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Nonclassical acoustics

A statistical approach to sound propagation is considered in situations where, due to the presence of large gradients of properties of the medium, the classical (deterministic) treatment of wave motion is inadequate. Mathematical methods for wave motions not restricted to small wavelengths (analogous to known methods of quantum mechanics) are used to formulate a wave theory of sound in nonuniform flows. Nonlinear transport equations for field probabilities are derived for the limiting case of noninteracting sound waves and it is postulated that such transport equations, appropriately generalized, may be used to predict the statistical behavior of sound in arbitrary flows.

Kentzer, C. P.↗

Simulating Atmospheric Turbulence

Dimensionless time series for gusts and gradients calculated with model. Single-sided one-dimensional spectra obtained from Fourier analysis of simulated vertical gust. Each of four plots represents spectrum in one of four altitude bands ranging from 0 to 10 km. Model differs from most models; is nondimensional for greater generality and uses spectra with finite wave number limits. Developed to predict effects of atmospheric turbulence in horizontal and near-horizontal flight also applicable to commercial aviation.

Tatom, F. B.↗

Distributed computer system enhances productivity for SRB joint optimization

Initial calculations of a redesign of the solid rocket booster joint that failed during the shuttle tragedy showed that the design had a weight penalty associated with it. Optimization techniques were to be applied to determine if there was any way to reduce the weight while keeping the joint opening closed and limiting the stresses. To allow engineers to examine as many alternatives as possible, a system was developed consisting of existing software that coupled structural analysis with optimization which would execute on a network of computer workstations. To increase turnaround, this system took advantage of the parallelism offered by the finite difference technique of computing gradients to allow several workstations to contribute to the solution of the problem simultaneously. The resulting system reduced the amount of time to complete one optimization cycle from two hours to one-half hour with a potential of reducing it to 15 minutes. The current distributed system, which contains numerous extensions, requires one hour turnaround per optimization cycle. This would take four hours for the sequential system.

Rogers, James L., Jr.↗

Preparative electrophoresis for space

A premise of continuous flow electrophoresis is that removal of buoyancy-induced thermal convection caused by axial and lateral temperature gradients results in ideal performance of these instruments in space. Although these gravity dependent phenomena disturb the rectilinear flow in the separation chamber when high voltage gradients or thick chambers are used, distortion of the injected sample stream due to electrohydrodynamic effects cause major broadening of the separated bands. The electrophoresis separation process is simple, however flow local to the sample filament produced by the applied electric field have not been considered. These electrohydrodynamic flows distort the sample stream and limit the separation. Also, electroosmosis and viscous flow combine to further distort the process. A moving wall concept is being proposed for space which will eliminate and control the disturbances. The moving wall entrains the fluid to move as a rigid body and produces a constant residence time for all samples distributed across the chamber thickness. The moving wall electrophoresis chamber can only be operated in space because there is no viscous flow in the chamber to stabilize against thermal convection.

Rhodes, Percy H.↗

The accuracy of dynamic attitude propagation

Propagating attitude by integrating Euler's equation for rigid body motion has long been suggested for the Earth Radiation Budget Satellite (ERBS) but until now has not been implemented. Because of limited Sun visibility, propagation is necessary for yaw determination. With the deterioration of the gyros, dynamic propagation has become more attractive. Angular rates are derived from integrating Euler's equation with a stepsize of 1 second, using torques computed from telemetered control system data. The environmental torque model was quite basic. It included gravity gradient and unshadowed aerodynamic torques. Knowledge of control torques is critical to the accuracy of dynamic modeling. Due to their coarseness and sparsity, control actuator telemetry were smoothed before integration. The dynamic model was incorporated into existing ERBS attitude determination software. Modeled rates were then used for attitude propagation in the standard ERBS fine-attitude algorithm. In spite of the simplicity of the approach, the dynamically propagated attitude matched the attitude propagated with good gyros well for roll and yaw but diverged up to 3 degrees for pitch because of the very low resolution in pitch momentum wheel telemetry. When control anomalies significantly perturb the nominal attitude, the effect of telemetry granularity is reduced and the dynamically propagated attitudes are accurate on all three axes.

