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At least 91 records · Page 5

Systems Theory Principles and Complex Systems Engineering Concepts for Protection and Resilience in Critical Infrastructure: Lessons from the Nuclear Sector

Part of the Presidential Policy Directive 21 (PPD-21) (PPD 2013) mandate includes evaluating safety, security, and safeguards (or nonproliferation) mechanisms traditionally implemented within the nuclear reactors, materials, and waste sector of critical infrastructure—including a complex, dynamic set of risks and threats within an all-hazards approach. In response, research out of Sandia National Laboratories (Sandia) explores the ability of systems theory principles (hierarchy and emergence) and complex systems engineering concepts (multidomain interdependence) to better understand and address these risks and threats. Herein, this Sandia research explores the safety, safeguards, and security risks of three different nuclear sector-related activities—spent nuclear fuel transportation, small modular reactors, and portable nuclear power reactors—to investigate the complex and dynamic risk related to the PPD-21-mandated all-hazards approach. This research showed that a systems-theoretic approach can better identify inter-dependencies, conflicts, gaps, and leverage points across traditional safety, security, and safeguards hazard mitigation strategies in the nuclear reactors, materials, and waste sector. Resulting from this, mitigation strategies from applying systems theoretic principles and complex systems engineering concepts can be (1) designed to better capture interdependencies, (2) implemented to better align with real-world operational uncertainties, and (3) evaluated as a systems-level whole to better identify, characterize, and manage PPD-21's all hazards strategies.

42 ENGINEERING↗

The electronic Raman scattering spectrum of PuO 2

Here the Raman spectrum of PuO 2 was measured up to 13,000 cm –1 with three different laser excitation wavelengths spanning the resonance (405 nm), near-resonance (457 nm), and preresonance (514 nm) energy range. Approximately 26 never-before-seen bands were observed between 3500 and 13,000 cm –1 . Given the very high energy of the Raman shifts of these bands and the relative insensitivity of their spectral position to the interrogating laser wavelength, they are believed to arise from an electronic origin. These bands are present in both freshly calcined and radiolytically aged PuO 2 , although a broad luminescence is observed in the aged material, which obscures many of the high frequency features. In situ laser annealing of the material attenuated this luminescence and allowed for clear observation of these never-before-seen spectral features. Discovery of these high-energy bands presents a new way of identifying PuO 2 for nuclear nonproliferation and forensics purposes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Xenon Trapping in Metal-Supported Silica Nanocages

Xenon (Xe) is a valuable and scarce noble gas used in various applications, including lighting, electronics, and anesthetics, among many others. It is also a volatile byproduct of the nuclear fission of uranium. In this work, a novel material architecture consisting of silicate nanocages in contact with a metal surface and an approach for trapping single Xe atoms in these cages is presented. The trapping is done at low Xe pressures and temperatures between 400 and 600 K, and the process is monitored in situ using synchrotron-based ambient pressure X-ray photoelectron spectroscopy. Release of the Xe from the cages occurs only when heating to temperatures above 750 K. A model that explains the experimental trapping kinetics is proposed and tested using Monte Carlo methods. Density functional theory calculations show activation energies for Xe exiting the cages consistent with experiments. This work can have significant implications in various fields, including Xe production, nuclear power, nuclear waste remediation, and nonproliferation of nuclear weapons. The results are also expected to apply to argon, krypton, and radon, opening an even more comprehensive range of applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Frictionless knowledge injection for few-shot learning

Cutting-edge machine learning methods often require large volumes of curated training data, precluding their use in national security problems with rare events in massive datasets. We present a method for incorporating abstract knowledge into models tailored for sparse data. A subject matter expert defines salient concepts using data examples, which are encoded in the model’s embedding space. Models are then trained to respect these concepts. This method enables knowledge injection, yielding effective models with limited labeled data and the ability to assess model sensitivity for subject matter expertise across the nonproliferation mission space, as demonstrated with Raman spectra analysis.

