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At least 235 records · Page 13

Correlations between electronic order and structural distortions and their ultrafast dynamics in the single-layer manganite P r 0.5 C a 1.5 Mn O 4

Time-resolved x-ray diffraction experiments on the half-doped single-layered manganite Pr 0.5 Ca 1.5 Mn O 4 are used to monitor the ultrafast photoinduced dynamics of the structural distortion associated with the charge and orbital ordering (CO/OO). As in the nonlayered three-dimensional counterpart, the ordered phase melts in less than 100 fs after 800-nm photoexcitation and subsequently partially recovers due to thermal equilibration of electronic and vibrational systems. Photoexciting Pr 0.5 Ca 1.5 Mn O 4 below the transition temperature of a second structural phase transition that occurs around 146 K (deep inside the CO/OO phase) releases this structural transition, but progresses on a much slower timescale. Finally, this additional reduction of crystal symmetry, which we ascribe to a further tilt of the oxygen octahedra, can thus be considered to be only weakly coupled to CO/OO. Furthermore, static hard-x-ray and resonant soft-x-ray diffraction at the Mn L 2,3 edges experiments identify correlations between structural distortions and electronic order in thermal equilibrium.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Short-Term Inhibition and Long-Term Enhancement of Irreversible Trace Metal Binding to Goethite in Multi-Metal Systems

Iron (oxyhydr)oxide minerals are important sorbents of trace metals in aquatic environments. Adsorption–desorption hysteresis has been documented for trace metals after aging, suggesting that they become incorporated over time. We previously found that ion size controls the extent of irreversible metal binding of single metals to goethite. In this study, we evaluate how the presence of multiple metals influences irreversible binding. Mixed Ni–Zn and Ni–Cd solutions were aged with goethite at pH 7 for 2 days, 30 days, and 60 days, after which isotope exchange experiments were performed to assess the lability of the adsorbed metal pools. After 2 days of aging, Ni and Cd in mixed-metal systems were more labile than in single-metal systems, indicating that competitive adsorption may partially block irreversible binding on short time scales. After 60 days, all three metals had larger irreversibly bound fractions than in single-metal systems. X-ray absorption near-edge structure (XANES) spectroscopy indicates that irreversibly bound fractions correlate with incorporation into goethite. This study demonstrates that pools of coadsorbed metals are bioaccessible on a time scale of minutes. Cooperative effects promote the structural sequestration of even large trace metals, causing reactive transport models to likely overpredict metal mobility. Long-term metal entrapment processes hinder micronutrient availability, impact contaminant sequestration and critical mineral recovery, and yield complex pathways through which metal solubilization may be enhanced or hindered during redox cycling.

58 GEOSCIENCES↗

Visualizing diverse lithium growth and stripping behaviors in anode-free solid-state batteries with operando X-ray tomography

Anode-free solid-state batteries (SSBs), which eliminate the need for lithium metal use during cell assembly, have the potential to enable high energy densities and simplified manufacturing. However, the factors that control lithium growth/stripping at the anode current collector are not well understood. Here, we use operando X-ray microcomputed tomography to comprehensively image and quantify lithium deposition and stripping under various conditions in three different Li|Li 6 PS 5 Cl|current collector cells, revealing diverse behavior that depends on interface morphology, cell resistance, and solid-state electrolyte (SSE) microstructure. A cell with high resistance exhibits extensive lithium filament growth across the entire current collector interface, with filaments that grow around pre-existing pores in the SSE rather than lithium filling these pores. Lithium filament formation is partially reversible, with the cracks shrinking as lithium metal is stripped. Uniform lithium deposition is achievable at low current densities in low-resistance cells, whereas higher current densities in these cells cause an increase in interfacial roughness, which is correlated with subsequent filamentary growth at the edges of the cell. These results provide insight into filamentary vs. planar lithium growth and highlight that the evolution of lithium is sensitively dependent on SSE microstructure and electrochemical processes.

