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At least 451 records · Page 25

Exploring the deformation behavior of nanotwinned Al–Zr alloy via in situ compression

Nanotwinned metals have demonstrated the capacity for concomitant high strength and ductility. However, metals with high stacking fault energies, such as aluminum (Al), have a low propensity for twin formation. Here, we show the fabrication of supersaturated solid-solution Al–Zr alloys with a high density of growth twins. Incoherent twin boundaries (ITBs) are strong barriers to dislocation motion, while mobile partial dislocations promote plasticity. These deformable nanotwinned Al–Zr alloys reach a flow stress of ∼1 GPa, as demonstrated using in situ micropillar compression tests. Density functional theory calculations uncover the role Zr solute plays in the formation and deformation of the nanotwinned microstructure. This study features a strategy for incorporating ITBs and 9R phase into Al alloys for simultaneous benefits to strength and deformability.

Richter, N. A. (ORCID:0000000332732276)↗

Magnetic phase diagram of a two-orbital model for bilayer nickelates with varying doping

Motivated by the recently discovered high-T c bilayer nickelate superconductor La 3⁢ Ni 2 ⁢O 7 , we comprehensively research a bilayer 2×2×2 cluster for different electronic densities n by using the Lanczos method. We also employ the random-phase approximation to quantify the first magnetic instability with increasing Hubbard coupling strength, also varying n. Based on the spin structure factor S(q), we have obtained a rich magnetic phase diagram in the plane defined by n and U/W, at fixed Hund coupling, where U is the Hubbard strength and W the bandwidth. We have observed numerous states, such as A-AFM, Stripes, G-AFM, and C-AFM. At half-filling, n=2 (two electrons per Ni site, corresponding to N=16 electrons), the canonical superexchange interaction leads to a robust G-AFM state (π,π,π) with antiferromagnetic couplings both in-plane and between layers. By increasing or decreasing electronic densities, ferromagnetic tendencies emerge from the “half-empty” and “half-full” mechanisms, leading to many other interesting magnetic tendencies. In addition, the spin-spin correlations become weaker both in the hole or electron doping regions compared with half-filling. At n=1.5 (or N=12), density corresponding to La 3 ⁢Ni 2 ⁢O 7 , we obtained the “Stripe 2” ground state (antiferromagnetic coupling in one in-plane direction, ferromagnetic coupling in the other, and antiferromagnetic coupling along the z axis) in the 2×2×2 cluster. In addition, we obtained a much stronger AFM coupling along the z axis than the magnetic coupling in the xy plane. The random-phase approximation calculations with varying n give very similar results as Lanczos, even though both techniques are based on quite different procedures. Additionally, a state with q/π=(0.6,0.6,1) close to the E-phase wavevector is found in our RPA calculations by slightly reducing the filling to n=1.25, possibly responsible for the E-phase SDW recently observed in experiments. In conclusion, our predictions can be tested by chemically doping La 3 ⁢Ni 2 ⁢O 7 .

36 MATERIALS SCIENCE↗

An Investigation of Liquefaction in Irradiated TRIGA Fuel Exposed to Relatively High Temperatures

This report presents the findings of an investigation into high temperature fuel cladding chemical interactions (FCCI) in Training, Research, Isotopes, General Atomics (TRIGA) fuel rods. A TRIGA fuel-rod core or meat is principally composed of uranium (U) particles dispersed in a zirconium hydride (Zr H) matrix. The fuel is clad in sealed 304SS or Incoloy 800 tubes. At high temperatures, the fuel will interact with the cladding, resulting in FCCI. To investigate the FCCI (in this case, liquefaction), irradiated TRIGA fuel rods were exposed to relatively high temperatures in furnace tests. The tests were performed at different temperatures using segments from an irradiated TRIGA fuel rod at the Hot Fuel Examination Facility located at Idaho National Laboratory (INL). The data from this study is important for developing a better understanding of the performance of U-ZrH fuel type during transient events (e.g., a Loss of Coolant Accident (LOCA) event) that may result in high temperatures while operating a TRIGA reactor. Furnace tests were run for 6 hours at 730, 800, 900, 950, and 1,000°C. One test was run for 12 hours at 950°C. Post-test microstructural characterization was performed on the heat-treated samples using optical metallography to look for evidence of liquefaction. Additionally, microstructural characterization was performed using scanning electron microscopy to investigate the microstructure of the as-irradiated fuel before heat treatment and the microstructural changes that occurred after heat treating for the 730 and 950°C heat treatments for 6 hours. Results of the analysis were compared to those produced during diffusion studies performed using unirradiated TRIGA fuel meat and type 304 stainless steel. A gap is typically present in as-irradiated fuel that limits any possibility for chemical interaction between the fuel and cladding. Optical metallography (OM) was used to identify areas in the specimens heat treated at 950 and 1000°C where fuel and cladding contact was satisfactory for the FCCI to transpire. The bulk of the interaction zones that form due to FCCI developed in the fuel meat and not as much in the cladding. Even in the sample tested at 1,000°C, no evidence was found that gross fuel meat or cladding melting had occurred. Only limited porosity was found in the fuel meat that possibly could have been due to melting of a particular precipitate phase or phases that had formed during FCCI. These results agreed with those reported for the unirradiated diffusion couple studies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Revisions of ORNL 188 W Process Based on Nonradiological Experiments