Harvie, E.↗

Low-frequency modes and nonbarotropic effects in pseudo-Newtonian accretion disks

A recently developed formalism is used to reexamine the question of the existence of hydrodynamical modes that pulsate with very low frequencies in the inner regions of accretion disks. The formalism is valid in an exact sense for the adiabatic pulsations of rotating Newtonian fluids that are generally nonbarotropic (such as those with 'nonadiabatic temperature gradients,' for example), and hence its application in the present context represents an improvement over previous analyses that are more approximate. The formalism is applied to thin non-self-gravitating disks, with the gravitational potential of the central source modified in the usual way in order to simulate relativistic effects. In the barotropic limit, the analyses indicate that in many cases nearly Keplerian disks exhibit nonaxisymmetric modes of pulsation that are trapped in the inner disk regions, with pulsation periods much longer than the dynamical timescale. These results are similar to those of earlier calculations that assume disks pulsate without changing the temperature distribution. A method is developed for including lowest order nonbarotropic effects. Previous analyses have been incapable of accurately treating the nonbarotropic regime. The application of the present method to the low-frequency modes reveals that, due to unexpected cancellations among terms, the nonbarotropic correction to the pusation frequency omega is only of order tilde-omega(sub BV exp 2) omega, where tilde-omega(sub BV) is the appropriate dimensionless Brunt-Vaisala frequency. This correction is much smaller than the expected correction of order tilde-omega(sub BV) Omega, where Omega is the rotation angular velocity. The important conclusion drawn from this is that nonbarotropic corrections are generally small and hence that low-frequency modes persist into the nonbarotropic regime. For disk temperatures appropriate to X-ray emission, the adiabatic frequencies of trapped modes are of the same order as the frequencies associated with quasi-periodic oscillations (QPOs) of certain low-mass X-ray binaries and other X-ray sources. It is suggested that further consideration be given to the possiblity that modulation of emission processes by these modes can explain at least some of the QPO phenomena.

Ipser, James R.↗

The Onset of the Madden-Julian Oscillation Within an Aquaplanet Model

A series of numerical experiments using a two-level atmospheric general circulation model (AGCM) were performed for the purpose of investigating the coupling between sea surface temperature (SST) profile and the onset of the Madden-Julian Oscillation (MJO). The AGCM was modified to run as an aquaplane with all seasonal forcing removed. SST distributions based on the New Global Sea-Ice and Sea Surface Temperature (GISST) Data Set for 1903-1994 were generated then modified to vary the north-south gradient and tropical temperatures. It was found that the MJO signal did not depend on the SST temperature gradients but rather on the absolute temperature of the equatorial region, EOF analysis revealed that the SST distribution which generated the strongest MJO signal produced a periodic fluctuation in velocity potential at the 250 millibar level with a phase speed of 15 m/s, and a periodicity of 30 days which falls within the shortest limit of observed oscillations. This distribution also possessed the coolest equatorial SSTs which suggests that increased stability in the atmosphere favors the occurrence of organized MJO propagation.

Colon, Edward↗

Assimilation of SMAP Observations Over Land Improves the Simulation and Prediction of Tropical Cyclone Idai