25 ENERGY STORAGE↗

High-resolution infrared spectroscopy of jet cooled CH 2 Br radicals: The symmetric CH stretch manifold and absence of nuclear spin cooling

Direct laser absorption of a slit supersonic discharge expansion provides the first high-resolution spectroscopic results on the symmetric CH stretch excitation (ν 1 ) of the bromomethyl (CH 2 Br) radical in the ground electronic state. Narrowband (<1 MHz) mid-infrared radiation is produced by difference-frequency generation of two visible laser beams, with the open shell halohydrocarbon radical generated by electron dissociative attachment of CH 2 Br 2 in a discharge and rapidly cooled to T rot = 18 ± 1 K in the subsequent slit-jet supersonic expansion. A rovibrational structure in the radical spectrum is fully resolved, as well as additional splittings due to spin-rotation effects and 79 Br/ 81 Br isotopologues in natural abundance. Spectroscopic constants and band origins are determined by fitting the transition frequencies to a non-rigid Watson Hamiltonian, yielding results consistent with a vibrationally averaged planar radical and an unpaired electron in the out-of-plane p π orbital. Additionally, extensive satellite band structure from a vibrational hot band is observed and analyzed. The hot band data is compared to CFOUR/VPT2 (CCSD(T)cc-pVQZ) ab initio anharmonic predictions of the vibration rotation alpha matrix, which permits unambiguous assignment to CH 2 symmetric-stretch excitation built on the singly excited CH 2 out-of-plane bending mode (ν 1 + ν 4 ← ν 4 ). Longitudinal cooling of the Doppler width in the slit-jet expansion geometry also reveals partially resolved hyperfine structure on transitions out of the lowest angular momentum states in excellent agreement with predictions based on microwave studies. High level ab initio MOLPRO calculations [CCSD(T)-f12b/VnZ-f12 (n = 3, 4, CBS)] are also performed with explicitly correlated f12 electron methods for the out-of-plane CH 2 bending mode over the halogen series CH 2 X (X = F, Cl, Br, I), which clearly reveals a non-planar geometry for X = F (with a ΔE ≈ 0.3 kcal/mol barrier) and yet planar equilibrium geometries for X = Cl, Br, and I. Finally, a detailed Boltzmann analysis of the transition intensities provides support for negligible collisional equilibration of the entangled H atom nuclear spin states on the few hundred microsecond time scale and high collision densities of a slit supersonic expansion.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Structural and dynamic effects of paraoxon binding to human acetylcholinesterase by X-ray crystallography and inelastic neutron scattering

Organophosphorus (OP) compounds, including nerve agents and some pesticides, covalently bind to the catalytic serine of human acetylcholinesterase (hAChE), thereby inhibiting acetylcholine hydrolysis necessary for efficient neurotransmission. Oxime antidotes can reactivate the OP-conjugated hAChE, but reactivation efficiency can be low for pesticides, such as paraoxon (POX). Understanding structural and dynamic determinants of OP inhibition and reactivation can provide insights to design improved reactivators. Here, in this study, X-ray structures of hAChE with unaged POX, with POX and oximes MMB4 and RS170B, and with MMB4 are reported. A significant conformational distortion of the acyl loop was observed upon POX binding, being partially restored to the native conformation by oximes. Neutron vibrational spectroscopy combined with molecular dynamics simulations showed that picosecond vibrational dynamics of the acyl loop soften in the ~20–50 cm –1 frequency range. The acyl loop structural perturbations may be correlated with its picosecond vibrational dynamics to yield more comprehensive template for structure-based reactivator design.