Tungsten-188 is in widespread use in the 188 W(t 1/2 = 69 d)/ 188 Re(t 1/2 =16.9 h) biomedical generator. Oak Ridge National Laboratory (ORNL) has been providing this product to the world since 1999. At ORNL, 188 W is produced via irradiation in ORNL’s High Flux Isotope Reactor (HFIR). Enriched 186 W targets in the form of sintered metallic pellets or rings achieve a compact loading in the irradiation vessel, providing a high yield per unit target. The enrichment of the target is >90% 186 W and this isotope undergoes double neutron capture to produce the desired 188W product. While 188 W is produced by neutron bombardment, 191 Os(t 1/2 = 15.4 d) is simultaneously produced as a byproduct requiring separation from 188 W by post irradiation treatment. In the current processing pathway, the irradiated W metal pellets or rings are first converted into an oxide form of WO 3 by heating the irradiated W metal target at 750°C in a quartz reaction vessel inside a vertical furnace under a constant flow of air. During heating, W metal reacts with oxygen in the air to produce WO 3 , which is soluble in 6 M NaOH for later purification process. This oxidation process also converts 188 Os (the decay daughter of 188 W) and 191 Os (the irradiation produced byproduct) into OsO 4 , a highly volatile and toxic gas. The gaseous effluents driven from the quartz reaction vessel are passed through a scrubbing array to remove OsO 4 before the air is discharged from the process. This heterogeneous oxidation method simultaneously achieves two goals: 1). converting metal target to a soluble oxide form and 2). separating volatile OsO 4 away from the solid WO 3 product, although harmful 191 OsO 4 is unfavorable but being taken care of by the down road scrubbing array. In the past twenty years the existing OsO 4 scrubbing array served well in preventing OsO 4 from being released into the environment, until July of 2020 when a minor amount of 191 Os was found to have been released into the environment which resulted in a standby of building 4501 from July 2020 to February 2021.Since October 20 of 2020 a team of researchers from groups of RSTD and NEFD were organized to work for the following tasks: (1) Fully understand the root causes of the July incident of 191 Os release and create a redesigned 191 Os scrubbing array to eliminate the possibility of 191 Os release in future 188 W processes; (2) In Phase-1 tests, select a correct air (O 2 ) flow rate in 188 W process, that provides sufficient oxygen for the oxidation of tungsten metal, while still allowing sufficient resonance time for 191 Os removal by the scrubbers; (3) In Phase-2 tests, confirm the efficiency of the redesigned scrubbing array to absorb excessive amount of non-rad OsO 4 (generated from Os metal powder) at the selected air flow; (4) In Phase-3 tests, simulate the hot cell 188 W process by heating pressed non-rad W-Os pellets in a quartz vessel of new design and the new array under operation parameters selected in Phase-1 and -2; (5) Complete a new operation procedure for 188 W process in hot cell and a TM report as a summary of the Os Mitigation Project. This TM report summarizes the investigation on root causes from technical aspects in July 191 Os release and the correspondent improvement towards the redesigned 191 Os scrubbing system. The report presents the efforts made on selection of optimal operational parameter with the new scrubbing array and the quartz vessel of new design, based on experiment data obtained in Phase-1, -2 and -3 tests. Further renovations for 188 W process and additional improvement of W target treatment will also be discussed.