Stomps, Jordan [ORNL] (ORCID:0000000178114479)↗

Measurement uncertainty of rossi-alpha neutron experiments

Rossi-alpha neutron experiments are used to estimate the prompt neutron decay constant of a fissile assembly, a quantity of widespread interest in applications including in nuclear nonproliferation and criticality safety. This work develops a mathematical model to efficiently estimate measurement uncertainty of Rossi-alpha neutron experiments inferred from a two-exponential fit model with histogram binning. The derived uncertainty estimates were validated using repeated Rossi-alpha measurements of a subcritical, 4.5-kg sphere of weapons-grade, alpha-phase plutonium with nickel, copper, tungsten, and polyethylene reflectors. The estimates of uncertainty for the histogram data produced by the model were conservative and agree with the reference uncertainties within noise. The estimates of the prompt neutron decay constant uncertainty agreed with the reference uncertainties within one standard deviation. In conclusion, the proposed model will reduce total measurement times, ultimately reducing operational and procedural costs in application.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

On the Feynman-alpha method for reflected fissile assemblies

The Feynman-alpha method is a neutron noise technique that is used to estimate the prompt neutron period of fissile assemblies. The method and quantity are of widespread interest including in applications such as nuclear criticality safety, safeguards and nonproliferation, and stockpile stewardship; the prompt neutron period may also be used to infer the k eff multiplication factor. The Feynman-alpha method is predicated on time-correlated neutron detections that deviate from a Poisson random variable due to multiplication. Traditionally, such measurements are diagnosed with one-region point kinetics, but two-region models are required when the fissile assembly is reflected. This paper presents a derivation of the two-region point kinetics Feynman-alpha equations based on a double integration of the Rossi-alpha equations, develops novel propagation of measurement uncertainty, and validates the theory. Validation is achieved with organic scintillator measurements of weapons-grade plutonium reflected by various amounts of copper to achieve k eff values of 0.83–0.94 and prompt periods of 5–75 ns. The results demonstrate that Feynman-alpha measurements should use the two-region model instead of the one-region model. The simplified one-region model deviates from the validated two-region models by as much as 10% in the estimate of the prompt neutron period, and the two-region model reduces to the one-region model for small amounts of reflector. The Feynman-alpha estimates of the prompt neutron period are compared to those of the Rossi-alpha approach. The comparative results demonstrate that the Feynman-alpha method is more precise than the Rossi-alpha method and more accurate for k eff < 0.92, whereas the Rossi-alpha method is generally more accurate for higher multiplications. Here, the uncertainty propagation developed in this work should be used for all Feynman-alpha measurements and will therein improve fitting accuracy and appropriate precision estimates.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Isotopic gamma lines for identification of shielding materials

Identifying the constituting materials of concealed objects is crucial in a wide range of sectors, such as medical imaging, geophysics, nonproliferation, national security investigations, and so on. Existing methods face limitations, particularly when multiple materials are involved or when there are challenges posed by scattered radiation and large areal mass. Here we introduce a novel brute-force statistical approach for material identification using high spectral resolution detectors, such as HPGe. The method relies upon updated semianalytic formulae for computing uncollided flux from source of gamma radiation, shielded by a sequence of nested spherical or cylindrical materials. These semianalytical formulae make possible rapid flux estimation for material characterization via combinatorial search through all possible combinations of materials, using a high-resolution HPGe counting detector. An important prerequisite for the method is that the geometry of the objects is known (for example, from X-ray radiography). We demonstrate the viability of this material characterization technique in several use cases with both simulated and experimental data in spherical geometry.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Delayed onset of discontinuous precipitation-based phase transformation in U10Mo alloys doped with Silicon

A uranium-10 wt% molybdenum (U-10Mo) alloy is one of the primary candidates for metallic fuels that would use low-enriched uranium in place of highly enriched uranium, to support nuclear nonproliferation efforts. Optimal performance of a U-based metallic nuclear fuel can be achieved by retaining the high-temperature, body-centered cubic (bcc) allotrope (γ-U) at room temperature, which can be accomplished in the U-10Mo alloy. However, presence of minor alloying elements can influence the final constitution of room-temperature phases in the U10Mo alloy, specifically, formation of α-U phase which results in anisotropic behavior of the fuel in reactor. Further, through a detailed transmission electron microscopy analysis, the present study reports the constituent phases that are present in a U10Mo alloy containing ~0.1 wt% Si after it is subjected to homogenization heat treatment and thermomechanical processing. For comparison, results from an undoped U10Mo alloy are also included. The experimental results reveal that γ-UMo solid solution is the major phase in a hot-rolled, Si-doped U10Mo alloy metallic fuel foil, along with U 2 MoSi 2 C, UC, and U 2 Mo, after isothermal annealing at 460 °C for 10h. In contrast, after the same heat treatment, the undoped U10Mo alloy metallic fuel had formed a noticeable amount of α-U along prior γ-UMo grain boundaries through discontinuous precipitation (DP, area fraction: ~27.9%) with characteristic lamellar morphology, together with γ-UMo, UC, and U 2 Mo. This result indicates that doping with Si could mitigate the DP reaction in U10Mo alloy and prevent formation of undesirable α-U. This work sheds light on optimizing Si-doping–dominated microstructure in U10Mo fuels and facilitates designing and tuning of microstructures of U10Mo alloys for tailoring the final designed performance of the fuel under irradiation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Impacts of future nuclear power generation on the international monitoring system