This work is focused on the role of soil moisture in the prediction of tropical cyclones (TCs) approaching land and after landfall. Soil moisture conditions can impact the circulation and structure of an existing tropical cyclone (TC) when part or all of the circulation is over land. For example, dry land surface conditions may lead to faster dissipation of a TC over land (often associated with changes in precipitation structure), whereas very wet conditions may help sustain or in rare cases re-intensify a TC. Moreover, the presence of strong soil moisture gradients may affect the symmetry and development of the TC circulation leading to changes in its over-land track. While the link between soil moisture conditions and TC evolution in proximity to land is relatively well understood in theory, applications of these findings in the context of numerical weather prediction (NWP) have been limited. Here we present a case study that explores the potential of improving TC predictions through an improved soil moisture initialization in an NWP framework. Specifically, we examine the impact of assimilating observations from the NASA Soil Moisture Active Passive (SMAP) mission into the NASA Goddard Earth Observing System (GEOS) global weather model on the prediction of South-West Indian Ocean TC Idai (2019). SMAP provides accurate L-band (1.4 GHz) brightness temperatures (Tb) observations that are sensitive to soil moisture globally and at high revisit times of 2-3 days. It has previously been shown that the assimilation of SMAP Tb observations significantly improves modeled land surface states. Thus, it is expected that SMAP can be used to constrain land surface initial conditions and potentially benefit TC forecasts. Here we present two sets of retrospective forecasts of TC Idai that are compared in an Observing System Experiment framework at ¼ degree resolution: (i) forecasts initialized from an analysis that is comparable to the GEOS operational analysis (without SMAP Tb assimilation) and (ii) forecasts initialized from an analysis that additionally assimilates SMAP brightness temperature observations over land using a weakly-coupled land analysis. We find that the assimilation of SMAP meaningfully improves the representation of TC Idai’s structure as well as the prediction of its intensity and track. The analyzed TC size, as measured by the wind speed radius, is improved by up to 18% in the analysis with SMAP assimilation relative to the control run. The forecast intensity error, measured against the observed intensity, is reduced by up to 23%. At the 1/4-degree resolution used here, GEOS unavoidably under-estimates TC intensity and over-estimates TC size. The SMAP assimilation therefore corrects the model in the right direction, leading to a storm that is more energetic and more compact. Furthermore, we find that the along-track forecast error is reduced by up to 34%, indicating a more accurate propagation speed, which is consistent with the fact that TC speed over land is strongly affected by surface processes. The impact of SMAP assimilation on the forecast cross-track error is neutral. Across the TC forecast skill metrics used here, the improvements from SMAP DA are largest at lead times of 36 to 72 hours, suggesting that the predictability of forecasts at shorter lead times may be dominated by short-term convective processes, while the land and its longer memory gains in importance as a source of predictability on a 2-3 day timescale. We further investigated the underlying mechanisms leading to the skill improvements from SMAP data assimilation by isolating the land areas that directly influence TC Idai using a back trajectory analysis. We find that the assimilation of SMAP leads to wetter soil moisture conditions that cause an increased latent heat flux, which ultimately results in TC analyzed representation that has higher column-integrated total moisture content and total energy compared to the analysis in the control run without SMAP assimilation. Overall, the results highlight that the assimilation of SMAP observations into a global numerical weather prediction model can lead to pronounced improvements of TC predictions. This is a crucial step towards a better mitigation of the socio-economic impact of landfalling TCs and thus safeguarding human lives. Finally, our study presents an event-based approach that assesses the impact of land data assimilation for a particular weather event rather than by globally averaging differences in skill. We argue that global skill assessments – while necessary – can mute the impact of land data assimilation, because the land’s influence on the atmosphere is constrained to certain locations and certain times. Instead, the event-based approach better highlights the true potential of land data assimilation in the context of NWP, especially for extreme events when accurate predictions are critical.

Jana Kolassa↗

Assimilation of SMAP Observations Over Land Improves the Simulation and Prediction of Tropical Cyclone Idai

