroscopy Detector Candidates and Radioisotope Identification Algorithms for Use in National Security Applications

In 2006, the United States Congress mandated for the Department of Homeland Security (DHS) to screen all cargo containers to protect against terrorist acts and ensure the safety and security of the nation. Containers are screened by gamma and neutron detectors to ensure threat material is not smuggled into the country. However, because commerce is radioactive, detecting the presence of radioactive materials is not sufficient in ensuring the safety and security of the nation. Radioactive materials must also be identified in real time, thus distinguishing threat sources (Uranium-235 and Plutonium-230) from non-threat sources (kitty litter, pot ash, medical isotopes). Screening cargo containers can be considered a two-step process (1) alerting to the presence of radioactive material when gamma counts exceed a threshold setting, and (2) once alerted, identifying the type of radioactive material, which is done by collecting a gamma spectra and analyzing it with an analysis tool/algorithm. For this reason, it is important to evaluate not only emerging technology in neutron and gamma detection, but also investigate new advances in algorithm development for radioisotope identification (RIID). New candidates in detection and on-board algorithm analysis might offer opportunities to make the scanning, detection, and identification process more efficient while still ensuring the health and safety of the public. This research will investigate emerging technology in radiation detection focused on gamma spectroscopy capabilities and RIID algorithms for DHS applications.

61 RADIATION PROTECTION AND DOSIMETRY↗

Apollo 17 mission Report. Supplement 6: Calibration results for gamma ray spectrometer sodium iodide crystal

A major difficulty in medium energy gamma-ray remote sensing spectroscopy and astronomy measurements was the high rate of unwanted background resulting from the following major sources: (1) prompt secondary gamma-rays produced by cosmic-ray interactions in satellite materials; (2) direct charged-particle counts; (3) radioactivity induced in the detector materials by cosmic-ray and trapped protons; (4) radioactivity induced in detector materials by the planetary (e.g., earth or moon) albedo neutron flux; (5) radioactivity induced in the detector materials by the interaction of secondary neutrons produced throughout the spacecraft by cosmic-ray and trapped proton interactions; (6) radioactivity induced in spacecraft materials by the mechanisms outlined in 3, 4, and 5; and (7) natural radioactivity in spacecraft and detector materials. The purpose of this experiment was to obtain information on effects 3, 4, and 5, and from this information start developing calculational methods for predicting the background induced in the crystal detector in order to correct the Apollo gamma-ray spectrometer data for this interference.

Dyer, C.↗

Analysis of Gamma-Ray Data from Solar Flares in Cycles 21 and 22

One of our primary accomplishments under grant NAGW-35381 was the systematic derivation and compilation, for the first time, of physical parameters for all gamma-ray flares detected by the SMM GRS during its ten year lifetime. The flare parameters derived from the gamma-ray spectra include: bremsstrahlung fluence and best-fit power-law parameters, narrow nuclear line fluence, positron annihilation line fluence, neutron capture line fluence, and an indication of whether or not greater than 10 MeV emissions were present. We combined this compilation of flare parameters with our plots of counting rate time histories and flare spectra to construct an atlas of gamma-ray flare characteristics. The atlas time histories display four energy bands: 56-199 kev, 298526 keV, 4-8 MeV, and 10-25 MeV. These energy bands respectively measure nonrelativistic bremsstrahlung, trans-relativistic bremsstrahlung, nuclear de-excitation, and ultra-relativistic bremsstrahlung. The atlas spectra show the integrated high-energy spectra measured for all GRS flares and dissects them into electron bremsstrahlung, positron annihilation and nuclear emission components. The atlas has been accepted for publication in the Astrophysical Journal Supplements and is currently in press. The atlas materials were also supplied to the Solar Data Analysis Center at Goddard Space Flight Center and were made available through a web site at the University of New Hampshire. Since a uniform methodology was adopted for deriving the flare parameters, this atlas will be very useful for future statistical and correlative studies of solar flares-three independent groups are presently using it to correlate interplanetary energetic particle measurements with our gamma-ray measurements. A better model for the response of the GRS instrument to high energy radiation was also developed. A refined response model was needed because the old model was not adequate for predicting the first and second escape peaks associated with strong nuclear lines nor could it accurately describe the Compton continuum shape. The new response was developed using a GEANT based simulation code and tested against preflight calibration data. The refinement of the response model and the removal of systematic errors now allow more detailed spectral studies of the GRS gamma-ray measurements. This refined response function was supplied to the Solar DAC at Goddard and was also made available via a web site at the University of New Hampshire.