07 ISOTOPE AND RADIATION SOURCES↗

5ω Optical Thomson Scattering Report

The 5ω Optical Thomson Scattering system on the National Ignition Facility (NIF) is a diagnostic designed to measure temporally and spatially resolved plasma conditions in Inertial Confinement Fusion (ICF) Hohlraums. The system was proposed in 2014 and a phased approach to implementation was developed. In phase one the collection system was designed, built, and fielded on the NIF to be used for 3ω Thomson scattering measurements and background measurements near 211 nm (5ω. The initial commissioning experiment for the collection system was completed in Oct. 2016. Commissioning of the collection system continued through 2017 and the system is now fielded for a range of user experiments and regularly produces publication quality data. A dedicated 5ω probe laser was designed and built to allow Thomson scattering measurements in the presence of 2 MJ of 3ω drive energy. Due to scattered light (spectral reflections, laser-plasma instabilities, and unconverted drive energy) from the 3w drive lasers typical wavelengths (2ω and 4ω) fielded at other laser facilities like the Nova Laser Facility and the Omega Laser Facility were unable to meeting the signal to background requirements in design studies. A 10 Joule 5ω probe was proposed as a solution that met requirements. This 10 Joule laser was more energetic than previously fielded 5w lasers by 2-3 orders of magnitude. As part of a risk reduction plan, phase two of the project was to develop a 1 Joule, 5ω laser to demonstrate conversion efficiency >20% from 1ω to 5ω and make initial Thomson scattering measurements in the first few nanoseconds of an ICF laser pulse. Initial tests of the 5w conversion were completed at the Laboratory for Laser Energetics (LLE) and produced record 5ω energies. Based on these results from LLE, a 1 Joule, 5w laser system was designed for the NIF in 2018 and commissioning began in 2019. Commissioning of the 5ω laser system continued through 2023 and was eventually paused in Q1 of FY24 due to completing resource constraints. Commissioning of the 5w laser system proved incredibly challenging. Multiple issues were identified during commissioning and resolved, but issues remain. Currently there is not a clear understanding of why 5ω scattered has not been detected on the OTS collection system. Based on offline measurements, calculations, and preshot measurements the system appears to meet all requirements. Potential target physics issues have been investigated and do not appear to be an issue. The current hypothesis is that there is an error in one or more aspects of the offline testing not translating to expected performance when the system is fielded on the NIF. Additional full system testing in-situ utilizing the complete OTS system and NIF target chamber center time is needed to further test potential failure modes.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Degradation of Simulated HLW Glass and International Simple Glass immersed partially in water - 16474

Water degradation of glass waste forms destined for geological disposal has been studied in a variety of conditions including of bulk glass immersed completely in static or dynamic water. During the course of repository life, the canisters may be only partially immersed in the initial stages of contact with water. Under these conditions glass degradation occurs on the glass immersed in water and on the glass above water by vapor condensation. In this work degradation of International Simple Glass (ISG) and Simulated High Level Waste Glass (HSG) is examined by immersing partially in distilled water during the course of test. Under static experimental conditions at 90 deg. C, the condensation of vapor on the ISG glass surface formed Ca-rich precipitates and pits after degrading for 1 and 3 weeks respectively. Whereas HSG precipitated Ca-rich phases predominantly after 1 week and no pits were found on the surface. When compared, HSG was found to change surface chemistry faster than ISG. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Novel Infiltration Diagnostics based on Laser-line Scanning and Infrared Temperature Field Imaging

