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At least 19 records

A quantitative method to determine the region not influenced by injected interstitial and surface effects during void swelling in ion-irradiated metals

We propose and demonstrate a microstructurally-based experimental method to quantitively determine the depth regions in self-ion-irradiated metals that are affected by the injected interstitial effect and various surface effects, focusing on the choice of safe analysis zones to minimize the impact of these phenomena. The goal is to define the depth ranges where extracted data can be confidently applied to ion-neutron correlations for reactor application. Since ion energies in the range of 1–5 MeV are most frequently employed by the radiation effects community, irradiations were conducted at four energies in this range, all proceeding at 475 °C. The experiment was conducted on relatively pure single crystal iron to focus only on physical phenomena, avoiding the influence of possibly confounding chemical or segregation processes. Care was also taken to minimize the influence of other physical factors such as crystalline orientation. It was shown that, at 475 °C, ion energies of ≤1 MeV were too shallow in penetration and did not yield a safe depth range, but irradiations at 2.5 MeV and above yielded useful safe zones with predicted swelling behavior becoming independent of ion energy. The surface-affected zone width was found to be roughly twice that of the void-denuded zone width and to be independent of accumulated displacement dose. The largest injected-interstitial effect arises from the injected interstitial depression of void nucleation and growth. The interstitial-affected region starts at about one half of the projected range and does not show any “spreading” of its influence in depth as the peak damage level increases from 50 to 100 dpa. This study provides some confidence that enhances the credibility of ion simulation when applied to prediction of void swelling in neutron environments.

36 MATERIALS SCIENCE↗

Towards Quantitative Inference of Nanoscale Defects in Irradiated Metals and Alloys

Quantifying the population of nanoscale defects that are formed in metals and alloys exposed to extreme radiation environments remains a pressing challenge in materials science. These defects both fundamentally alter material properties and seed long-timescale performance degradation, which often limits the lifespan of engineering systems. Unlike ceramic and semiconducting materials, these defects in metals and alloys are not spectroscopically active, forcing characterization to rely on indirect measurements from which the distribution of nanoscale defects may be inferred. In this mini-review, different experimental methodologies which have been employed for defect inference are highlighted to capture the current state of the art. Future directions in this area are proposed, which, by combining data streams from multiple and complementary characterization methods in concert with multi-scale modeling and simulation, will enable the ultimate goal of quantifying the full spectrum of defects in irradiated metals and alloys.

Hirst, Charles A.↗

Analysis of position-dependent cavity parameters in irradiated metals to obtain insight on fundamental defect migration phenomena

Motion of point defects is a fundamental process that governs microstructure and properties of materials. Here, we examine the near-surface and grain boundary cavity swelling depth profiles in neutron- and ion-irradiated simple metals (Cu, Ni, and Fe-Cr) and investigate diffusional broadening of implanted Ni ions in Fe-Cr alloys. Vacancy migration energies and radiation-enhanced diffusion were experimentally estimated. Cavity denuded zone widths near planar sinks are shown to be dependent on temperature, damage rate, balance of point defects and sinks, and vacancy migration energies. An enhanced cavity swelling zone adjacent to the void-denuded zone was observed in specimens with low to moderate sink strength and interpreted as evidence of 1D gliding interstitial clusters. Radiation-enhanced diffusional broadening of implanted Ni ions (at 400–550 °C) in Fe and Fe-Cr was up to 250 nm toward the surface, which leads to a much broader near-peak-damage region where cavity swelling is suppressed. Diffusional broadening of implanted ions is calculated to be similarly pronounced for self-ion irradiations, particularly near the peak and higher swelling temperature regimes. Adequately high ion energies (~8–15 MeV) are recommended for ion-irradiation studies to provide a sufficiently broad midrange safe analysis region with minimized surface and injected ion effects.

36 MATERIALS SCIENCE↗

Depth-resolved thermal conductivity and damage in swift heavy ion irradiated metal oxides

