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At least 19 records

Secondary Ion Mass Spectrometry Methodology for Isotopic Ratio Measurement of Micro‐Grains in Thin Sections: True Grain Size Estimation and Deconvolution of Inter‐Grain Size Gradients and Intra‐Grain Radial Gradients

In a thin section, grains that were approximately spherical in situ appear circular in cross section, and the distribution of apparent diameters frequently assumed to be their size distribution. Scanning ion imaging by secondary ion mass spectrometry (SIMS) is capable of providing precise (< 1‰) stable isotope ratio measurements of such grains, but, importantly, also registers their rate of evolution in apparent size as they are ablated by the primary beam. By assessing rates of radius change with depth, the described methodology enables the ‘true’ size of grains to be estimated, as well as the distance of the sectioned surface from the original grain centre. Transects in three dimensions are made possible, and this capability enables better identification (and thus separation) of both inter‐grain chemical signatures as a function of grain size, and intra‐grain radial trends. In this example, we highlight the specific application to pyrite (FeS 2 ) minerals, which are frequently analysed by SIMS to determine their inter‐grain and intra‐grain geochemical variations, particularly in their sulfur stable isotopic ratios (δ 34 S). Benefits of the new methodology over the Faraday cup ‘spot mode’ are described. Data correction algorithms and precision considerations are discussed.

Jones, Clive↗

Grain-Size Based Additivity Models for Scaling Multi-rate Uranyl Surface Complexation in Subsurface Sediments

This study statistically analyzed a grain-size based additivity model that has been proposed to scale reaction rates and parameters from laboratory to field. The additivity model assumed that reaction properties in a sediment including surface area, reactive site concentration, reaction rate, and extent can be predicted from field-scale grain size distribution by linearly adding reaction properties for individual grain size fractions. This study focused on the statistical analysis of the additivity model with respect to reaction rate constants using multi-rate uranyl (U(VI)) surface complexation reactions in a contaminated sediment as an example. Experimental data of rate-limited U(VI) desorption in a stirred flow-cell reactor were used to estimate the statistical properties of multi-rate parameters for individual grain size fractions. The statistical properties of the rate constants for the individual grain size fractions were then used to analyze the statistical properties of the additivity model to predict rate-limited U(VI) desorption in the composite sediment, and to evaluate the relative importance of individual grain size fractions to the overall U(VI) desorption. The result indicated that the additivity model provided a good prediction of the U(VI) desorption in the composite sediment. However, the rate constants were not directly scalable using the additivity model, and U(VI) desorption in individual grain size fractions have to be simulated in order to apply the additivity model. An approximate additivity model for directly scaling rate constants was subsequently proposed and evaluated. The result found that the approximate model provided a good prediction of the experimental results within statistical uncertainty. This study also found that a gravel size fraction (2-8mm), which is often ignored in modeling U(VI) sorption and desorption, is statistically significant to the U(VI) desorption in the sediment.

Zhang, Xiaoying↗

Grain size variation in nanocrystalline silicon carbide irradiated at elevated temperatures

This study reports on ion irradiation-induced grain growth in nanocrystalline SiC films on Si substrates. The SiC grains with average size ranging from ~2 to 20 nm were embedded in amorphous SiC matrices. Irradiation was performed using 5 MeV Xe23+ ions to 115 ions/nm2 at 700 K. The irradiated films were characterized using x-ray diffraction, transmission electron microscopy and Raman spectroscopy. Significant grain growth is observed for smaller grains that tend to saturate at ~8 nm. In contrast, irradiation of larger grains (~20 nm in size) leads to a decrease in the grain size, which could be associated with the production of lattice disorder within the grains. Homonuclear C-C bonds in the irradiated amorphous SiC matrix are found to be graphitized. This bonding transformation could limit or inhibit grain growth and contribute to the size saturation. The results from this study may suggest nanocrystalline SiC as a promising candidate structural or cladding material for applications in advanced nuclear reactors.