This project targets the building energy efficiency problems induced by building infiltration/leaks. The current infiltration inspection techniques often require extensive visual inspection and/or whole building pressure test. These current techniques cannot meet more than three of the below five criteria of ideal infiltration diagnostics: 1. location and extent diagnostics, 2. building-level application, 3. least surface preparation, 4. weather-proof, and 5. non-disruption to building occupants. These techniques are either too expensive or time consuming, and often lack accuracy and repeatability. They are hardly applicable to facades/facades section. The goal of the project was to develop a novel infiltration diagnostics technology based on laser line-scanning and simultaneous infrared temperature imaging. A laboratory scale experimental setup was designed to mimic a model house of well-defined pressure difference below or above the outside pressure. Algorithms and Matlab-based programs had been developed for recognition of the hole location in infrared images. Our experiment based on laser wavelengths of 450 and 1550 nm and laser beam diameters of 4-25 mm showed that the location of the holes could be identified using laser heating; the diagnostic approach however could not readily distinguish between infiltration and non-infiltration points. To significantly improve the scanning throughput and recognition accuracy, a second approach was explored, developed, and extensively tested. It incorporates a liquid spray on the surface to induce extra phase change cooling effect. In this spray method, we termed it as PECIT (Phase-change Enhanced Cooling Infrared Thermography), phase-change enhanced cooling was used, which significantly amplifies the effect of air flow (infiltration and exfiltration). This heat transfer method worked extremely well to identify infiltration and exfiltration locations with high accuracy and increased throughput. The PECIT technique was systematically developed and tested for through holes with diameters 1 mm to 2 mm, and diagonal lines of 0.5 mm width at different camera-wall distances of 46 cm to 200 cm, under different pressure differences from 5 Pa to 20 Pa, and under different wind conditions. The PECIT technique had either met or exceeded the goals proposed in the project. For exfiltration, we achieved 100% accuracy under a much lower pressure difference of 10 Pa (proposed one: 50 Pa with stretch goal of 15 Pa). For infiltration, we achieved >90% accuracy under a much lower pressure difference of 10 Pa (proposed one: 50 Pa with stretch goal of 15Pa). For exfiltration, we achieved 100% accuracy under a much lower pressure difference of 10 Pa. For infiltration, we achieved 100% accuracy under a much lower pressure difference of 10 Pa. The PECIT technique can reach a throughput of 120 m2/h, which is 4 times the proposed goal for the laser line-scanning and simultaneous infrared temperature imaging approach. For commercialization and market penetration, we had meetings with two companies for feedback collection and further improvement for practical use. Also, we have interacted with Office of Intellectual Property and Technology Transfer of Iowa State University for idea disclosure and patent application.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Characterizing Natural Attenuation of Cr(VI) in a Chromium Plume at Los Alamos National Laboratory - 18594

Characterization of natural attenuation of hexavalent (Cr(VI)) on aquifer sediments within the Cr plume at Los Alamos National Laboratory has been conducted to (1) refine conceptual and numerical models of chromium fate and transport, (2) evaluate the long-term stability of Cr(III)/Cr(VI) in the complex groundwater system along flow paths from the source to the regional aquifer, and (3) evaluate and develop options for successful remediation. The naturally high chromium abundance in aquifer sediments at Los Alamos pose an unique challenge for characterization of chromium reduction, making conventional approaches such as uptake tests and advanced spectroscopic measurements ineffective in identifying relatively small amounts of anthropogenic Cr(VI) in the sediments. To address this challenge and as complimentary to these conventional methods, sequential leaching tests were conducted on core hole sediments obtained from sonic drilled cores taken from both contaminated and non-contaminated horizons among two mineralogically distinct formations (Puye formation and Miocene Pumiceous Unit) within the Cr plume. A series of three and coherent sequential leaching steps were conducted: 1) an alkaline leach to determine the amount of Cr(VI) sorbed on the sediments. 2) a weak acid leach (using 0.01 M and 0.1 M HNO{sub 3}) to determine the amount of anthropogenic chromium (Cr(III) and Cr(VI)) on aquifer sediment surfaces, and 3) a strong acid leach (using 2 M HNO{sub 3}) to characterize the amount of releasable Cr(III) from aquifer minerals. Additionally we tested the efficiency and detection limit of sequential leaching on bentonite, which consists mainly of smectite, used in drill muds and laboratory-grade biotite spiked with known concentrations of Cr(VI). Smectite and biotite are two phases considered to be potentially important host minerals in aquifer sediments within the plume. Thus, by comparing contaminated and uncontaminated sediment leachate results of chromium and other major and trace elements, the signature and quantity of anthropogenic Cr(VI) can be derived. Our results from the weak acid leaching test indicate that the method detection limit for Cr 'uptake' was about 1 μg/g for biotite and about 0.5 μg/g for bentonite. Our results also indicate that all samples taken from known contaminated horizons in comparison to non-contaminated ones within the Puye formation showed no statistical difference in the amount of Cr leached indicative of its insignificant Cr(VI) attenuation capacity. The amount of excess Cr leached from the magnetic fraction of the contaminated Miocene Pumiceous samples was about 2 μg/g of sediment. Considering that the magnetic fraction was about 11% by mass of the bulk sample, the excess amount of Cr leached from the bulk material would be about 0.2 μg/g of sediment, suggesting the potential for some Cr(VI) attenuation capacity in the Miocene pumice unit. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Performance of a Steel/Oxide Composite Waste Form for Combined Waste Steams from Advanced Electrochemical Processes