This work is focused on the role of soil moisture in the prediction of tropical cyclones (TCs) approaching land and after landfall. Soil moisture conditions can impact the circulation and structure of an existing tropical cyclone (TC) when part or all of the circulation is over land. For example, dry land surface conditions may lead to faster dissipation of a TC over land (often associated with changes in precipitation structure), whereas very wet conditions may help sustain or in rare cases re-intensify a TC. Moreover, the presence of strong soil moisture gradients may affect the symmetry and development of the TC circulation leading to changes in its over-land track. While the link between soil moisture conditions and TC evolution in proximity to land is relatively well understood in theory, applications of these findings in the context of numerical weather prediction (NWP) have been limited. Here we present a case study that explores the potential of improving TC predictions through an improved soil moisture initialization in an NWP framework. Specifically, we examine the impact of assimilating observations from the NASA Soil Moisture Active Passive (SMAP) mission into the NASA Goddard Earth Observing System (GEOS) global weather model on the prediction of South-West Indian Ocean TC Idai (2019). SMAP provides accurate L-band (1.4 GHz) brightness temperatures (Tb) observations that are sensitive to soil moisture globally and at high revisit times of 2-3 days. It has previously been shown that the assimilation of SMAP Tb observations significantly improves modeled land surface states. Thus, it is expected that SMAP can be used to constrain land surface initial conditions and potentially benefit TC forecasts. Here we present two sets of retrospective forecasts of TC Idai that are compared in an Observing System Experiment framework at ¼ degree resolution: (i) forecasts initialized from an analysis that is comparable to the GEOS operational analysis (without SMAP Tb assimilation) and (ii) forecasts initialized from an analysis that additionally assimilates SMAP brightness temperature observations over land using a weakly-coupled land analysis. We find that the assimilation of SMAP meaningfully improves the representation of TC Idai’s structure as well as the prediction of its intensity and track. The analyzed TC size, as measured by the wind speed radius, is improved by up to 18% in the analysis with SMAP assimilation relative to the control run. The forecast intensity error, measured against the observed intensity, is reduced by up to 23%. At the 1/4-degree resolution used here, GEOS unavoidably under-estimates TC intensity and over-estimates TC size. The SMAP assimilation therefore corrects the model in the right direction, leading to a storm that is more energetic and more compact. Furthermore, we find that the along-track forecast error is reduced by up to 34%, indicating a more accurate propagation speed, which is consistent with the fact that TC speed over land is strongly affected by surface processes. The impact of SMAP assimilation on the forecast cross-track error is neutral. Across the TC forecast skill metrics used here, the improvements from SMAP DA are largest at lead times of 36 to 72 hours, suggesting that the predictability of forecasts at shorter lead times may be dominated by short-term convective processes, while the land and its longer memory gains in importance as a source of predictability on a 2-3 day timescale. We further investigated the underlying mechanisms leading to the skill improvements from SMAP data assimilation by isolating the land areas that directly influence TC Idai using a back trajectory analysis. We find that the assimilation of SMAP leads to wetter soil moisture conditions that cause an increased latent heat flux, which ultimately results in TC analyzed representation that has higher column-integrated total moisture content and total energy compared to the analysis in the control run without SMAP assimilation. Overall, the results highlight that the assimilation of SMAP observations into a global numerical weather prediction model can lead to pronounced improvements of TC predictions. This is a crucial step towards a better mitigation of the socio-economic impact of landfalling TCs and thus safeguarding human lives. Finally, our study presents an event-based approach that assesses the impact of land data assimilation for a particular weather event rather than by globally averaging differences in skill. We argue that global skill assessments – while necessary – can mute the impact of land data assimilation, because the land’s influence on the atmosphere is constrained to certain locations and certain times. Instead, the event-based approach better highlights the true potential of land data assimilation in the context of NWP, especially for extreme events when accurate predictions are critical.

Jana Kolassa↗

Evaluation of Vertical Patterns in Chlorophyll-A Derived From A Data Assimilating Model of Satellite-Based Ocean Color

Satellite-based sensors of ocean color have become the primary tool to infer changes in surface chlorophyll, while BGC-Argo floats are now filling the information gap at depth. Here we use BGC-Argo data to assess depth-resolved information on chlorophyll-a derived from an ocean biogeochemical model constrained by the assimilation of surface ocean color remote sensing. The data-assimilating model replicates well the general seasonality and meridional gradients in surface and depth-resolved chlorophyll-a inferred from the float array in the Southern Ocean. On average, the model tends to overestimate float-based chlorophyll, particularly at times and locations of high productivity such as the beginning of the spring bloom, subtropical deep chlorophyll maxima, and non-iron limited regions of the Southern Ocean. The highest model RMSE in the upper 50 m with respect to the float array is of 0.6 mg Chl m −3 , which should allow the detection of seasonal changes in float-based biomass (varying between 0.01 and >1 mg Chl m −3 ) but might hinder the identification of subtle changes in chlorophyll at narrow local scales. Both model and float profiling data show good agreement with in situ data from station ALOHA, with model estimates showing a slight accuracy edge in inferring depth-resolved observations. Uncertainties in float bio-optical estimates impede their use as a reliable benchmark for validation, but the general qualitative agreement between model and float data provides confidence in the ability of model to replicate biogeochemical features below the surface, where data is not directly constrained by the assimilation of satellite ocean color.

