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Fission with Exotic Nuclei (Abbreviated Report)

Nuclear fission is a key mechanism involved in the synthesis of heavy elements in the Cosmos and is the primary explanation for the stability of superheavy elements. Nevertheless, our knowledge of fission remains extremely fragmented. Most experiments have been conducted only on a tiny number of stable actinide nuclei and are often incomplete, leading to gaps in our basic understanding of the process. For many radioactive isotopes, basic fission data such as the charge or mass distribution of the fragments is unknown. These gaps cannot always be filled by simulation alone. Common fission models contain too many free parameters and lack predictive power. In contrast, the fundamental theory of fission under development at LLNL is much more predictive, but its current computational cost is too high to be used extensively for data evaluations. A unique window of opportunity to resolve these limitations has recently opened: the U.S. nuclear science community is ramping up major experimental programs at the Facility for Rare Isotope Beams (FRIB, the DOE flagship facility in low-energy nuclear science), and techniques from machine learning have shown great potential to simplify the use of a fundamental, quantum-mechanical theory of fission. This project has two components. On the experimental side, we acquired and deployed at the HIGS facility a new dual Frisch-Grid ionization chamber to measure correlated fragment-mass, kinetic energy, and angular distributions of fission fragments from induced fission. This new device was used to perform measurements of charge, mass and total kinetic energy of fission fragments in the photofission of 238 U and eight gamma-ray beam energies between 6.2 and 13 MeV, which allowed extracting high-precision independent yields for this reaction. The device was also used to perform measurements of the same quantities in the neutron-induced fission of 234 U with monoenergetic beams of energy between 5 and 8 MeV. In parallel, we collaborated with a team at Commissariat à l’énergie atomique et aux énergies alternatives (CEA) to perform a series of measurements of fission yields in inverse kinematics for the two isotopes of 236 U and 240 Pu. The experiment took place at the Grand Accélérateur National d’Ions Lourds in France in June 2023. The deployment of the VAMOS spectrometer with a new array called PISTA allowed determining the excitation energy of the fissioning system within 1 Mega-electronvolts. The second component of the project involved using deep neural networks to build fast and reliable emulators of our current fission models. In an invited paper published in Frontier in Physics, we showed that autoencoders could successfully compress nuclear wavefunctions in nuclear density functional theory. We achieved a dimensionality reduction of the order of two orders of magnitude while keeping the error in the total energy to less than 0.01%. In a second paper submitted to Physical Review Letters in June 2023 with our collaborators at CEA, we showed that variational autoencoders can learn the collective degrees of freedom driving the fission process.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Experimental study of ECH pre-ionization on J-TEXT

An experimental study on electron cyclotron heating (ECH) pre-ionization has been conducted on J-TEXT in support of the joint experiment research for ITER plasma initiation. In this experiment, ECH power was injected to the vessel before the application of loop voltage ionize the neutral gas and form the initial plasma or so-called pre-plasma. The impact of several significant factors, such as magnetic field configuration, pre-fill gas pressure, ECH toroidal injection angle and ECH power on the evolution of pre-plasma are systematically studied, aiming to identify shared features, clarify their potential relationship and optimize the discharge parameters to generate a rather high pre-plasma density. By separating ECH power from the inductive start-up, the effect of pre-plasma on tokamak start-up can be observed. A dynamic magnetic configuration facilitates the transition of pre-plasma to tokamak plasma. To assess the influence of pre-plasma density on tokamak start-up, two kinds of magnetic field configurations are examined. While the effect of different pre-plasma densities on tokamak start-up is negligible, a significant difference is observed between pure ohmic start-up and start-up with pre-ionization. The studies presented here show evolutionary trends and threshold values needed to optimize ECH pre-ionization and also a feasible way to improve pre-plasma density and a configuration to stabilize pre-plasma for transition. Eventually, these results may contribute to multi-machine research and physics analysis that can assist ITER with its optimal preparation for first plasma operation.