Many countries are considering nuclear power as a means of reducing greenhouse gas emissions, and the IAEA (IAEA, 2022) has forecasted nuclear power growth rates up to 224% of the 2021 level by 2050. Nuclear power plants release trace quantities of radioxenon, an inert gas that is also monitored under international agreements as a signature of nuclear weapons tests. To better understand how nuclear energy growth (and resulting Xe emissions) could affect this global nonproliferation architecture, we modeled daily releases of radioxenon isotopes used for nuclear explosion detection in the International Monitoring System (IMS) that is part of the Comprehensive Nuclear Test-Ban Treaty: 131m Xe, 133 Xe, 133m Xe, and 135 Xe to examine the change in the number of radioxenon detections as compared to the 2021 detection levels. If a 40-station IMS network is used, the detections of 133 Xe in 2050 would range from 82% for the low-power scenario to 195% for the high-power scenario, compared to the detections in 2021. If an 80-station IMS network is used, the detections of 133 Xe in 2050 would range from 83% of the 2021 detection rate for the low-power scenario to 209% for the high-power scenario. Essentially no detections of 131m Xe and 133m Xe are expected. The high growth scenario could lead to a six-fold increase in 135 Xe detections, but the total number of detections is still small (on the order of 1 detection per day in the entire network).

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Cell design for laser-induced breakdown spectroscopy measurements on reactive gas samples

Uranium hexafluoride (UF 6 ) is the primary material used for the enrichment of uranium in the production of light water nuclear reactor fuels worldwide. Accurate, rapid quantification of uranium isotopic composition in nuclear materials is required for safeguards programs and nonproliferation purposes. One potential technique for isotopic measurements in uranium species in the field is laser induced breakdown spectroscopy (LIBS). Safe and effective application of LIBS to UF 6 for enrichment measurements is uniquely challenging due to the chemical and physical properties of UF 6 , which necessitate specific handling procedures. The objective of this work is to design a cell for isotopic analysis of UF 6 that is (1) compatible with chemical and physical properties of UF 6 , (2) compatible with LIBS laser, and (3) portable-sized for nuclear safeguards applications. Along with cell design, initial testing of the cell for basic performance and chemical compatibility is performed. As designed and constructed, the portable gas cell was gas-tight, chemically compatible with UF 6 , and withstood long-duration laser exposure. In this work, the cell has proven capability for handling reactive gasses, such as UF 6 , with specification application to isotopic analysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Performance of a dynamic single bubbler in single and two-phase immiscible liquids

Ensuring nonproliferation and safeguards of special nuclear materials (SNM) is a critical aspect of advancing the nuclear fuel cycle. Traditional bubbler systems used to estimate liquid levels and densities in nuclear recycling processes have limitations, particularly in harsh environments where dip-tube corrosion and buildup necessitate frequent maintenance and recalibration. This study explores the Dynamic Single Bubbler (DSB) method, which utilizes a single dip-tube attached to a linear actuator to estimate liquid properties dynamically. This approach is extended to estimate liquid-liquid interfaces in immiscible liquids and employs a linear regression method to reduce uncertainties and improve accuracy. The DSB method achieved density estimate uncertainties of less than 0.5% and surface level estimate uncertainties typically under 0.5%, across various fluids including water, acetone, methanol, mineral oil, glycerol, and aqueous salt solutions. Results indicate that the DSB method provides accurate and robust estimates of liquid density and surface levels with minimal maintenance and without the need for calibration. Additionally, the method's applicability to immiscible liquids and various dip-tube geometries was demonstrated, showing promise for widespread use in nuclear and other industrial applications.