We investigated thermal transport in swift heavy ion (SHI) irradiated insulating single crystalline oxide materials: yttrium aluminum garnet- Y 3 Al 5 O 12 (YAG), sapphire (Al 2 O 3 ), zinc oxide (ZnO) and magnesium oxide (MgO) irradiated by 167 MeV Xe ions at 10 12 – 10 14 ions/cm 2 fluences. Depth profiling of the thermal transport on nano- and micro- meter scales was assessed by time-domain thermoreflectance (TDTR) and modulated thermoreflectance (MTR) methods, respectively. This combination allowed us to isolate the conductivities of different sub-surface damage-regions characterized by their distinct microstructure evolution regimes. Thermal conductivity degradation in SHI irradiated YAG and Al 2 O 3 is attributed to formation of ion tracks and subsequent amorphization, while in ZnO and MgO it is mostly due to point defects. Additionally, notably lower conductivity when probed by very low penetrating thermal waves is consistent with surface hillock formation. An analytical model based on Klemens-Callaway method for thermal conductivity coupled with a simplified microstructure evolution capturing saturation in defect concentration was used to obtain depth dependent damage across the ion impacted region. The studies showed that YAG has the highest damage profile resulting in the less dependence of thermal conductivity with the depth, while MgO on the contrary has the strongest dependence. The presented work sheds new light on how SHI induced defects affect thermal transport degradation and recovery of oxide ceramics as promising candidates for next generation nuclear reactor applications.

36 MATERIALS SCIENCE↗

Temperature Measurement of Laser-Irradiated Metals Using Hyperspectral Imaging

Accurate noncontact surface-temperature measurements during laser-based materials processing remain challenging due to the difficulty of establishing reliable emissivity values as a function of temperature and wavelength. Direct measurement of emissivity is difficult, as the emissivity may be changing constantly in the laser-material interaction region, where the temperature gradients are extreme and surface displacement can complicate the measurement. Here, we present a hyperspectral imaging method using a multiwavelength camera to capture the spectral radiance in eight different bands and fit the wavelength-dependent radiance to Planck’s law. Time-resolved temperature measurements during microsecond pulsed-laser irradiation of a metal plate made of the titanium alloy Ti -6 Al -4 V provide temperature information about the irradiated surface with an estimated accuracy of ± 10 % . The extracted wavelength-dependent emissivity slope compares well with reported results for macroscale titanium melts obtained using IR spectroscopy, which measure temperature without any built-in assumptions about the emissivity. The results are directly applicable to temperature monitoring during welding, additive manufacturing, and semiconductor growth.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Complex dislocation loop networks as natural extensions of the sink efficiency of saturated grain boundaries in irradiated metals

The development of radiation-tolerant structural materials is an essential element for the success of advanced nuclear energy concepts. A proven strategy to increase radiation resistance is to create microstructures with a high density of internal defect sinks, such as grain boundaries (GBs). However, as GBs absorb defects, they undergo internal transformations that limit their ability to capture defects indefinitely. Here, we show that, as the sink efficiency of GBs becomes exhausted with increasing irradiation dose, networks of irradiation loops form in the vicinity of saturated or near-saturated GB, maintaining and even increasing their capacity to continue absorbing defects. The formation of these networks fundamentally changes the driving force for defect absorption at GB, from “chemical” to “elastic.” Using thermally-activated dislocation dynamics simulations, we show that these networks are consistent with experimental measurements of defect densities near GB. Our results point to these networks as a natural continuation of the GB once they exhaust their internal defect absorption capacity.

36 MATERIALS SCIENCE↗

An efficient instance segmentation approach for studying fission gas bubbles in irradiated metallic nuclear fuel

Abstract Gaseous fission products from nuclear fission reactions tend to form fission gas bubbles of various shapes and sizes inside nuclear fuel. The behavior of fission gas bubbles dictates nuclear fuel performances, such as fission gas release, grain growth, swelling, and fuel cladding mechanical interaction. Although mechanical understanding of the overall evolution behavior of fission gas bubbles is well known, lacking the quantitative data and high-level correlation between burnup/temperature and microstructure evolution blocks the development of predictive models and reduces the possibility of accelerating the qualification for new fuel forms. Historical characterization of fission gas bubbles in irradiated nuclear fuel relied on a simple threshold method working on low-resolution optical microscopy images. Advanced characterization of fission gas bubbles using scanning electron microscopic images reveals unprecedented details and extensive morphological data, which strains the effectiveness of conventional methods. This paper proposes a hybrid framework, based on digital image processing and deep learning models, to efficiently detect and classify fission gas bubbles from scanning electron microscopic images. The developed bubble annotation tool used a multitask deep learning network that integrates U-Net and ResNet to accomplish instance-level bubble segmentation. With limited annotated data, the model achieves a recall ratio of more than 90%, a leap forward compared to the threshold method. The model has the capability to identify fission gas bubbles with and without lanthanides to better understand the movement of lanthanide fission products and fuel cladding chemical interaction. Lastly, the deep learning model is versatile and applicable to the micro-structure segmentation of similar materials.