ECH↗

New loading method for high precision Sm isotope analysis of nuclear materials using thermal ionization mass spectrometry

This work demonstrates an analytical protocol for high precision Sm isotope analysis by thermal ionization mass spectrometry (TIMS) using a Pt activator. Here, the method permits precise measurements of small aliquots (1–20 ng) of Sm on single Re filament using a modified static-total evaporation technique. This study represents the first attempt to use such protocols for Sm isotope analyses while reducing the loading size of Sm for TIMS. The method could potentially be deployed to study geological, meteorites and lunar samples containing low Sm concentrations, to monitor neutron irradiation exposure based on 149,150 Sm, or to measure Sm isotopic composition in other types of nuclear samples.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Single-Cell Metabolic Profiling: Metabolite Formulas from Isotopic Fine Structures in Heterogeneous Plant Cell Populations

Characterization of the metabolic heterogeneity in cell populations requires the analysis of single cells. Most current methods in single-cell analysis rely on cell manipulation, potentially altering the abundance of metabolites in individual cells. Small sample volume and the chemical diversity of metabolites are additional challenges in single-cell metabolomics. Here, we describe the combination of fiber-based laser ablation electrospray ionization (f-LAESI) with 21 tesla Fourier transform ion cyclotron resonance mass spectrometry (21TFTICR-MS) for in situ single-cell metabolic profiling in plant tissue. Single plant cells infected by bacteria were selected and sampled directly from the tissue without cell manipulation through mid-infrared ablation with a fine optical fiber tip for ionization by f-LAESI. Finally, ultrahigh performance 21T-FTICR-MS enabled the simultaneous capture of isotopic fine structures (IFSs) for 47 known and 11 unknown compounds, thus elucidating their elemental compositions from single cells, and providing information on metabolic heterogeneity in the cell population.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Skipper-CCD sensors for the Oscura experiment: requirements and preliminary tests

Oscura is a proposed multi-kg skipper-CCD experiment designed for a dark matter (DM) direct detection search that will reach unprecedented sensitivity to sub-GeV DM-electron interactions with its 10 kg detector array. Oscura is planning to operate at SNOLAB with 2070 m overburden, and aims to reach a background goal of less than one event in each electron bin in the 2–10 electron ionization-signal region for the full 30 kg-year exposure, with a radiation background rate of 0.01 dru.[1 dru (differential rate unit) corresponds to 1 event/kg/day/keV.] In order to achieve this goal, Oscura must address each potential source of background events, including instrumental backgrounds. In this work, we discuss the main instrumental background sources and the strategy to control them, establishing a set of constraints on the sensors' performance parameters. We present results from the tests of the first fabricated Oscura prototype sensors, evaluate their performance in the context of the established constraints and estimate the Oscura instrumental background based on these results.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Investigating PVC polymer–plasticizer interactions with atomistic MD simulations and potential of mean force calculations

For this work, atomistic molecular dynamics (MD) simulations coupled with potential of mean force (PMF) calculations were employed to investigate the interactions between PVC polymer chains containing 6–20 repeating units and various plasticizers, with the goal of identifying potential replacements for the toxic plasticizer di(2-ethylhexyl)phthalate (DEHP) used in blood bags. The selected plasticizers belong to various chemical families, such as orthophthalates, citrates, adipates, and the terephthalate DEHT. Both the polymer and the plasticizers lack ionizable groups, and their interactions are primarily governed by van der Waals and electrostatic forces. A model correlating PMF profiles with interaction forces was developed and validated across polyvinyl chloride (PVC) polymers of different lengths and all investigated plasticizers. This model provides insight into how structural variations in plasticizers influence their respective PMF values. The study ranks the investigated plasticizers based on binding affinity, identifying TOTM (tris(2-ethylhexyl) trimellitate, TEHTM), BTHC (butyryl trihexyl citrate, Citroflex B-6), ATHC (acetyl trihexyl citrate, Citroflex A-6, CA-6), and DEHT (bis(2-ethylhexyl)terephthalate, DOTP/DEHTP) as promising alternatives for further investigation. This comprehensive study encompasses PVC polymers of four different lengths and 14 plasticizers, with all data averaged over 30 independent simulations. The approach provides a deeper understanding of molecular interactions, enabling the tailoring of polymer–plasticizer systems for diverse applications, including extractables and leachables, with relevance spanning materials science to biomedical engineering, and also serves as a basis for developing coarse-grained simulation protocols. Overall, this study provides valuable insights for designing safer and more efficient plasticizer substitutes and is well supported by other studies.