The results of electrochemical corrosion tests and modeling activities performed collaboratively by researchers at the University of Illinois at Chicago and Argonne National Laboratory as part of workpackage NU-13-IL-UIC-0203-02 are summarized herein. The overall objective of the project was to develop and demonstrate testing and modeling approaches that could be used to evaluate the use of composite alloy/ceramic materials as high-level durable waste forms. Several prototypical composite waste form materials were made from stainless steels representing fuel cladding, reagent metals representing metallic fuel waste streams, and reagent oxides representing oxide fuel waste streams to study the microstructures and corrosion behaviors of the oxide and alloy phases. Microelectrodes fabricated from small specimens of the composite materials were used in a series of electrochemical tests to assess the corrosion behaviors of the constituent phases and phase boundaries in an aggressive acid brine solution at various imposed surface potentials. The microstructures were characterized in detail before and after the electrochemical tests to relate the electrochemical responses to changes in both the electrode surface and the solution composition. The results of microscopic, electrochemical, and solution analyses were used to develop equivalent circuit and physical models representing the measured corrosion behaviors of the different materials pertinent to long-term corrosion behavior. This report provides details regarding (1) the production of the composite materials, (2) the protocol for the electrochemical measurements and interpretations of the responses of multi-phase alloy and oxide composites, (3) relating corrosion behaviors to microstructures of multi-phase alloys based on 316L stainless steel and HT9 (410 stainless steel was used as a substitute) with added Mo, Ni, and/or Mn, and (4) modeling the corrosion behaviors and rates of several alloy/oxide composite materials made with added lanthanide and uranium oxides. These analyses show the corrosion behaviors of the alloy/ceramic composite materials are very similar to the corrosion behaviors of multi-phase alloy waste forms, and that the presence of oxide inclusions does not impact the corrosion behaviors of the alloy phases. Mixing with metallic waste streams is beneficial to lanthanide and uranium oxides in that they react with Zr in the fuel waste to form highly durable zirconates. The measured corrosion behaviors suggest properly formulated composite materials would be suitable waste forms for combined metallic and oxide waste streams generated during electrometallurgical reprocessing of spent nuclear fuel. Electrochemical methods are suitable for evaluating the durability and modeling long-term behavior of composite waste forms: the degradation model developed for metallic waste forms can be applied to the alloy phases formed in the composite and an affinity-based mineral dissolution model can be applied to the ceramic phases.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Broadband Calibration of Acoustic Emission and Ultrasonic Sensors from Generalized Ray Theory and Finite Element Models

This paper describes a calibration method for acoustic emission and ultrasonic sensors that is effective from 1 kHz to 1 MHz. The method combines generalized ray theory and finite element analysis to model wave propagation at higher and lower frequencies, respectively. A ball impact is used as a calibration source, a thick aluminum plate is used as the test block, and hot glue is used as the couplant. We demonstrate this method on five commercial piezoelectric sensors: Physical Acoustics (PAC) R15a, PAC WSa, Panametrics V101, Panametrics V103, and Valpey-Fisher Pinducer. Our calibration results show that reflections and other wave phases can be more clearly identified with the less-resonant Panametrics sensors. The PAC sensors have the greatest sensitivity and are able to detect surface normal displacements at least down to 1 pm amplitude in the 100s of kHz frequency band. Aperture effect is minimized by the small size of the Pinducer. Our method focuses on the amplitude response of the sensors (phase is ignored) and extends the calibration to a frequency band that is lower than typical analyses. Low frequency information is useful for determining the seismic moment of a seismic source (analogous to the magnitude of an earthquake) and can increase the amount of information acquired in a single recording.