59 BASIC BIOLOGICAL SCIENCES↗

A comparison of deep-learning-based inpainting techniques for experimental X-ray scattering

The implementation is proposed of image inpainting techniques for the reconstruction of gaps in experimental X-ray scattering data. The proposed methods use deep learning neural network architectures, such as convolutional autoencoders, tunable U-Nets, partial convolution neural networks and mixed-scale dense networks, to reconstruct the missing information in experimental scattering images. In particular, the recovered pixel intensities are evaluated against their corresponding ground-truth values using the mean absolute error and the correlation coefficient metrics. The results demonstrate that the proposed methods achieve better performance than traditional inpainting algorithms such as biharmonic functions. Overall, tunable U-Net and mixed-scale dense network architectures achieved the best reconstruction performance among all the tested algorithms, with correlation coefficient scores greater than 0.9980.

97 MATHEMATICS AND COMPUTING↗

Phase IB study of ziv-aflibercept plus pembrolizumab in patients with advanced solid tumors

Background The combination of antiangiogenic agents with immune checkpoint inhibitors could potentially overcome immune suppression driven by tumor angiogenesis. We report results from a phase IB study of ziv-aflibercept plus pembrolizumab in patients with advanced solid tumors. Methods This is a multicenter phase IB dose-escalation study of the combination of ziv-aflibercept (at 2–4 mg/kg) plus pembrolizumab (at 2 mg/kg) administered intravenously every 2 weeks with expansion cohorts in programmed cell death protein 1 (PD-1)/programmed death-ligand 1(PD-L1)-naïve melanoma, renal cell carcinoma (RCC), microsatellite stable colorectal cancer (CRC), and ovarian cancer. The primary objective was to determine maximum tolerated dose (MTD) and recommended dose of the combination. Secondary endpoints included overall response rate (ORR) and overall survival (OS). Exploratory objectives included correlation of clinical efficacy with tumor and peripheral immune population densities. Results Overall, 33 patients were enrolled during dose escalation (n=3) and dose expansion (n=30). No dose-limiting toxicities were reported in the initial dose level. Ziv-aflibercept 4 mg/kg plus pembrolizumab 2 mg/kg every 2 weeks was established as the MTD. Grade ≥3 adverse events occurred in 19/33 patients (58%), the most common being hypertension (36%) and proteinuria (18%). ORR in the dose-expansion cohort was 16.7% (5/30, 90% CI 7% to 32%). Complete responses occurred in melanoma (n=2); partial responses occurred in RCC (n=1), mesothelioma (n=1), and melanoma (n=1). Median OS was as follows: melanoma, not reached (NR); RCC, 15.7 months (90% CI 2.5 to 15.7); CRC, 3.3 months (90% CI 0.6 to 3.4); ovarian, 12.5 months (90% CI 3.8 to 13.6); other solid tumors, NR. Activated tumor-infiltrating CD8 T cells at baseline (CD8+PD1+), high CD40L expression, and increased peripheral memory CD8 T cells correlated with clinical response. Conclusion The combination of ziv-aflibercept and pembrolizumab demonstrated an acceptable safety profile with antitumor activity in solid tumors. The combination is currently being studied in sarcoma and anti-PD-1-resistant melanoma. Trial registration number NCT02298959 .

Rahma, Osama E.↗

Evidence for unconventional superconductivity in twisted bilayer graphene

The emergence of superconductivity and correlated insulators in magic-angle twisted bilayer graphene (MATBG) has raised the intriguing possibility that its pairing mechanism is distinct from that of conventional superconductors, as described by the Bardeen–Cooper–Schrieffer (BCS) theory. However, recent studies have shown that superconductivity persists even when Coulomb interactions are partially screened5. This suggests that pairing in MATBG might be conventional in nature and a consequence of the large density of states of its flat bands. In this work, we combine tunnelling and Andreev reflection spectroscopy with a scanning tunnelling microscope to observe several key experimental signatures of unconventional superconductivity in MATBG. We show that the tunnelling spectra below the transition temperature T c are inconsistent with those of a conventional s-wave superconductor, but rather resemble those of a nodal superconductor with an anisotropic pairing mechanism. We observe a large discrepancy between the tunnelling gap Δ T , which far exceeds the mean-field BCS ratio (with 2Δ T /k B T c ~ 25), and the gap Δ AR extracted from Andreev reflection spectroscopy (2Δ AR /k B T c ~ 6). The tunnelling gap persists even when superconductivity is suppressed, indicating its emergence from a pseudogap phase. Moreover, the pseudogap and superconductivity are both absent when MATBG is aligned with hexagonal boron nitride. These findings and other observations reported here provide a preponderance of evidence for a non-BCS mechanism for superconductivity in MATBG.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Impacts on product quality attributes of monoclonal antibodies produced in CHO cell bioreactor cultures during intentional mycoplasma contamination events