Shet, Sai Athmeeya G. [Sri Sathya Sai Institute of↗

Correlation between the gas-phase metallicity and ionization parameter in extragalactic H II regions

The variations of the metallicity and ionization parameter in H II regions are usually thought to be the dominant factors that produce the variations we see in the observed emission line spectra. There is an increasing amount of evidence that these two quantities are physically correlated, although the exact form of this correlation is debatable in the literature. Simulated emission line spectra from photoionized clouds provide important clues about the physical conditions of H II regions and are frequently used for deriving metallicities and ionization parameters. Through a systematic investigation on the assumptions and methodology used in applying photoionization models, we find that the derived correlation has a strong dependence on the choice of model parameters. On the one hand, models that give consistent predictions over multiple emission-line ratios yield a positive correlation between the metallicity and ionization parameter for the general population of H II regions or star-forming galaxies. On the other hand, models that are inconsistent with the data locus in high-dimensional line ratio space yield discrepant correlations when different subsets of line ratios are used in the derivation. The correlation between the metallicity and ionization parameter has a secondary dependence on the surface density of the star formation rate (SFR), with the higher SFR regions showing a higher ionization parameter but weaker correlations. The existence of the positive correlation contradicts the analytical wind-driven bubble model for H II regions. We explore assumptions in both dynamical models and photoionization models, and conclude that there is a potential bias associated with the geometry. However, this is still insufficient to explain the correlation. Mechanisms that suppress the dynamical influence of stellar winds in realistic H II regions might be the key to solving this puzzle, though more sophisticated combinations of dynamical models and photoionization models to test are required.

79 ASTRONOMY AND ASTROPHYSICS↗

Progenitor and close-in circumstellar medium of type II supernova 2020fqv from high-cadence photometry and ultra-rapid UV spectroscopy

ABSTRACT We present observations of SN 2020fqv, a Virgo-cluster type II core-collapse supernova (CCSN) with a high temporal resolution light curve from the Transiting Exoplanet Survey Satellite (TESS) covering the time of explosion; ultraviolet (UV) spectroscopy from the Hubble Space Telescope (HST) starting 3.3 d post-explosion; ground-based spectroscopic observations starting 1.1 d post-explosion; along with extensive photometric observations. Massive stars have complicated mass-loss histories leading up to their death as CCSNe, creating circumstellar medium (CSM) with which the SNe interact. Observations during the first few days post-explosion can provide important information about the mass-loss rate during the late stages of stellar evolution. Model fits to the quasi-bolometric light curve of SN 2020fqv reveal 0.23 M⊙ of CSM confined within 1450 R⊙ (1014 cm) from its progenitor star. Early spectra (<4 d post-explosion), both from HST and ground-based observatories, show emission features from high-ionization metal species from the outer, optically thin part of this CSM. We find that the CSM is consistent with an eruption caused by the injection of ∼5 × 1046 erg into the stellar envelope ∼300 d pre-explosion, potentially from a nuclear burning instability at the onset of oxygen burning. Light-curve fitting, nebular spectroscopy, and pre-explosion HST imaging consistently point to a red supergiant (RSG) progenitor with $M_{\rm ZAMS}\approx 13.5\!-\!15 \, \mathrm{M}_{\odot }$, typical for SN II progenitor stars. This finding demonstrates that a typical RSG, like the progenitor of SN 2020fqv, has a complicated mass-loss history immediately before core collapse.

Tinyanont, Samaporn (ORCID:0000000214814676)↗

Competing ionization and dissociation: Extension of the energy-dependent frame transformation to the gerade symmetry of H 2

This article solves two major tasks that frequently arise in the theory of electron collisions with a target molecular cation. First, it extends the energy-dependent frame transformation (EDFT) treatment, which is needed to map fixed-nuclei electron-molecule scattering matrices into an energy-dependent laboratory-frame scattering matrix with vibrational channel indices. The EDFT mapping can now be carried out even when the target molecule possesses multiple low-energy potential curves, significantly transcending previous applications. Second, it implements a method to extract the rest of the full laboratory-frame scattering matrix, i.e., the columns and rows describing input and/or output dissociation channels. The treatment is benchmarked in this article against the essentially exact solution of a refined two-dimensional model of the singlet gerade Σ symmetry of H 2 . Our tests demonstrate that the theory accurately maps fixed-nuclei scattering information, of the type provided by existing electron-molecule computer codes, into a laboratory-frame scattering matrix that includes both ionization and dissociation. Furthermore, this treatment can provide a general framework applicable to a broad class of electron collision processes involving diatomic target ions, suitable for an accurate description of challenging processes such as dissociative recombination.