36 MATERIALS SCIENCE↗

Precision Local Burnup Assessment Through Dynamic Peak Fitting in Atom Probe Tomography for Depleted, Enriched, and Irradiated Metallic and Ceramic Fuels

Abstract Burnup estimation in nuclear fuels is vital for evaluating fuel performance, transportation, and safe fuel storage. Accurate assessments of burnup from service period and spent fuels involve tracking the consumption of fissile isotopes of uranium (U) offering a direct insight into energy changes within the fuels especially for thermal spectrum reactors. In current approach, mass spectroscopic technique in atom probe tomography (APT) is utilized for accurate quantification of U isotopes. Quantification of U peaks in mass spectrum is performed on asymmetric shapes due to delayed signals, known as thermal tails, particularly for poorly conducting samples analyzed in laser mode. In this study, we introduce a novel quantification tool for isotopic analysis from APT datasets by developing a fitting algorithm based on shapes of the peaks. A MATLAB-based dynamic peak fitting toolbox is developed and designed to adapt to various peak shapes, ensuring accurate quantification of U isotopes. The effectiveness of this approach is demonstrated in standard Ni-Cr sample, depleted and enriched U samples, and U-based fuels with different burnup levels. The viability of this approach for isotopic quantification is demonstrated on both metallic and ceramic fuels.

Burnup↗

Chapter 21. Atomic-Level Dislocation Dynamics in Irradiated Metals

Primary damage and microstructure evolution in structural nuclear materials operating under conditions of a high flux of energetic atomic particles and high temperature and stress lead to the formation of a high concentration, non-homogeneous distribution of defect clusters in the form of dislocation loops, voids, gas-filled bubbles and radiation-induced precipitates of nanometer scale. They cause changes in many material properties. Being obstacles to dislocation glide, they strongly affect the mechanical properties, with an increase in yield and flow stresses and a reduction in ductility. Atomic-scale computer simulations can provide details of how these effects are influenced by the obstacle structure, applied stress, strain rate and temperature. Processes such as obstacle cutting, transformation, absorption and drag are observed. Some recent results for body-centered and face-centered cubic metals are described in this review and, where appropriate, comparisons are drawn with predictions based on the elasticity theory of crystal defects. Perspectives on how to use this information at higher scales and in particular in mesoscale, dislocation dynamics simulations are also discussed.

Osetskiy, Yury N.↗

FIPD: The SFR metallic fuels irradiation & physics database

The DOE Advanced Reactor Technology (ART) program has supported efforts to recover and preserve metallic fuel data generated throughout the US sodium-cooled fast reactor (SFR) program. Those efforts have been focused on establishing databases of the experimental data that were mainly generated during the Integral Fast Reactor (IFR) program including data generated at Experimental Breeder Reactor-II (EBR-II), Fast Flux Test Facility (FFTF), and Transient Reactor Test Facility (TREAT) reactors, as well as out of pile data. The data is essential for future licensing activities of metallic fuel based advanced fast reactors. This paper describes the development of the SFR Metallic Fuels Irradiation & Physics Database (FIPD) and covers the scientific knowledge available in the database. Furthermore, the architecture of the FIPD is described by showing the available reactor operation data, fabrication, and post-irradiation examination (PIE) data, and other documents. The applications of the fuel database are also discussed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Production of zirconium-88 via proton irradiation of metallic yttrium and preparation of target for neutron transmission measurements at DICER

Abstract A process for the production of tens to hundreds of GBq amounts of zirconium-88 ( 88 Zr) using proton beams on yttrium was developed. For this purpose, yttrium metal targets (≈20 g) were irradiated in a ~16 to 34 MeV proton beam at a beam current of 100–200 µA at the Los Alamos Isotope Production Facility (IPF). The 88 Zr radionuclide was produced and separated from the yttrium targets using hydroxamate resin with an elution yield of 94(5)% (1σ). Liquid DCl solution in D 2 O was selected as a suitable 88 Zr sample matrix due to the high neutron transmission of deuterium compared to hydrogen and an even distribution of 88 Zr in the sample matrix. The separated 88 Zr was dissolved in DCl and 8 µL of the obtained solution was transferred to a tungsten sample can with a 1.2 mm diameter hole using a syringe and automated filling station inside a hot cell. Neutron transmission of the obtained 88 Zr sample was measured at the Device for Indirect Capture Experiments on Radionuclides (DICER).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The Recovery of Medical Isotope 188 W from Irradiated W Metal Target - A New Approach