42 ENGINEERING↗

Glass-bonded iodosodalite waste form for immobilization of 129I

Immobilization of radioiodine (e.g., 129I, 131I) is an important need for current and future nuclear fuel cycles. For the current work, iodosodalite [Na8(AlSiO4)6I2] was synthesized hydrothermally from metakaolin, NaI, and NaOH. Following hydrothermal treatment, dried unwashed powders were used to make glass-bonded iodosodalite waste forms by heating pressed pellets at 650, 750, or 850 °C with two different types of sodium borosilicate glass binders, i.e., NBS-4 and SA-800. These heat-treated specimens were characterized with X-ray diffraction, Fourier-transform infrared spectroscopy, scanning electron microscopy, energy dispersive spectroscopy, thermal analysis, porosity and density measurements, neutron activation analysis, and inductively-coupled plasma mass spectrometry. The pellets mixed with 10 mass% of NBS-4 or SA-800 and heat-treated at 750 °C contained relatively high percentage iodine retention (~44-47 % of the maximum iodine loading) with relatively low porosities, while other pellets with higher percentages iodine retention either contained higher porosity or were not completely sintered. ASTM C1308 chemical durability tests of monolithic specimens showed a large initial release of Na, Al, Si, and I on the first day, possibly from water-soluble salt crystals or non-durable amorphous phases. Release rates of Na and Si were higher than for Al and I, probably due to a poorly durable Na-Si-O phase from the glass bonding matrix. The cumulative normalized release of iodine was 12.5 g m-2 for the first 10 1-d exchanges, suggestive of coherent dissolution. The average release rate from 10-24 days during the 7-d exchange intervals was 0.2336 g m-2 d-1.

sodalite, iodosodalite, waste forms, iodine↗

Precision vector control of a superconducting RF cavity driven by an injection locked magnetron

The technique presented in this paper enables the regulation of both radio frequency amplitude and phase in narrow band devices such as a Superconducting RF (SRF) cavity driven by constant power output devices i.e. magnetrons [1]. The ability to use low cost high efficiency magnetrons for accelerator RF power systems, with tight vector regulation, presents a substantial cost savings in both construction and operating costs - compared to current RF power system technology. An operating CW system at 2.45 GHz has been experimentally developed. Vector control of an injection locked magnetron has been extensively tested and characterized with a SRF cavity as the load. Amplitude dynamic range of 30 dB, amplitude stability of 0.3% r.m.s, and phase stability of 0.26 degrees r.m.s. has been demonstrated.

43 PARTICLE ACCELERATORS↗

Mechanical properties examined by nanoindentation for selected phases relevant to the development of monolithic uranium-molybdenum metallic fuels

Nanomechanical properties, specifically the reduced modulus and hardness of several intermetallic and solid solution phases are reported here to assist the development of the U-10 wt% Mo (U-10Mo) monolithic fuel system for research and test reactors. Findings from this study and reported values of mechanical properties provide data critical for understanding and predicting the structural behavior of the fuel system during fabrication and irradiation. The phases examined are products of interdiffusion and reaction between (1) the AA6061 cladding and the Zr diffusion barrier, namely (Al,Si) 3 Zr and Al 3 Zr, (2) the U-10Mo fuel and the Zr diffusion barrier, namely UZr 2 , Mo 2 Zr, and a-U, and (3) the U (or U-10Mo) and Mo, namely a mixture gradient of α- and γ-phases. The UC inclusions observed within the fuel alloy were also examined. Only phases present in thick or continuous microstructure on cross-sectioned fuel plates and diffusion couples were investigated for reduced modulus and hardness. Concentration-dependence of room-temperature reduced modulus in U solid solution with 0–10 wt% Mo was semi-quantitatively modeled based on mixture of α- and γ-phases and solid solutioning within the γ-phase.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Development and Testing of Diglycolamide Functionalized Mesoporous Silica for Sorption of Trivalent Actinides and Lanthanides