74 ATOMIC AND MOLECULAR PHYSICS↗

Double-Atom Catalysts Featuring Inverse Sandwich Structure for CO 2 Reduction Reaction: A Synergetic First-Principles and Machine Learning Investigation

Electrocatalytic CO 2 reduction reactions (CO 2 RR) based on scalable and highly efficient catalysis provide an attractive strategy for reducing CO 2 emissions. Here in this work, we combined first-principles density functional theory (DFT) and machine learning (ML) to comprehensively explore the potential of double-atom catalysts (DACs) featuring an inverse sandwich structure anchored on defective graphene (gra) to catalyze CO 2 RR to generate C 1 products. We started with five homonuclear M 2 ⊥gra (M = Co, Ni, Rh, Ir, and Pt), followed by 127 heteronuclear MM'⊥gra (M = Co, Ni, Rh, Ir, and Pt, M' = Sc–Au). Stable DACs were screened by evaluating their binding energy, formation energy, and dissolution potential of metal atoms, as well as conducting first-principles molecular dynamics simulations with and without solvent water molecules. Based on DFT calculations, Rh 2 ⊥gra DAC was found to outperform the other four homonuclear DACs and the Rh-based single- and double-atom catalysts of noninverse sandwich structures. Out of the 127 heteronuclear DACs, 14 were found to be stable and have good catalytic performance. An ML approach was adopted to correlate key factors with the activity and stability of the DACs, including the sum of radii of metal and ligand atoms (d M–M' , d M–C , and d M'–C ), the sum and difference of electronegativity of two metal atoms (P M + P M' , P M – P M '), the sum and difference of first ionization energy of two metal atoms (I M + I M' , I M – I M '), the sum and difference of electron affinity of two metal atoms (A M + A M' , A M – A M '), and the number of d-electrons of the two metal atoms (Nd). The obtained ML models were further used to predict 154 potential electrocatalysts out of 784 possible DACs featuring the same inverse sandwich configuration. Overall, this work not only identified promising CO 2 RR DACs featuring the reported inverse sandwich structure but also provided insights into key atomic characteristics associated with high CO 2 RR activity.

30 DIRECT ENERGY CONVERSION↗

Two-Center Interference in the Photoionization Delays of Kr 2

Herein we present the experimental observation of two-center interference in the ionization time delays of Kr 2 . Using attosecond electron-ion-coincidence spectroscopy, we simultaneously measure the photoionization delays of krypton monomer and dimer. The relative time delay is found to oscillate as a function of the electron kinetic energy, an effect that is traced back to constructive and destructive interference of the photoelectron wave packets that are emitted or scattered from the two atomic centers. Our interpretation of the experimental results is supported by solving the time-independent Schrödinger equation of a 1D double-well potential, as well as coupled-channel multiconfigurational quantum-scattering calculations of Kr 2 . This work opens the door to the study of a broad class of quantum-interference effects in photoionization delays and demonstrates the potential of attosecond coincidence spectroscopy for studying weakly bound systems.

74 ATOMIC AND MOLECULAR PHYSICS↗

Phase Diagram of a Deep Potential Water Model

Using the Deep Potential methodology, we construct a model that reproduces accurately the potential energy surface of the SCAN approximation of density functional theory for water, from low temperature and pressure to about 2400 K and 50 GPa, excluding the vapor stability region. The computational efficiency of the model makes it possible to predict its phase diagram using molecular dynamics. Satisfactory overall agreement with experimental results is obtained. Here, the fluid phases, molecular and ionic, and all the stable ice polymorphs, ordered and disordered, are predicted correctly, with the exception of ice III and XV that are stable in experiments, but metastable in the model. The evolution of the atomic dynamics upon heating, as ice VII transforms first into ice VII" and then into an ionic fluid, reveals that molecular dissociation and breaking of the ice rules coexist with strong covalent fluctuations, explaining why only partial ionization was inferred in experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Utilization of the LS-APGD microplasma/orbitrap-FTMS booster system for detection and isotopic analysis of neodymium nanoparticles