Lionel A Quintero↗

Performance of first prototype multi-cell low-surface-field shape cavity

The idea of cavity shaping for higher ultimate acceleration gradients has been proposed for some time, Low Loss/Ichiro and Re-entrant being examples, both seeking a lower Hpk/Eacc at the expense of a higher Epk/Eacc. While experimental verification in single-cell cavities of those shapes was very successful including the record gradient of 59 MV/m, pushing multi-cell cavities of those shapes to higher gradients was prevented by field emission. The Low-Surface-Field (LSF) shape seeks not only a lower Hpk/Eacc but also a lower Epk/Eacc, therefore it has the advantage of raising ultimate gradient at reduced field emission. The first multi-cell LSF shape prototype cavity was built using the standard forming and welding techniques. RF tests have been carried out, following standard ILC TDR baseline surface processing and treatment recipe. Three out of five cells achieved Hpk values corresponding to Eacc 50 MV/m. The current limit is the field emission in end cells. Instrumented testing following end-cell wiping and HPR with larger nozzles is in progress. We will present detailed experimental results and preparation procedures.

Geng, R.-L.↗

Modelling and Experimental Validation of Improved Performance of Lithium-Ion Batteries Having Thick Electrodes with Laser-Ablated Micro-Structures

For widespread adoption of electric vehicles, lithium-ion batteries (LiBs) need to achieve energy densities of >275 Wh/kg, cost less than $100/Wh, and charge to more than 80% capacity within 15 minutes. Increasing the battery electrode thicknesses is one way to increase cell energy densities while also saving on cell manufacturing cost by increasing the ratio of electrode active material to inactive material within each cell. However, increased electrode loading is often accompanied by decreased Li+-ion diffusion across the full thick electrodes. This leads to significant cell polarization that prevents full capacity utilization and accelerates cell degradation, especially at fast charging/discharging rates. The introduction of secondary pore networks in thick battery electrodes alleviates some of the trade-offs between energy and power performance. These microstructures provide low tortuosity pathways for facile Li+-ion diffusion deep into the thick electrodes, diminishing detrimental concentration gradients within the cell. Ultrafast-pulsed laser ablation is a promising method to introduce micro pores or channels in thick battery electrodes as it allows for precise control of pattern geometries, results in minimal damage to the electrode and can be introduced into existing roll-to-roll electrode manufacturing lines. Herein, the limitations of thick planer electrodes and the advanced predictive models to identify optimal electrode patterns for improved cycling performance will be presented. The impact of electrode laser patterning to create secondary pore networks also will be discussed. Materials characterization techniques (SEM-EDS, XRD) were used to explore the affect ultrafast laser ablation had on the electrode materials’ morphology and structure. The improvements in the patterned electrodes’ electrochemical cycling performances and degrees of wetting will be compared to a pristine baseline case. Finally, the discrepancies between experimentally obtained data and model predictions will be explained.

DIRECT ENERGY CONVERSION,ENERGY STORAGE↗

Topological Guided Detection of Extreme Wind Phenomena: Implications for Wind Energy: Preprint

Extreme wind phenomena play a crucial role in the efficient operation of wind farms for renewable energy generation. However, existing detection methods are computationally expensive, limited to specific coordinate. In real-world scenarios, understanding the occurrence of these phenomena over a large area is essential. Therefore, there is a significant demand for a fast and accurate approach to forecast such events. In this paper, we propose a novel method for detecting wind phenomena using topological analysis, leveraging the gradient of wind speed or critical points in a topological framework. By extracting topological features from the wind speed profile within a defined region, we employ topological distance to identify extreme wind phenomena. Our results demonstrate the effectiveness of utilizing topological features derived from regional wind speed profiles. We validate our approach using high-resolution simulations with the Weather Research and Forecasting model (WRF) over a month in the US East Coast.