Sequestration of trivalent actinides and lanthanides present in used nuclear fuel and legacy wastes is necessary for appropriate long-term stewardship of these metals, particularly to prevent their release into the environment. Organically modified mesoporous silica is an efficient material for recovery and potential subsequent separation of actinides and lanthanides because of its high surface area, tunable ligand selection, and chemically robust substrate. Here, we have synthesized the first novel hybrid material composed of SBA-15 type mesoporous silica functionalized with diglycolamide ligands (DGA-SBA). Because of the high surface area substrate, the DGA-SBA was found to have the highest Eu capacity reported so far in the literature of all DGA solid-phase extractants. The sorption behavior of europium and americium on DGA-SBA in nitric and hydrochloric acid media was tested in batch contact experiments. DGA-SBA was found to have high sorption of Am and Eu in pH 1, 1 M, and 3 M nitric and hydrochloric acid concentrations, which makes it promising for sequestration of these metals from used nuclear fuel or legacy waste. The kinetics of Eu sorption were found to be two times slower than that for Am in 1 M HNO 3 . Additionally, the short-term susceptibility of DGA-SBA to degradation in the presence of acid was probed using 29 Si and 13 C solid-state NMR spectroscopy. Finally, the material was found to be relatively stable under these conditions, with the ligand remaining intact after 24 h of contact with 1 M HNO 3 , an important consideration in use of the DGA-SBA as an extractant from acidic media.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nonlinear saturation and oscillations of collisionless zonal flows

Abstract In homogeneous drift-wave turbulence, zonal flows (ZFs) can be generated via a modulational instability (MI) that either saturates monotonically or leads to oscillations of the ZF energy at the nonlinear stage. This dynamics is often attributed as the predator–prey oscillations induced by ZF collisional damping; however, similar dynamics is also observed in collisionless ZFs, in which case a different mechanism must be involved. Here, we propose a semi-analytic theory that explains the transition between the oscillations and saturation of collisionless ZFs within the quasilinear Hasegawa–Mima model. By analyzing phase-space trajectories of DW quanta (driftons) within the geometrical-optics (GO) approximation, we argue that the parameter that controls this transition is N ∼ γ MI / ω DW , where γ MI is the MI growth rate and ω DW is the linear DW frequency. We argue that at N ≪ 1, ZFs oscillate due to the presence of so-called passing drifton trajectories, and we derive an approximate formula for the ZF amplitude as a function of time in this regime. We also show that at N ≳ 1, the passing trajectories vanish and ZFs saturate monotonically, which can be attributed to phase mixing of higher-order sidebands. A modification of N that accounts for effects beyond the GO limit is also proposed. These analytic results are tested against both quasilinear and fully-nonlinear simulations. They also explain the earlier numerical results by Connaughton et al (2010 J. Fluid Mech. 654 207) and Gallagher et al (2012 Phys. Plasmas 19 122115) and offer a different perspective on what the control parameter actually is that determines the transition from the oscillations to saturation of collisionless ZFs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Nonlinear saturation and oscillations of collisionless zonal flows

In homogeneous drift-wave (DW) turbulence, zonal flows (ZFs) can be generated via a modulational instability (MI) that either saturates monotonically or leads to oscillations of the ZF energy at the nonlinear stage. This dynamics is often attributed as the predator-prey oscillations induced by ZF collisional damping; however, similar dynamics is also observed in collisionless ZFs, in which case a different mechanism must be involved. Here, we propose a semi-analytic theory that explains the transition between the oscillations and saturation of collisionless ZFs within the quasilinear Hasegawa-Mima model. By analyzing phase-space trajectories of DW quanta (driftons) within the geometrical-optics (GO) approximation, we argue that the parameter that controls this transition is N ~ \gamma_MI/\omega_DW, where \gamma_MI is the MI growth rate and \omega_DW is the linear DW frequency. We argue that at N << 1, ZFs oscillate due to the presence of so-called passing drifton trajectories, and we derive an approximate formula for the ZF amplitude as a function of time in this regime. We also show that at N >~ 1, the passing trajectories vanish and ZFs saturate monotonically, which can be attributed to phase mixing of higher-order sidebands. A modification of N that accounts for effects beyond the GO limit is also proposed. These analytic results are tested against both quasilinear and fully-nonlinear simulations. They also explain the earlier numerical results by Connaughton et al. [J. Fluid Mech. 654, 207 (2010)] and Gallagher et al. [Phys. Plasmas 19, 122115 (2012)] and offer a revised perspective on what the control parameter is that determines the transition from the oscillations to saturation of collisionless ZFs.

collisionless zonal flows, modulational instabilit↗

Development and Validation of a Polarimetric-MCScene 3D Atmospheric Radiation Model