98 - NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL↗

Raman and infrared spectra of plutonium (IV) oxalate and its thermal degradation products

For over 80 years, plutonium dioxide has been routinely produced via thermal decomposition of hydrated plutonium(IV) oxalate. Despite the longstanding utility of this process, the chemical structures of starting materials and intermediates produced during this thermal conversion remain ill-defined. To help resolve this uncertainty, we measured high-resolution Raman and infrared spectra of Pu(C 2 O 4 ) 2 ·6H 2 O that was heated to 25, 100, 220, 250, 350, and 450 °C in air. Our measurements show that Pu(C 2 O 4 ) 2 ·6H 2 O has a rich vibrational spectrum with at least 15 Raman bands between 180 cm -1 and 1900 cm -1 and 9 infrared bands between 800 cm -1 and 4000 cm -1 . As Pu(C 2 O 4 ) 2 ·6H 2 O is heated, water is liberated, and the oxalate ligand decomposes to produce plutonium oxycarbide species. When heated to 350 °C or higher, vibrational spectra are consistent with PuO 2 with some residual carbon-containing species. Full vibrational spectra, powder X-ray diffraction, and scanning electron microscopy measurements of Pu(C 2 O 4 ) 2 ·6H 2 O and its thermal degradation products are presented herein along with approximate assignments for observed spectral bands. These data can be used to validate and potentially improve existing computational models that describe the chemical structure of compounds produced during thermal degradation of plutonium (IV) oxalate. Given the utility of plutonium (IV) oxalate in synthesizing plutonium dioxide, these results are expected to provide value in the fields of nuclear fuel processing, nuclear nonproliferation, and nuclear forensics.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Performance of 8 × 8 × 32 and 10 × 10 × 32 mm 3 CdZnTe position-sensitive virtual Frisch-grid detectors for high-energy gamma ray cameras

CdZnTe (CZT) crystals with thicknesses up to 20 mm and diameters up to 75 mm have become available from Redlen Technologies, Inc. for making large-volume gamma-ray detectors. The modified growth and optimized annealing conditions allowed Redlen to minimize the dark current and improve the uniformity of CZT crystals. Two detector designs, pixelated (H3D) and position-sensitive virtual Frisch-grid (VFG), have greatly benefitted from the availability of such big crystals. Encouraging results from testing of 40×40×15 mm 3 pixelated detectors were recently reported by the University of Michigan. In this work, we evaluated the spectroscopic properties of 8×8×32 and 10×10×32 mm 3 crystals configured as position-sensitive VFG detectors. Both digitized waveforms and an analog ASIC were used to read and process the signals from the detectors and test their spectral- and spatial-resolution. The VFG design provides the flexibility to scale-up the dimensions of the detectors for the desired efficiency, while the position information allows for correcting the detectors' response non-uniformity caused by crystal defects and devices geometry, thereby reducing the instrument cost and making them more feasible for emerging applications in gamma-ray astronomy, nonproliferation, portal screening and nuclear safeguards, where large detector arrays are often required.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Validation of the two-region Rossi-alpha model for reflected assemblies

Nuclear criticality safety, nonproliferation and safeguards, emergency response, and stockpile stewardship utilize estimates of the k eff multiplication factor. The value of k eff cannot be directly measured, but it can be inferred from the prompt neutron period. One modality of measuring the prompt neutron period is the Rossi-alpha method, which is predicated on fitting a histogram of detection time differences due to the nonrandom temporal distribution of same-fission-chain neutrons. Recent works have developed the motivation and theory to expand traditional one-region point kinetic models resulting in one-exponential histogram fits to two-region models that result in two-exponential fits. This paper validates the new two-region model using organic scintillator measurements of copper-reflected weapons-grade plutonium (0:83 ≤ k eff ≤ 0:94) and high-density- polyethylene-reflected highly enriched uranium (0:73 ≤ k eff ≤ 0:95). Furthermore, the results show that more thermal systems have shorter prompt neutron periods in the core region due to increased induced-fission probabilities for moderated neutrons. Here, a new parameter introduced by the two- region model is also shown to be correlated to the amount of reflection, and may be used to infer assembly properties such as type and amount of reflector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Short-lived photofission product yields from 238 U and 232 Th at Bremsstrahlung X-ray endpoint energies of 8, 14, and 20 MeV for nuclear forensics isotope production applications