Vestrand, W. Thomas↗

Associated Particle Imaging of Neutron Inelastic Scatter: 3-D Reconstruction, Capabilities, and Challenges

Associated particle imaging (API) offers unique advantages for 3-D imaging of neutron inelastic scatter, including single-view tomographic imaging and data acquisition when access is limited to only one side of the interrogated object. However, widespread adoption of neutron inelastic scatter imaging has been impeded by several inherent challenges, most prominently spatial resolution, self-attenuation, and statistical noise. Here, in this work, the capabilities and challenges of neutron inelastic scatter imaging are investigated. Instead of focusing on a single imaging application, we identify imaging principles that hold for various neutron inelastic scatter imaging techniques. The primary challenges for 3-D imaging are characterized. The inherent spatial resolution in the time-of-flight (TOF) dimension is derived based on the known system timing resolution and scan geometry. Three reconstruction algorithms are described and demonstrated, including the introduction of modern iterative reconstruction incorporating a physics-based system model. Simulation is leveraged to demonstrate imaging capability with varying coincidence count levels and system timing resolution. An example of measured data with both back-scatter and forward-scatter detector positioning is presented. System design characteristics and their effects on image quality are identified. The imaging framework presented in this article has the potential to facilitate growth of 3-D neutron inelastic scatter API by identifying applications that are a good match for the technique and by targeting system development resources toward the requirements of a specific imaging task.

Associated particle imaging (API)↗

The Resource Prospector Neutron Spectrometer System: RP's Bloodhound

The primary goal of the Resource Prospector Neutron Spectrometer System (NSS) is to locate and characterize hydrogen-bearing volatile deposits, especially subsurface ice, that may exist at the lunar poles. A key objective is to detect water-equivalent hydrogen concentrations of 0.5 wt% or greater while on a moving rover. A second objective is to determine approximate burial depth of enhanced hydrogen-bearing materials up to 1 meter below otherwise dry regolith. The instrument will be carried aboard a landed mobility system at the lunar poles. The instrument operates by measuring the changes in the leakage flux of low energy neutrons out of the regolith. These neutrons are produced by galactic cosmic rays, which are so energetic that they shatter the nuclei in surface materials. The neutrons interact with other nuclei and lose energy, becoming thermalized in the process. Hydrogen is most efficient at thermalizing neutrons owing to protons' similar mass - statistically, neutrons lose half their energy per collision with protons. With hydrogen in the soil, leakage fluxes of neutrons in the 0.5 eV to 500 keV energy range are reduced. A concentration of only1-2 wt% water-equivalent hydrogen results in a decrease in epithermal leakage flux of a factor of two. The leakage flux of thermal neutrons, from 0 to 0.5 eV in energy, can either increase or decrease depending on the hydrogen abundance and stratigraphy. As with the highly successful Lunar Prospector Neutron Spectrometer, the RP NSS detects both thermal and epithermal neutrons by using two helium-3 gas proportional counters, one covered by cadmium and the other uncovered. The former detects only epithermal neutrons with energies above approximately 0.5 eV, the latter detects both thermal (less than 0.5 eV) and epithermal energies (greater than 0.5 eV). When a neutron enters the detector tube and interacts with a helium-3 nucleus, the resulting reaction produces an energetic proton and triton that ionize the gas. The resulting electrons are accelerated toward a high-voltage anode and cascade, amplifying the net charge, which is collected at the anode. The number of electrons produced is proportional to the energy that the triton and proton deposit in the gas. A charge sensitive pre-amplifier converts the total charge to a step voltage output. A shaper amplifier then shapes this step into a uni-polar waveform with peaking time appropriate for the detection depending on the event rate. The integrated shaped waveform, representing the deposited triton/proton energy, is then measured. A histogram, or pulse height analysis, is performed to record the main capture peak and wall effect pulses. A threshold for detection is also required to limit the low amplitude counting rate such as noise floor. The system electronics consists of 2 modules - the Sensor Module (SM) front-end and the Data Processing Module (DPM) back-end circuits. SM is designed as a light-weight and low power front-end housing the two helium-3 proportional counter detectors, preamp and HVPS. It is mounted external to the rover body to detect the thermalized neutron flux with a minimum of host background. The DPM is located inside the rover; it digitizes the SM signals, performs pulse height analysis and accumulates the count rate for each spectral channel. The DPM controls high voltage and thresholding, and sends the science data to the host craft via an RS422 serial asynchronous protocol. The payload host provides all thermal management and control for the SM and DPM.