Tungsten-188 is in widespread use in 188 W(t 1/2 = 69 d )/ 188 Re(t 1/2 = 16.9 h ) biomedical generators. Oak Ridge National Laboratory 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 188 W product. While 188 W is produced by neutron bombardment, 191 Os(t 1/2 = 15.4 d ) is simultaneously produced as a by-product and expected to be separated from 188 W by postirradiation treatment.In the current processing pathway, the irradiated W metal 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 preparation of 188 W product. This oxidation process also converts 188 Os (the decay daughter of 188 W) and 191 Os (15.4 d , 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 goals of (1) converting metal target to a soluble oxide form and (2) removing volatile OsO 4 away from the solid WO 3 product by air flow and absorbing the harmful Os species by the scrubbing array. But this method has two potential problems as well: (1) O 2 reacts with only W metal at high temperatures, not with W alloyed with other elements. The O 2 –W reaction will be retarded when formation of WRe or WC occurs, or even when a layer of non-W materials on the surface of the irradiated W rings.; (2) 100% absorption of OsO 4 of high yield (>90%) from the reaction of Os + O 2 is a strict requirement to the OsO 4 scrubbing system--so NaOH scrubbers of a redundant size (2x 1.5 L) are in use for safety reasons.To resolve above two potential problems, direct dissolution of the irradiated W metal target by a selected reagent is a preferred pathway to avoid heating step with generation of tremendous amount of volatile OsO 4 . Hydrogen peroxide (H 2 O 2 ) is such a candidate to dissolve W in forms of either metal or alloys, although literature lacks information of solubilities of Re or Os in H 2 O 2 . With experimental results of dissolving non-radioactive W, Re and Os in H 2 O 2 under various conditions, this report illustrates a method of H 2 O 2 dissolution for irradiated W target, with a complete dissolution of W and Re, but ≤10% dissolution of Os (converted into gaseous OsO 4 and carried out into a scrubbing for absorption) during processing irradiated W target. The portion of undissolved Os can be separated from W solution by a follow up filtration step. Solubilities of W, Re and Os in H 2 O 2 at a temperature range from 14° to 50°C are presented. And a dissolution rate of W metal per surface area of W metal in H 2 O 2 is calculated based on results of dissolving a W metal cylinder of known surface area in H 2 O 2 at room temperature without stirring.

07 ISOTOPE AND RADIATION SOURCES↗

High resolution microstructural, chemical studies and localized burnup analysis in an irradiated U–10Zr metallic fuel

This study involves high resolution characterization of a sodium bonded solid uranium (U)-10 wt% zirconium (Zr) metallic fuel irradiated in Fast Flux Test Facility (FFTF). The fuel centerline temperature during irradiation was estimated to be around 675 °C with the peak burnup 13.1 atomic percent. Samples for transmission electron microscopy (TEM) and atom probe tomography (APT) were prepared from different regions/zones in the fuel cross section radially to elucidate the microstructural changes and chemical redistribution of solute elements as well as fission products during irradiation experiment. TEM results indicate the irradiation in fast flux testing leads to the formation of extensive Zr-rich precipitates with varying sizes in the U–Zr fuel matrix. APT analysis performed to investigate redistribution of Zr, U and fission products along the radial direction of fuel pin showed Zr-rich precipitates entrapping the fission products in higher concentration as compared to the α-U phases. Here, the local burnup ( 235 U depletion) is found to be consistent, calculated by quantification of 235 U, 236 U and 238 U isotopes from mass spectrum obtained from APT along the radial direction. Zr-rich precipitation and its implication on fuel constitutional redistribution are discussed based on SEM, TEM and APT results.

APT↗

Development and formulation of physics based metallic fuel models and comparison to integral irradiation data

Metallic fuel has an important historical significance in the development of nuclear reactors and continues to be relevant to the progression of advanced test and power reactors. A number of models, ranging from empirical to mechanistic, have been developed and implemented in various fuel performance codes to describe U-Zr and U-Pu-Zr fuel and typical fast reactor cladding materials. One challenge of using these models to simulate fuel performance is the inevitable tangling of coupled phenomena that can cloud proper implementation, calibration, and eventual utilization of new models. Here in an effort to provide a baseline capability that will facilitate the use of advanced models, new capabilities have been implemented into the fuel performance code BISON specific to metallic fuel simulations, ranging from materials properties, fission gas release and swelling calculations, coolant channel models, and cladding correlations. These models have been applied to the X441/X441A EBR-II experimental assembly data, a set of irradiated metallic UPuZr fuel rods of varying pin designs. The models implemented in BISON are able to capture the general trend of the expected response of the fuel and cladding to irradiation in EBR-II, especially when considering the spread in experimental measurements and the uncertainties inherited from the historical material models. Ultimately, the models outlined here provide the baseline capabilities on which new models can build upon in order to improve the prediction of metallic fuel performance simulations in off-normal designs or operations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