MATHEMATICS AND COMPUTING,WIND ENERGY↗

Phase Equilibria in Systems Relevant to Pyroprocessing

Pyroprocessing has many advantages for the recovery and recycle of actinides, especially the transuranic elements, in used nuclear fuel. It has several unique features that distinguish it from other used fuel treatment technologies such as the ability to handle short-cooled fuel, a small process footprint, and production of metallic uranium and uranium - transuranic (U/TRU) products that can be directly fabricated into metallic fuel for advanced reactors. Recovery of the uranium and U/TRU products from the used fuel occurs in an electrorefining step. Uranium and transuranics in the used fuel (metal or reduced oxide) are dissolved at the anode in a molten chloride electrolyte, and electrodeposited at two different cathodes - one for uranium and another for the uranium - transuranic product. During this process, fission products less noble than uranium and transuranics (i.e., lanthanides, alkali and alkaline earth) anodically dissolve into the electrolyte, while only uranium and U/TRU are electrodeposited at the respective cathodes. Thus, there is a buildup of active metal and lanthanide fission products in the molten salt electrolyte. The goal of this work is to improve the fundamental understanding of the chemistry of actinides and transuranics in this complex, multicomponent solution. The fundamental thermodynamic properties of the multi-component molten salt electrolytes are complicated due to the formation of ternary and more complex compounds. As the actinides anodically dissolve at the anode and deposited at the cathode, a gradient in the concentration develops at the anode/electrolyte and the cathode/electrolyte interfaces. Ternary phase formation could impact the performance of the electrorefining system by influencing the chemical activity and thus the redox potentials of the actinide chlorides in the molten salt solution. Literature data on the LiCl-KCl-UCl{sub 3} system is limited, sometimes conflicting, and may reflect the use of older analytical instrumentation, which was less accurate than that currently available. In addition, there has not been any investigation of the low UCl{sub 3} concentration region of the system, which is the region relevant to electrorefining. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Precipitation mediates sap flux sensitivity to evaporative demand in the neotropics

Transpiration in humid tropical forests modulates the global water cycle and is a key driver of climate regulation. Yet, our understanding of how tropical trees regulate sap flux in response to climate variability remain elusive. With a progressively warming climate, atmospheric evaporative demand (i.e., vapor pressure deficit, VPD) will be increasingly important for plant functioning, becoming the major control of plant water use in the 21st century. Using measurements in 34 tree species at seven sites across a precipitation gradient in the neotropics, we determined how the maximum sap flux velocity (vmax) and the VPD threshold at which vmax is reached (VPDmax) vary with precipitation regime (long-term annual precipitation, MAP; seasonal drought intensity, PDRY) and two functional traits related to foliar and wood economics spectra (leaf mass per area, LMA; wood specific gravity, WSG). We show that, even though vmax is highly variable within sites, it follows a negative trend in response to increasing MAP and PDRY across sites. LMA and WSG exerted little effect on vmax and VPDmax, suggesting that these widely-used integrative traits provide limited explanatory power of dynamic plant responses to environmental variation within hyper-diverse forests. This study demonstrates that long-term precipitation plays an important role in the sap flux response of humid tropical forests to VPD. Our findings suggest that under higher evaporative demand, trees growing in wetter environments in humid tropical regions may be subjected to reduced water exchange with the atmosphere relative to trees growing in drier climates.

Grossiord, Charlotte↗

Improved proton computed tomography by dual modality image reconstruction

Purpose: Proton computed tomography (CT) is a promising image modality for improving the stopping power estimates and dose calculations for particle therapy. However, the finite range of about 33 cm of water of most commercial proton therapy systems limits the sites that can be scanned from a full 360° rotation. In this paper the authors propose a method to overcome the problem using a dual modality reconstruction (DMR) combining the proton data with a cone-beam x-ray prior. Methods: A Catphan 600 phantom was scanned using a cone beam x-ray CT scanner. A digital replica of the phantom was created in the Monte Carlo code Geant4 and a 360° proton CT scan was simulated, storing the entrance and exit position and momentum vector of every proton. Proton CT images were reconstructed using a varying number of angles from the scan. The proton CT images were reconstructed using a constrained nonlinear conjugate gradient algorithm, minimizing total variation and the x-ray CT prior while remaining consistent with the proton projection data. The proton histories were reconstructed along curved cubic-spline paths. Results: The spatial resolution of the cone beam CT prior was retained for the fully sampled case and the 90° interval case, with the MTF = 0.5 (modulation transfer function) ranging from 5.22 to 5.65 linepairs/cm. In the 45° interval case, the MTF = 0.5 dropped to 3.91 linepairs/cm For the fully sampled DMR, the maximal root mean square (RMS) error was 0.006 in units of relative stopping power. For the limited angle cases the maximal RMS error was 0.18, an almost five-fold improvement over the cone beam CT estimate. Conclusions: Dual modality reconstruction yields the high spatial resolution of cone beam x-ray CT while maintaining the improved stopping power estimation of proton CT. In the case of limited angles, the use of prior image proton CT greatly improves the resolution and stopping power estimate, but does not fully achieve the quality of a 360° proton CT scan.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Nanoscale Mechanical Behavior of Nuclear Materials