Abstract A mycoplasma contamination event in a biomanufacturing facility can result in costly cleanups and potential drug shortages. Mycoplasma may survive in mammalian cell cultures with only subtle changes to the culture and penetrate the standard 0.2‐µm filters used in the clarification of harvested cell culture fluid. Previously, we reported a study regarding the ability of Mycoplasma arginini to persist in a single‐use, perfusion rocking bioreactor system containing a Chinese hamster ovary (CHO) DG44 cell line expressing a model monoclonal immunoglobulin G 1 (IgG1) antibody. Our previous work showed that M. arginini affects CHO cell growth profile, viability, nutrient consumption, oxygen use, and waste production at varying timepoints after M. arginini introduction to the culture. Careful evaluation of certain identified process parameters over time may be used to indicate mycoplasma contamination in CHO cell cultures in a bioreactor before detection from a traditional method. In this report, we studied the changes in the IgG1 product quality produced by CHO cells considered to be induced by the M. arginini contamination events. We observed changes in critical quality attributes correlated with the duration of contamination, including increased acidic charge variants and high mannose species, which were further modeled using principal component analysis to explore the relationships among M. arginini contamination, CHO cell growth and metabolites, and IgG1 product quality attributes. Finally, partial least square models using NIR spectral data were used to establish predictions of high levels (≥10 4 colony‐forming unit [CFU/ml]) of M. arginini contamination, but prediction of levels below 10 4 CFU/ml were not reliable. Contamination of CHO cells with M. arginini resulted in significant reduction of antibody product quality, highlighting the importance of rapid microbiological testing and mycoplasma testing during particularly long upstream bioprocesses to ensure product safety and quality.

60 APPLIED LIFE SCIENCES↗

Balmer emission measurements in JET-ILW hydrogen, deuterium, tritium and deuterium-tritium low-confinement mode plasmas

Measurements of Balmer-alpha (B-α) and Balmer-gamma (B-γ), where B = H, D, or T isotopes of hydrogen, emission across the low-field side (LFS) divertor in JET ITER-like Wall (ILW), low-confinement mode (L-mode) plasma indicate that the divertor plasma was more strongly detached in deuterium, tritium and deuterium–tritium than in hydrogen plasmas. These measurements are consistent with the lower degree of detachment in hydrogen versus tritium plasmas inferred from Langmuir probes (Groth et al., 2023). The ratio of B-γ to B-α is a suitable indicator of high density/low temperature conditions because B-α emission is dominated by electron impact excitation with a small electron–ion recombination component regardless of electron temperature and density (for conditions in tokamak plasmas) whilst for B-γ the recombination component increases and the excitation component decreases as the electron temperature decreases and the electron density increases. Within the uncertainty of the measurements, the electron density at the low-field side separatrix and the power crossing the separatrix are similar to permit these comparisons. The B-©/B-α ratio is well correlated with the onset of detachment as measured by Langmuir probes (McCracken et al., 1998; Groth et al., 2023). The ratios of B-γ and B-α varied between 0.005 and 0.035 for low-recycling, high-recycling and partially detached conditions, and were 60–70 % higher in partially detached hydrogen than in tritium plasmas. In contrast, the difference between deuterium, tritium and 40–60 % deuterium–tritium is within 10 % and thus within the uncertainties of the measurements. Profiles of the B-α and B-γ emission was measured with two filtered CCDs connected to the visible lost light leg of JET’s mirror link spectroscopy system (Meigs et al., 2010; Lomanowski et al., 2014). Spatially (radial) narrower B-α profiles were measured with increasing isotope mass, while similarly broadened B-γ profiles were measured.