Detection and isotopic analysis of particle populations has seen rapid growth across several application areas, including environmental analysis, nuclear forensics, and food safety. The ability to characterize the particles' unique elemental and isotopic fingerprints could provide information related to formation, processing history, and transport. Regarding nuclear forensics, isotopic analysis of particles derived from diverse materials is often used as a tool to trace the origin and processing history. Mass spectrometric-based techniques currently used for particle population analysis often suffer from limited mass resolution, particularly when dealing with real-world samples that are affected by isobaric and polyatomic interferences from the matrix. To address these analytical challenges, we propose a novel method utilizing the liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma ionization source coupled to an ultrahigh resolution Orbitrap mass spectrometer, further enhanced with the FTMS X2T Booster data acquisition and processing unit. The FTMS Booster enables acquisition of extended transient times of up to 3 s, significantly improving mass resolution, thereby reducing or even eliminating the need for prior separation of isobaric or polyatomic interferences. Additionally, the detection of low-abundance isotopes was improved by increasing the signal-to-noise (S/N) ratio. As proof of concept, this study demonstrates the feasibility of the LS-APGD/Orbitrap-FTMS X2T Booster platform for direct analysis using a suspension of well-characterized ∼120 nm neodymium particles. The quality of the isotope ratios values obtained from a few hundred particles were in good agreement with those obtained from homogeneous ionic solutions. These results highlight the potential of the LS-APGD/Orbitrap platform for rapid, accurate, and interference-resilient isotope ratio analysis of particle populations without the need for dissolution and subsequent chemical separations, offering significant advantages for nuclear forensics, safeguards, and environmental applications. The effort here also points to further paths forward, hopefully towards single particle (SP) analysis using microplasma ionization and the ultrahigh resolving power of the Orbitrap mass analyzer.

FTMS X2T booster↗

Chemical ionization mass spectrometry utilizing benzene cations for measurements of volatile organic compounds and nitric oxide

We evaluate the capability of chemical ionization mass spectrometry (CIMS) using benzene cations as reagent ions (benzene CIMS) for detecting atmospheric trace gases. We characterize the ionization pathways and product ion distributions for 27 analytes spanning diverse chemical classes. To interpret the complex ion chemistry involving two reagent ions (C 6 H$^{+}_{6}$ and (C 6 H 6 )$^{+}_{2}$) and multiple ionization pathways (charge transfer, proton transfer, adduct formation, and hydride abstraction), we introduce a thermodynamics-based framework that classifies analytes into three categories based on their ionization energy (IE), relative to those of benzene monomer (9.24 eV) and dimer (8.69 eV). Each class exhibits distinct ionization mechanisms and product ions. Analytes with IE smaller than 8.69 eV (low IE) undergo charge transfer with both reagent ions; analytes with IE between 8.69 and 9.24 eV (mid IE) undergo charge transfer with C 6 H$^{+}_{6}$ and potential adduct formation with (C 6 H 6 )$^{+}_{2}$; analytes with IE larger than 9.24 eV (high IE) could undergo adduct formation, proton transfer, or hydride abstraction. Analytes within each class also show similar sensitivity, enabling sensitivity estimation for compounds lacking calibration standards. In addition to volatile organic compounds (VOCs), benzene CIMS detects nitric oxide (NO) with a detection limit of 5 pptv for 1 min integration time, exceeding the performance of most commercial NOx analyzers. Field deployments in Chicago and St. Louis demonstrate good agreement with reference NO measurements. Isoprene measurements show good agreement with a co-located gas chromatography–photoionization detector (GC-PID) in St. Louis, but exhibit substantial positive bias in Chicago, likely due to interferences from anthropogenic VOCs in the polluted urban environment. These results highlight the potential of benzene CIMS for concurrent measurements of NO, VOCs, and their oxidation products using a single instrument, while also underscoring challenges in complex atmospheric conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

An electrochemical generator for the continual supply of 213 Bi from 225 Ac for use in targeted alpha therapy applications

Bismuth-213 is a radionuclide of interest for targeted alpha therapy and is supplied via a radiochemical generator system through the decay of 225 Ac. Radionuclide generators employ longer lived “parent” radionuclides to routinely supply shorter-lived “daughter” radionuclides. The traditional 225 Ac/ 213 Bi radiochemical generator relies on an organic cation exchange resin where 225 Ac binds to the resin and 213 Bi is routinely eluted. These resins degrade when they absorb large doses of ionizing radiation (>1 × 10 6 Gy/mg), which has been observed when the loading activity of 225 Ac exceeds 2.59*10 9 Bq (70 mCi). Herein we report the development of an electrochemical generator for the supply of 213Bi that has the potential to overcome this limitation. Bismuth-213 spontaneously electrodeposits onto nickel foils in 0.1 M hydrochloric acid at 70 °C. Using this method, we were able to plate an average of 73 ± 4 % of the 213 Bi in solution and obtain a final 213 Bi recovery of 65 ± 8 % in 0.1 M citrate pH 4.5 via reverse electrolysis using titanium as the cathode. The recovered 213Bi had an average radiochemical purity of >99.8 % and was successfully used to radiolabel DOTATATE with an average radiochemical yield of 85.1 % (not optimized).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Radon Photoionization: Project Technical Report