The existing photofission product yield data sets are often based on nuclear models, and limited experimental measurements of these fission product yields have been performed. These experiments resulted in measured cumulative fission product yields (CFPYs) for 238 U and 232 Th for the bremsstrahlung X-ray endpoint energies of 8, 14, and 20 MeV. The half-lives of the reported fission products range from 1.07–40.8 s. This work is motivated by a demonstrated need for novel isotope production methods for nuclear forensics and improved nuclear data to support the nonproliferation community. A high-purity germanium detector and a pneumatic transfer system were employed for measurements of short-lived fission products, collecting data between cycles of accelerator irradiation and measurement.

07 ISOTOPE AND RADIATION SOURCES↗

The effects of low- Z shielding on uranium isotope discrimination using the time-emission profiles of long-lived delayed neutrons

Characteristic radiation signals can often be obscured or distorted by relatively small amounts of shielding, as is the case for highly-enriched uranium (HEU). Methods that can detect and identify special nuclear material (SNM) even in the presence of shielding are therefore of high value in many nuclear security and nonproliferation applications. It has been previously shown that the buildup and decay time profiles of long-lived delayed neutron emission from induced fission are unique and can be used to successfully discriminate between uranium isotopes and infer enrichment without the need for a calibration standard. Because the long-lived delayed neutron precursors exhibit decay times on the order of tens of seconds, their time profiles are not sensitive to the delays associated with scattering or diffusion in shielding materials, which occur on much shorter time scales. The use of capture-based neutron detectors can also mitigate the effects of shielding, because unlike recoil-based detectors, they do not have a low-energy detection threshold, so that neutrons that lose their energy in the shielding are still detectable. In this work, the effects of low-Z shielding on the discrimination of uranium isotopes using delayed neutron time profile measurements are investigated for the first time. Furthermore, the delayed neutron buildup and decay time profiles of polyethylene-shielded HEU and depleted uranium objects are measured using two different capture-gated detector designs. The recorded profiles show good agreement with the shapes predicted from six-group delayed neutron models even with the shielding in place, and the enrichment of the HEU and DU objects was estimated accurately to within 5%. While this method shows potential for discriminating and characterizing extreme cases of enrichment when a moderate amount of shielding is present, simulation results suggest that significant limitations exist for intermediate enrichment levels due to distortions to the delayed neutron time profile caused by neutron reflection in the shielding.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Development of 17 N as a time-tagged neutron source for calibration of large antineutrino detectors

Large antineutrino detectors hold the potential for remote nuclear reactor monitoring and discovery, which is of great interest for nonproliferation and treaty verification applications. Correlated-particle calibration sources are especially useful for large-volume designs based on detection of inverse beta-decay events, as the timing information of the coincident particles improves background rejection and event reconstruction. 17 N is a promising calibration source since it emits beta-correlated delayed neutrons and can be produced relatively easily using high-energy neutrons. In this work, we examine the feasibility of 17 N as a time-tagged calibration source for large antineutrino detectors. 17 N was produced using a DT neutron generator from a water sample enriched in 17 O, and the observed production rates were found to be consistent with previous measurements of the 17 O(n,p) 17 N reaction cross-section. As a result, time-tagging of 17 N delayed neutrons is demonstrated via beta-neutron coincidence measurements conducted using a specialized beta detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radiation effects induced by the energetic protons in 8x8x32 mm3 CdZnTe detectors

We report CdZnTe (CZT) detectors have been used in the past and are being actively considered for future gamma-ray space telescopes. One of the challenges of operating CZT detectors in low Earth orbit is radiation damage caused by energetic protons. Previous studies concluded that fluences of 10 8 -10 9 p/cm 2 are sufficient to cause shifting of peak positions and degradations of energy resolution. Degradation of detectors after proton irradiation has been extensively investigated to determine their radiation resistance limits and performance recovering procedures for their applications in space and nuclear nonproliferation. Here we present the study of radiation effects induced by 100 MeV protons in 3-cm long CdZnTe detectors that we recently proposed for the gamma-ray telescope GECCO. The goal this study is to evaluate the feasibility of using such long CZT detectors in future space missions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