Grain growth, ion irradiation, SiC↗

Radiation pressure on fluffy submicron-sized grains

We investigate the claim that the ratio β of radiation pressure force to gravitational force on a dust grain in our solar system can substantially exceed unity for some grain sizes, provided that grain porosity is high enough. For model grains consisting of random aggregates of silicate spherules, we find that the maximum value of β is almost independent of grain porosity, but for small (<0.3 μm) grains, β actually decreases with increasing porosity. We also investigate the effect of metallic iron and amorphous carbon inclusions in the dust grains and find that while these inclusions do increase the radiation pressure cross-section, β remains below unity for grains with 3 pg of silicate material. These results affect the interpretation of the grain trajectories estimated from the Stardust mission, which were modeled assuming β values exceeding one. We find that radiation pressure effects are not large enough for particles Orion and Hylabrook captured by Stardust to be of interstellar origin given their reported impact velocities. We also consider the effects of solar radiation on transverse velocities and grain spin, and show that radiation pressure introduces both transverse velocities and equatorial spin velocities of several hundred meters per second for incoming interstellar grains at 2 au. These transverse velocities are not important for modeling trajectories, but such spin rates may result in centrifugal disruption of aggregates.

79 ASTRONOMY AND ASTROPHYSICS↗

Impact of Grain Size on Performance Degradation of TREAT LEU

We argue that radiation damage induced degradation of thermal conductivity does not set a lower limit on fuel grain sizes for the low enriched uranium fuel design of the Transient Reactor Test Facility (TREAT). Earlier work reports that smaller grains cause a larger degradation of thermal conductivity than larger grains constraining the smallest feasible size of fuel grains. This work assesses TREAT’s transient performance in the presence of radiation damage. The difference between the two studies is in treating damaged and fresh graphite as serial (this work) or parallel (previous) heat resistors. We use a multiphysics model of TREAT fuel grains to compute the reduction in transient capability measured by the total deposited energy as a function of irradiation dose. We find that radiation damage has a negligible effect on energy deposition.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Phase transformation kinetics in rolled U-10 wt. % Mo foil: Effect of post-rolling heat treatment and prior γ-UMo grain size

The effect of sub-eutectoid heat treatment on the phase transformation behavior in rolled U-10 wt.percent Mo (U10Mo) foils was systematically investigated. The as-cast 5 mm thick foils were initially homogenized at 900 degrees C for 48 hours and were hot rolled to 2 mm and later cold rolled down to 0.2 mm. Three starting microstructures were evaluated: (i) hot- + cold-rolled to 0.2 mm (as-rolled condition), (ii) hot- + cold-rolled to 0.2 mm + annealed at 700 deg. C for 1 hour, and (iii) hot- + cold-rolled to 0.2 mm + annealed at 1000 deg. C for 60 hours. U10Mo rolled foils went through various degrees of decomposition when subjected to the sub-eutectoid heat-treatment step and formed a lamellar microstructure through a cellular reaction mostly along the previous γ-UMo grain boundaries.

Jana, Saumyadeep↗

Correlation between Grain Size Distribution and Grain Boundary Character in Polycrystalline Uranium Dioxide

Thermo-mechanical behavior of oxide nuclear fuels is extremely important to overall fuel element performance. Critical to the understanding of Pellet-Cladding Mechanical Interactions (PCMI) are elasticity, plasticity and creep, as this interaction with the cladding can lead to fuel rod fracture and in turn affect its thermal performance significantly. In addition, sub-grain scale mechanical behavior, e.g. elastic anisotropy, as well as dislocation-driven plasticity and creep, can also play a significant role on microstructure evolution of the fuel elements and their cladding, failure of which would severely reduce the useful service life of the elements and allow the release of fission products out into the working fluid of the reactor. Therefore, careful measurements of mechanical properties are key to validate robust fuel performance codes able to predict this PCMI behavior from inputs at the micro-scale, e.g., MARMOT, and to quantify its effects on other aspects of fuel behavior. In uranium dioxide (UO{sub 2}), the thermomechanical response at the meso-scale depends strongly on crystallography of individual grains, and available datasets are far from complete in terms of temperature, stress, and stoichiometry in parameter space. Therefore, details of the fuel microstructure, such as porosity distribution and location, as well as grain boundary (GB) character, distribution, and location are needed to create accurate multiscale models to predict the fuel's evolution in-pile, and in turn aid in the design and development of more efficient fuels that can last longer cycles.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effects of non-hydrostaticity and grain size on the pressure-induced phase transition of the CoCrFeMnNi high-entropy alloy

Recently, an irreversible polymorphic transition from face-centered cubic to hexagonal close-packing was surprisingly observed under high pressure in the prototype CoCrFeMnNi high-entropy alloys (HEAs) by various research groups. This unexpected phase transition brings new insights into the stability of HEAs, and its irreversibility stimulates exploration for new HEAs via high-pressure compression synthesis. However, the onset pressure for the phase transition was reported to fluctuate over a vast range from ~7 to above 49 GPa in the reported experiments. The reason for this inconsistency remains unclear and puzzles the HEA community. To address this problem, this work systematically investigates the effects of non-hydrostaticity and grain size. Our results demonstrate that larger deviatoric stress induced by the non-hydrostaticity of the pressure medium and larger grain size of the initial sample can both promote a phase transition and, therefore, considerably depress the onset pressure.