In most low-background physics experiments, radon is a significant and problematic source of background radiation because it is inert and sufficiently long-lived to pervade laboratory spaces. It may be possible to manipulate (and thus mitigate) radon electromagnetically by taking advantage of its relatively low first ionization energy. When considering ambient-temperature gas phases, only iodine is comparable. The other noble gases, and the most important constituents of breathable air (nitrogen and oxygen), all have higher ionization energies; so it may be possible to selectively manipulate radon in a variety of gas streams by ionizing it with an appropriately low-energy source of photons. Radon’s first ionization energy is in the vacuum UV part of the electromagnetic spectrum, which can be produced using a deuterium lamp. In this report, we present our attempts to manipulate radon via UV photoionization in a laboratory setting. This approach has the potential to increase radon removal efficiency from gases and/or to improve the efficiency of radon detectors. Unfortunately, our experiments suggest that either the life-time of a photoionized radon ion (before it re-neutralizes) is too short to be of much practical use and/or that our low-cost UV-photon source was not sufficiently energetic for efficient photoionization of radon.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Sensitivity projections for a dual-phase argon TPC optimized for light dark matter searches through the ionization channel

Dark matter lighter than 10 GeV / c 2 encompasses a promising range of candidates. A conceptual design for a new detector, DarkSide-LowMass, is presented, based on the DarkSide-50 detector and progress toward DarkSide-20k, optimized for a low-threshold electron-counting measurement. Sensitivity to light dark matter is explored for various potential energy thresholds and background rates. These studies show that DarkSide-LowMass can achieve sensitivity to light dark matter down to the solar neutrino fog for GeV-scale masses and significant sensitivity down to 10 MeV / c 2 considering the Migdal effect or interactions with electrons. Requirements for optimizing the detector’s sensitivity are explored, as are potential sensitivity gains from modeling and mitigating spurious electron backgrounds that may dominate the signal at the lowest energies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Assessing high fidelity multi-component models to facilitate safeguards at Gas Centrifuge Enrichment Plants

We report that the International Atomic Energy Agency (IAEA) inspectors routinely carry out environmental sampling (ES) as a verification method. Collection of environmental swipe samples at various locations in Gas Centrifuge Enrichment Facilities (GCEPs) is an important process in detecting misuse of a declared facility and possibly the existence of undeclared nuclear material. These samples are measured for isotopic composition in uranium containing particles by Thermal Ionization Mass Spectrometry (TIMS) or Inductively Coupled Plasma Mass Spectrometry (ICP-MS). Even though ES is highly effective in detecting the absolute value of enrichments and their deviations from the declared values, it cannot explain the cause of those changes. Several potential explanations can serve as possibilities for particles detected above or other than the declared enrichment. These include normal and non-malicious events such as the design of the enrichment cascades, unintentional failures of the machines, or overshoot during startup of a cascade. It can also be the result of deliberate misuse by the facility operators. The primary objective of this work is to understand how these factors affect the enrichments produced by a cascade and quantify anticipated multi-isotopic concentrations for each case. The following methodology is employed to determine signatures at a particular facility. 1) Utilize a new two-dimensional multi-component diffusion code to obtain centrifuge performance data and use that information to design and perform cascade analysis. Compare and contrast the results with previous 1-D radially averaged solutions from the Pancake code. 2) Design a GCEP cascade with the production goal of 19.75% 235 U for each set of machine data above. Investigate two cascade scenarios that include enrichment of natural uranium (NU) feed to 19.75% 235U in a single cascade compared to a two-step process of NU to 5% and then 5% to 19.75%. 3) Simulate the intentional vs. unintentional off-normal scenarios in the cascades to assess the differences in isotopic concentrations. A non-ideal squared-off cascade model developed at the University of Virginia is used to calculate flow rates and isotopic concentrations of the process gas. The analysis is performed using the Rome machine model operated at 600 m/s rotor speed. The upper and lower bounds of normal and abnormal enrichments in a typical facility are used in conjunction with ES results to understand the root causes of such observations.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