hydrogen-bearing volatile deposits↗

Realistic application of short-lived fission product delayed neutron, gamma-ray analysis for simultaneous nondestructive trace quantification of U, Pu mixtures on cellulose swipes

Detection and characterization of fissile traces are of interest to the international nuclear nonproliferation community, including the International Atomic Energy Agency. Pre-inspection check samples are analyzed by neutron activation analysis at the High Flux Isotope Reactor operated by the Oak Ridge National Laboratory under the umbrella of the IAEA Network of Analytical Laboratories. The simultaneous quantification of U and Pu mixtures was accomplished using the combined delayed neutron (DN) delayed gamma-ray (DG) method to analyze cellulose swipes with actinide loading <1ng in a blind field trial. The total fissile quantity was measured by the DN counts and the relative proportions of U, Pu were determined by calibration of the 104 Tc / 141 Ba fission product count ratio using known mixtures. The DNDG method demonstrated high accuracy in flagging the presence of 239 Pu in uranium down to <100 pg mass loading. In conclusion, peak significance tests helped to control false positive Pu flagging and simultaneous quantification of U and Pu loading was accomplished on samples that passed the significance tests.

36 MATERIALS SCIENCE↗

Evolution of Bonding and Magnetism via Changes in Valence Electron Count in CuFe 2– x Co x Ge 2

A series of solid solutions, CuFe 2–x Co x Ge 2 (x = 0, 0.2, 0.4, 0.8, and 1.0), have been synthesized by arc-melting and characterized by powder X-ray and neutron diffraction, magnetic measurements, Mössbauer spectroscopy, and electronic band structure calculations. All compounds crystallize in the CuFe 2 Ge 2 structure type, which can be considered as a three-dimensional framework built of fused MGe6 octahedra and MGe 5 trigonal bipyramids (M = Fe and Co), with channels filled by rows of Cu atoms. As the Co content (x) increases, the unit cell volume decreases in an anisotropic fashion: the b and c lattice parameters decrease while the a parameter increases. The changes in all the parameters are nearly linear, thus following Vegard’s law. CuFe 2 Ge 2 exhibits two successive antiferromagnetic (AFM) orderings, corresponding to the formation of a commensurate AFM structure, followed by an incommensurate AFM structure observed at lower temperatures. Additionally, as the Co content increases, the AFM ordering temperature (TN) gradually decreases, and only one AFM transition is observed for x ≥ 0.2. The magnetic behavior of unsubstituted CuFe 2 Ge 2 was found to be sensitive to the preparation method. The temperature-dependent zero-field 57 Fe Mössbauer spectra reveal two hyperfine split components that evolve in agreement with the two consecutive AFM orderings observed in magnetic measurements. In contrast, the field-dependent spectra obtained for fields ≥ 2 T reveal a parallel arrangement of the moments associated with the two crystallographically unique metal sites. Electronic band structure calculations and chemical bonding analysis reveal a mix of strong M–M antibonding and non-bonding states at the Fermi level, in support of the overall AFM ordering observed in zero field. The substitution of Co for Fe reduces the population of the M–M antibonding states and the overall density of states at the Fermi level, thus suppressing the T N value.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