36 MATERIALS SCIENCE↗

Novel effects of grain size and ion implantation on grain boundary segregation in ion irradiated austenitic steel

Nuclear reactor environments are extreme in nature due to the combination of exposure to corrosive coolant, mechanical stresses, and neutron irradiation damage. This combination of environments can lead to irradiation induced/assisted precipitation, segregation, and embrittlement coupled with enhanced creep and stress corrosion cracking. While nanostructured materials are of interest in a variety of applications due to their unique properties including high mechanical strength, for nuclear applications nanostructured materials have the added benefit of irradiation resistance due to the high volume density of sinks for irradiation-induced defects. In this study, we show unique radiation-induced segregation (RIS) behavior in nanocrystalline 304 stainless steel (SS304). Typical RIS in austenitic steels includes Ni enrichment and Cr depletion within the grain boundaries. In nanostructured SS304 this RIS is reduced. Furthermore, interestingly, some grain boundaries in the nanocrystalline SS304 in this study were found to be enriched in Cr after Fe 2+ ion irradiation at 500 °C up to 50 displacements per atom (dpa). To understand this unique observation, lattice-based atomic kinetic Monte Carlo simulations were performed to investigate the effects of grain size, thermal segregation, as well as injected interstitials (introduced as Fe self-ions). The results indicate that the Cr enrichment at grain boundaries may be caused by combined effects of grain size, self-ion injection and preferential Cr diffusion via the interstitial mechanism. In conclusion, the findings also suggest a possible difference in RIS between ion and neutron irradiations.

36 MATERIALS SCIENCE↗

Estimation of volume-weighted average grain size in Fe-based nanocrystalline soft magnetic materials by autocorrelation function

Highlights: • Normalized ACF of TEM images estimates the volume-weighted average grain size. • Grain size estimation by normalized ACF shows good accuracy and time efficiency. • Normalized ACF can reveal grain size difference in different areas of a TEM sample. • Normalized ACF helps modelling of grain size distributions in Fe-B nanostructures. - Abstract: The coercivity of Fe-based nanocrystalline soft magnetic materials depends critically on the grain size of bcc-Fe grains. Accurately estimating the volume-weighted mean grain size is extremely important to develop new Fe-based nanocrystalline soft magnetic materials with low coercivity. This article shows that autocorrelation analysis of dark-field transmission electron microscope (TEM) images provides a very good estimation of bcc-Fe grain size in nanocrystalline soft magnetic materials. This method can be used to efficiently estimate the volume-weighted average grain size from multiple TEM images with much less inherent bias than manual measurement techniques. The estimated grain sizes show good consistency to the grain sizes estimated by X-ray diffraction (XRD) and manual measurement. In contrast to XRD, this method can also reveal the differences in grain size from different micron-sized regions of a sample.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

The Effect of Grain Size on the Strain Hardening Behavior for Extruded ZK61 Magnesium Alloy

The effects of grain size on the tensile and compressive strain hardening behaviors for extruded ZK61 alloys have been investigated by uniaxial tensile and compressive tests along the extrusion directions. Cylindrical tension and compression specimens of extruded ZK61 alloys with various sized grain were fabricated by annealing treatments. Tensile and compressive tests at ambient temperature were conducted at a strain rate of 0.5 × 10{sup −3} s{sup −1}. The results indicate that both tensile strain hardening and compressive strain hardening of ZK61 alloys with different grain sizes have an athermal regime of dislocation accumulation in early deformation. The threshold stress value caused dynamic recovery is predominantly related to grain size in tensile strain hardening, but the threshold stress values for different grain sizes are almost identical in compressive strain hardening. There are obvious transition points on the tensile strain hardening curves which indicate the occurrence of dynamic recrystallization (DRX). The tensile strain hardening rate of the coarse-grained alloy obviously decreases faster than that of fine-grained alloys before DRX and the tensile strain hardening curves of different grain sizes basically tend to parallel after DRX. The compressive strain hardening rate of the fine-grained alloy obviously increases faster than that of coarse-grained alloy for twin-induced strain hardening, but compressive strain hardening curves also tend to parallel after twinning is exhausted.

36 MATERIALS SCIENCE↗