Polarimetric measurements can substantially enhance the ability of both spectrally resolved and single band imagery to detect the proliferation of weapons of mass destruction, providing data for locating and identifying facilities, materials, and processes of undeclared and proliferant nuclear weapons programs worldwide. Unfortunately, models do not exist that efficiently and accurately predict spectral polarized signatures for the materials of interest embedded in complex 3D environments. Having such a model would enable one to test hypotheses and optimize both the enhancement of scene contrast and the signal processing for spectral signature extraction. The Phase I set the groundwork for development of fully validated polarimetric spectral signature and scene simulation models. This has been accomplished 1. by (a) identifying and downloading state-of-the-art surface and atmospheric polarimetric data sources, (b) implementing tools for generating custom polarimetric data, and (c) identifying and requesting US Government funded field measurement data for use in validation; 2. by formulating an approach for upgrading the radiometric spectral signature model MODTRAN to generate polarimetric intensities through (a) ingestion of the polarimetric data, (b) polarimetric vectorization of existing MODTRAN modules, and (c) integration of a newly developed algorithm for computing polarimetric multiple scattering contributions; 3. by generating an initial polarimetric model that demonstrates calculation of polarimetric solar and lunar single scatter intensities arising from the interaction of incoming irradiances with molecules and aerosols; 4. by developing a design and implementation plan to (a) automate polarimetric scene construction and (b) efficiently sample polarimetric scattering and reflection events, for use in a to be developed polarimetric version of the existing first-principles synthetic scene simulation model, MCScene; and 5. by planning a validation field measurement program in collaboration with the Remote Sensing and Exploitation group at Sandia National Laboratories (SNL) in which data from their ongoing polarimetric field and laboratory measurement program will be shared and, to the extent allowed, tailored for model validation in exchange for model predictions under conditions and for geometries outside of their measurement domain.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Grating-Based Imaging-Scattering with Portable Neutron Generator

Company: Adelphi Technology, Inc. Title: Grating-Based Imaging-Scattering with Portable Neutron Generator PI: Dr. Jay Theodore Cremer, Jr. Topic: 26a Statement of the problem or situation that is being addressed. Successful plant growth depends upon an efficient and robust root system. The plant root is part of a larger system of water and microbial flows in the soil system. While much effort has been exerted to develop an imaging system for water, microbes, and roots, the problem is challenging, and no widely accepted imaging method currently exists. The optical solutions use a highly modified soil system. X-ray imaging methods are insensitive to the soft tissues in the presence of sand. Thermal neutron imaging has been often tested, but found inadequate, due to limited access and low image resolution. This project will develop a new strategy for neutron imaging of plant/soil systems. The project will allow long duration experiments in greenhouse environments and increase the image information content to the micron scale. General statement of how this problem is being addressed. Portable, rugged thermal and fast neutron sources are being developed where portable means a two-soldier team can carry the source and power unit to survey rough terrain for explosives. In the past decade, microfabrication of X-ray and thermal/cold neutron optics has opened a new imaging strategy. The standard transmission image is now supplemented with simultaneous acquisition of a phase contrast image and an image revealing scattering features. In materials science, the interferometric neutron scattering image has been used to detect early crack formation in stressed additive manufacturing test samples. The detection requires sensitivity to scattering features at the 1-micron scale. By addition of our proposed grating-optic to Adelphi Technology’s radiographic/tomographic imaging system, which is based on portable thermal neutron source, the resulting thermal neutron scatter image of the plant/soil system, will reveal details at 1-micron. Commercial Applications and Other Benefits Neutron interferometry imaging has greater penetration through large metal components compared to industrial X-ray imaging. The low-cost, large area optics developed for greenhouse applications, combined with the robust, portable neutron generator, can then be marketed as a system for inspection of additive manufactured components. In the aerospace industry, all freshly printed components are validated with X-ray CT. Scheduled maintenance again requires X-ray CT as the ability to predict aerospace component lifetime does not yet exist. Large aerospace components are only partially observed with X-ray imaging. Key Words Neutron radiography/tomography, grating interferometry, thermal neutron generator imaging, plant root and soil imaging, rhizosphere imaging, deployable neutron imaging systems Summary for Members of Congress A rugged, portable source of thermal neutrons is adapted for neutron interferometry imaging with the addition of low-cost, 3D printed optics. The first application of our proposed deployable, compact thermal neutron generator imaging system, using a grating optic, is plant root/soil science in greenhouse settings and agricultural laboratories.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