One of the primary performance objectives targeted for improved performance of nuclear fuels is fracture toughness. New materials or composite fuel architectures that offer greater resistance to cracking under the extreme environments encountered during nuclear reactor service would provide significant improvements to steady state (e.g. heat transfer, fuel redistribution) and transient (e.g. radionuclide release at elevated temperatures) conditions. Options currently under investigation include 'nontraditional' nuclear fuels designated around high uranium density. These include uranium silicides, uranium borides, and composite fuel materials constructed of these and uranium nitride or uranium dioxide. The increase uranium density compared with uranium dioxide (UO{sub 2}) has made them interesting to a new generation of nuclear fuels research driven by the renewed push for accident-tolerant light water reactor (LWR) fuels. Measurement of the thermophysical and thermodynamic properties of these constituent materials has progressed in recent years, but evaluation of mechanical properties at relevant temperatures is necessary to support further evaluations. While thermophysical properties such as thermal conductivity, heat capacity, and thermal expansion are generally the primary properties of interest, mechanical properties will play an important role in governing the deformation and fracture of the fuel during both normal operation and potential transients. It is therefore necessary to develop techniques capable of measuring these properties to predict the response of a candidate fuel form to anticipated thermal gradients. Nanoindentation techniques provide a demonstrated alternative to traditional mechanical test methods. Much work has also been carried out over the past few years to obtain stress-strain curves using a spherical nanoindentation approach. The techniques are expected to be useful for measurement of the mechanical properties of local structure of various materials. Nanomechanical test techniques have particular value in the area of nuclear materials, where numerous factors motivate limiting the sample volume to the extent possible. However, few attempts at application of nanoindentation to evaluate the mechanical properties of the nuclear fuels and cladding materials are reported in the literature. The effect of a limited set of variables (e.g. porosity, temperature dependence) on the mechanical properties of UO{sub 2} has been explored using early nanomechanical testing techniques. However, nanomechanical evaluation has not been extended to other nuclear fuels. In this work, we demonstrate the effectiveness of using instrumented spherical nanoindentation test techniques to capture the mechanical response of regions within individual grains in ion-irradiated W and Zr over a range of ion-irradiation conditions. As well as the nanomechanical response of U-Si and UO{sub 2} fuel materials Nanoindentation results obtained at room temperature will be used to express nano- and bulk- mechanical properties as a function of material stoichiometry. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Contribution of atom-probe tomography to a better understanding of glass alteration mechanisms: Application to a nuclear glass specimen altered 25 years in a granitic environment

Here, we report and discuss results of atom probe tomography (APT) and energy-filtered transmission electron microscopy (EFTEM) applied to a borosilicate glass sample of nuclear interest altered for nearly 26 years at 90°C in a confined granitic medium in order to better understand the rate-limiting mechanisms under conditions representative of a deep geological repository for vitrified radioactive waste. The APT technique allows the 3D reconstruction of the elemental distribution at the reactive interphase with sub-nanometer precision. Profiles of the B distribution at pristine glass/hydrated glass interface obtained by different techniques are compared to show the challenge of accurate measurements of diffusion profiles at this buried interface on the nanometer length scale. Our results show that 1) Alkali from the glass and hydrogen from the solution exhibit anti-correlated 15 ± 3 nm wide gradients located between the pristine glass and the hydrated glass layer, 2) boron exhibits an unexpectedly sharp profile located just at the outside of the alkali/H interdiffusion layer; this sharp profile is more consistent with a dissolution front than a diffusion-controlled release of boron. The resulting apparent diffusion coefficients derived from the Li and H profiles are D Li = 1.5 × 10 -22 m 2 .s -1 and D H = 6.8 × 10 -23 m 2 .s -1 . These values are around two orders of magnitude lower than those observed at the very beginning of the alteration process, which suggests that interdiffusion is slowed at high reaction progress by local conditions that could be related to the porous structure of the interphase. As a result, the accessibility of water to the pristine glass could be the rate-limiting step in these conditions. More generally, these findings strongly support the importance of interdiffusion coupled with hydrolysis reactions of the silicate network on the long-term dissolution rate, contrary to what has been suggested by recent interfacial dissolution-precipitation models for silicate minerals.

36 MATERIALS SCIENCE↗