Balmer↗

Development of an accelerator-based neutron source to prototype Mo-99 production, Part II: A liquid LBE loop under a high vacuum

To provide US domestic supply of Mo-99 without using high-enriched uranium (HEU), a subcritical uranium target assembly (UTA) is irradiated by an accelerator-based neutron source to create Mo-99 through fission. Part I of this work discusses the design of a liquid lead–bismuth eutectic (LBE) windowless target for an accelerator-based neutron source development. Part II discusses how to couple this windowless target to an accelerator operating at an ultra-high vacuum and the subcritical UTA cooled by water at room temperature. Due to the windowless design of the target, the liquid LBE flow shares an ultra-high vacuum (<1.3 × 10 -7 Pa or 10 -9 Torr) space with the accelerator. As a result of this shared vacuum space, the LBE system must operate at a high vacuum (10 -3 ~10 -6 Pa or 10 -5 ~10 -8 Torr). A magnetic rotary motion feedthrough unit utilizes magnetic fluid to allow rotation of the pump while maintaining a high vacuum environment. Prior to testing the LBE system under vacuum, a pump curve measurement is performed to estimate flowrate in the system. This measurement also generates data on orifice loss coefficients, which are compared to correlations in literature. The second experiment investigates vacuum level in the LBE system during operation. High vacuum is maintained (10 -3 ~10 -5 Pa or 10 -5 ~10 -7 Torr) during system operation, and a residual gas analyzer (RGA) scan shows that partial pressures of residual gases in the LBE system lower over the duration of LBE system operations. The third experiment investigates the gravity driven liquid LBE flowing out of the target chamber in the return line, which is partially full. If the liquid LBE is not drained quickly enough, flooding in the target chamber could occur. The coefficient n in the Manning equation is found to be around 0.008 s/m 1/3 . The last experiment performed is a demonstration that a vacuum jacket could provide sufficient thermal insulation to allow coupling between 300 °C LBE loop and a water tank at room temperature. In conclusion, the results from these experiments have influenced the development of the neutron source for the future commercial scale Mo-99 production system.

43 PARTICLE ACCELERATORS↗

Mechanism for Anomalous Hall Ferromagnetism in Twisted Bilayer Graphene

Motivated by the recent observation of an anomalous Hall effect in twisted bilayer graphene, here we use a lowest Landau level model to understand the origin of the underlying symmetry-broken correlated state. This effective model is rooted in the occurrence of Chern bands which arise due to the coupling between the graphene device and its encapsulating substrate. Our model exhibits a phase transition from a spin-valley polarized insulator to a partial or fully valley unpolarized metal as the bandwidth is increased relative to the interaction strength, consistent with experimental observations. In sharp contrast to standard quantum Hall ferromagnetism, the Chern number structure of the flat bands precludes an instability to an intervalley coherent phase, but allows for an excitonic vortex lattice at large interaction anisotropy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Thermodynamics of Tritium Trapping by Point Defects at Interfacial Cr-based Phases of the Al Coating

Density functional theory (DFT) simulations have been carried out to evaluate the potential for tritium trapping by metal vacancies in four phases Cr-containing phases (i.e., Cr3Si, Al0.3Cr0.7, Al8Cr5-HT, and Al8Cr5) identified near the interface between the Al coating and 316 stainless steel (316 SS) cladding. In addition, an ab initio thermodynamics approach has been employed to predict the temperature and T2-partial pressure dependence on the thermodynamics of singly tritiated defects. Key results in this work suggest that metal vacancies in the four phases have the potential to favorably trap tritium species, especially Si vacancies in Cr3Si phase. This overall thermodynamic trend can be correlated to the energy cost of having an interstitial tritium in the lattice, which has been calculated to range from 0.17 eV in Al8Cr5-HT to 0.89 eV in Cr3Si. A comparison of the results from this study with previous theoretical works investigating tritium behavior in other Fe-Al phases identified in the aluminide coating, suggests that metal vacancies are generally able to trap tritium in various Fe-Al aluminide phases. Especially, it was found that Si and Al vacancies would be the most efficient to trap for tritium, followed by Cr vacancies, then Fe and Ni vacancies. In the four Cr-based material phases investigated in this work, it is interesting to note that, in the absences of Fe or Ni species, strong interactions between tritium and the metal vacancies are always occurring by the formation of preferential Cr—T bonds (i.e., no Si—T or Al—T bonds were formed).

Sassi, Michel J.↗

The 650 °C Tensile Deformation of Graded IN718-René41 Superalloy Fabricated by Laser Blown-Powder Directed Energy Deposition

The microstructure and 650 °C tensile properties of a compositionally graded IN718-René41 (718-R41) superalloy fabricated by laser blown-powder directed energy deposition (DED-LB/M) are investigated to understand structure–property relationships and baseline tensile properties. Digital Image Correlation (DIC), in situ neutron diffraction, and conventional characterization techniques are performed to study the as-built and heat-treated states. The applied heat treatment generates static recrystallization and equiaxed grains in 718-rich compositions, while R41-rich compositions remain partially or un-recrystallized possibly influenced by a higher MC carbide fraction (>0.5%). The yield strengths of the 718 and R41 sections in the heat-treated state are comparable to wrought forms but the graded compositions show weakness due to unoptimized heat treatment. Diffraction elastic constants first decrease and then increase along the 718-R41 composition gradient, while a small difference is observed between the as-built and heat-treated states and γ, γ′ phases. Overall, the compositionally graded region shows a smooth transition in the elastic properties. Grain-level load transfer from the (220) to (200) grains shows compositional dependence, and qualitatively agrees with DIC-measured macroscopic yield strength. Within the (200) grains, the γ/γ′ phases deform elastically until the γ phase yields and afterwards, the γ′ phase takes load from the γ phase.

Huang, Shenyan (ORCID:0000000196528114)↗

A Catalog of Candidate Double and Lensed Quasars from Gaia and WISE Data

Making use of strong correlations between closely separated multiple or double sources and photometric and astrometric metadata in Gaia Early Data Release 3 (EDR3), we generate a catalog of candidate double- and multiply imaged lensed quasars and active galactic nuclei (AGNs), comprising 3140 systems. It includes two partially overlapping parts: a sample of distant (redshifts mostly greater than 1) sources with perturbed data; and systems that have been resolved into separate components by Gaia at separations less than 2''. For the first part, which is roughly one-third of the published catalog, we synthesized 0.617 million redshifts using multiple machine-learning prediction and classification methods, using independent photometric and astrometric data from Gaia EDR3 and the Wide-field Infrared Survey Explorer, with accurate spectroscopic redshifts from the Sloan Digital Sky Survey (SDSS) as a training set. Using these synthetic redshifts, we estimate a 4.9% rate of interlopers with spectroscopic redshifts below 1 in this part of the catalog. Unresolved candidate double and dual AGNs and quasars are selected as sources with a marginally high BP/RP excess factor (phot_bp_rp_excess_factor), which is sensitive to source extent, limiting our search to high-redshift quasars. For the second part of the catalog, additional filters on measured parallax and near-neighbor statistics are applied to diminish the propagation of the remaining stellar contaminants. The estimated rate of the positives (double or multiple sources) is 98%, and the estimated rate of dual (physically related) quasars is greater than 54%. A few dozen serendipitously found objects of interest are discussed in more detail, including known and new lensed images, planetary nebulae, young IR stars of peculiar morphology, and quasars with catastrophic redshift errors in SDSS.

79 ASTRONOMY AND ASTROPHYSICS↗

Active Causal Machine Learning for Molecular Property Prediction

Predicting properties from molecular structures is paramount to design tasks in medicine, materials science, and environmental management. However, design rules derived from the structure-property relationships using correlative data-driven methods fail to elucidate underlying causal mechanisms controlling chemical phenomena. This preliminary work proposes a workflow to actively learn robust cause-effect relations between structural features and molecular property for a broad chemical space utilizing smaller subsets, entailing partial information.

Fox, Zach↗

Persistent flat band splitting and strong selective band renormalization in a kagome magnet thin film

Magnetic kagome materials provide a fascinating playground for exploring the interplay of magnetism, correlation and topology. Many magnetic kagome systems have been reported including the binary Fe m X n (X = Sn, Ge; m:n = 3:1, 3:2, 1:1) family and the rare earth RMn 6 Sn 6 (R = rare earth) family, where their kagome flat bands are calculated to be near the Fermi level in the para magnetic phase. While partially filling a kagome flat band is predicted to give rise to a Stoner-type ferromagnetism, experimental visualization of the mag netic splitting across the ordering temperature has not been reported for any of these systems due to the high ordering temperatures, hence leaving the nature of magnetism in kagome magnets an open question. Here, we probe the electronic structure with angle-resolved photoemission spectroscopy in a kagome magnet thin film FeSn synthesized using molecular beam epitaxy. We identify the exchange-split kagome flat bands, whose splitting persists above the magnetic ordering temperature, indicative of a local moment picture. Such local moments in the presence of the topological flat band are consistent with the compact molecular orbitals predicted in theory. We further observe a large spin-orbital selective band renormalization in the Fe d xy + d x 2 -y 2 spin majority channel reminiscent of the orbital selective correlation effects in the iron based superconductors. Our discovery of the coexistence of local moments with topological flat bands in a kagome system echoes similar findings in magic-angle twisted bilayer graphene, and provides a basis for theoretical effort towards modeling correlation effects in magnetic flat band systems.

36 MATERIALS SCIENCE↗

The calculation of light element impurity (α, n) yield curves in a PuO 2 matrix and associated specific yield coefficients: Influence of the reaction cross sections

Most of the Pu separated from irradiated commercial nuclear fuel is stored as PuO 2 . The primary quantitative nondestructive measurement technique used to verify the amount of Pu in storage containers is passive neutron correlation counting. An important physical property of the oxide material is the ratio, α, of the rate of (α, n) neutrons produced inside the item to the rate of neutrons produced by spontaneous fission. This ratio influences the precision of the correlated counting method and affects the interpretation of the data because of how it changes both the primary total neutron production rate and the rate of induced fission events taking place inside the item. In addition to the main O(α, n) contribution, additional contributions come from α-particle interactions with light element impurities that are inevitably present. In this work, we calculate specific (α, n) yield coefficients, expressed in units of neutrons per second per gram of α-emitting nuclide per part per million by mass of the specified impurity element distributed in a pure PuO 2 matrix, for some key α-emitting actinides commonly present in reprocessed Pu ( 238–242 Pu+ 241 Am). These coefficients are directly applicable to nuclear safeguards verification work in which the α ratio is often calculated from the Pu-isotopic composition and chemical information obtained by other means. Further, they also provide a convenient up-to-date reference set against which values generated by other methods can be compared. Results are presented for impurities with atomic number from 3 to 17 inclusive, plus K and Fe. In most cases, these coefficients are not expected to change by more than 5%–10% at any time in the future. However, as new data become available, changes as large as 20% may be needed for some targets (e.g., F). The present yield calculations are limited by the general shortage of quality experimental total (α, n) reaction cross section data, which, together with unexplained variation between determinations, means that an objective and coherent evaluation is not possible. The situation is even less satisfactory for the partial differential cross section needed to calculate neutron spectra.

(𝛼, n) reactions↗