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DOE OSTI2023

Development of Mechanistic Fission Gas Release and Swelling Models for UN Fuels in BISON

This report describes the work in NEAMS (Nuclear Energy Advanced Modeling and Simulation) to develop a mechanistic fission gas model for uranium nitride fuels in BISON. The existing Sifgrs (Simple integrated fission gas release and swelling) model tracks the average properties of two bubble populations in the bulk and at the grain boundaries. It was recognized that dislocations play a crucial role in the fission gas swelling of UN, and an irradiation-induced dislocation density model was needed, as well as a model describing how fission gas interacts with dislocations creating a third population of bubbles along dislocations. A mechanistic model that tracks dislocation bubbles was implemented in Sifgrs. This model was used to simulate fission gas swelling and release in UN. Lower-length-scale calculations and experimental observations from carbide fuel were leveraged to help populate the model with essential parameters. As a placeholder, an empirical function was formulated for the evolution of the dislocation network. Because of the difference in evolution of this network at different temperatures, the dislocation bubbles are able to capture behavior that the bulk intragranular bubbles cannot. It was found that the bulk bubbles dominate microscopic swelling at low temperatures, and the dislocation bubbles dominate at higher temperatures. Based on this model, the transition between the two bubble types is the main factor behind the breakaway swelling phenomenon in UN. In order to test the model, a couple of assessments were run. For the lower temperature JOYO pins, the model produces reasonable fission gas release and swelling values. For the higher temperature SP1 pin, the model dramatically underestimates the fission gas release. This issue is attributed to the gas being trapped inside dislocation bubbles, unable to escape to grain boundaries to cause fission gas release, and could be remedied by a mechanistic dislocation model that allows the dislocation density to decrease at very high temperatures. A preliminary mechanistic dislocation model was developed supported by first-principle calculations. These calculations provided valuable insight into how interstitial defects cluster in UN in the {110} orientation, and may eventually form dislocation loops, leading to the conclusion that dislocation loops may nucleate from these clusters. An estimate of the dislocation line energy in UN was obtained and will be improved in future work. The free-energy cluster dynamics code Centipede was used to track interstitial and vacancy absorption at dislocation loops and calculate their growth. In addition, improvements to Centipede were made including new convergence criteria for transient simulations and sink driving force updates.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Atomic-scale mechanisms of void strengthening in tungsten

Neutron and heavy-ion irradiation of tungsten produces nanometer-size vacancy voids, gas-filled bubbles and dislocation loops. These defect features can affect mechanical properties and the impact can be quite significant because of their high density. Understanding the basic mechanisms of mechanical properties degradation is necessary for predicting radiation effects. Predictions can be made using discrete dislocation dynamics or/and finite element approaches which, however, need local interaction mechanisms as inputs. Such knowledge can be provided only by atomic-scale modeling. This paper reports the results of an extensive atomic-scale modeling study of the interactions between moving edge dislocations and voids in tungsten. Furthermore, the main focus is on the effects of the void size and ambient temperature. Critical resolved shear stress was calculated for voids up to 9 nm in diameter. Atomistic results are compared with the theoretical approach and with those obtained earlier for voids in body centered cubic (bcc) iron. An important role of the void surface has been revealed.

36 MATERIALS SCIENCE↗

NASA NTRS2012

Electron Beam Induced Luminescence of SiO2 Optical Coatings

Optical coatings of disordered thin film SiO,/SiO, samples undergoing electron beam bombardment exhibited a cathodoluminescence effect. Measurements were made of the absolute illuminance and emission spectra as functions of incident electron energy (0.2 keV to 30 keV). flux (approx. 0.1 nA/sq cm to > 100 nA/sq cm) and power (<50 nW/sq cm to > 3mW/sq cm) for coatings (approx.60 nm to approx.200 nm thick) on reflective metal substrates over a range of sample temperatures (approx.40 K to approx.400 K) and emission wavelengths (approx.260 nm to approx.5000 nm). Illuminance reached a plateau saturation intensity I(sub sat) approx. 10(exp -4)W/sq cm. scaling as [I(sub mc)/(I + I(sub mc)/I(sub sat)] as incident power I(sub mc) approached I(sub sat). Well below I(sub sat), illuminance scaled linearly with incident power for lower-energy non-penetrating radiation that deposited all of its energy in the dielectric film. At higher incident energies (> 1-5 keV) electrons penetrate the dielectric, depositing only a fraction of their energy in the dielectric film, where deposited energy scales as the ratio of film thickness to penetration range. Since electron range exhibits a peak below approx. 1 keV, the illuminance decreased with increasing energy for penetrating radiation. The temperature dependence of the illuminance. in general, increased with decreasing temperature. Changes in apparent color with temperature were also observed. Four bands in the UV/VIS/NIR range from 300 nm to 1000 nm were observed in spectral measurements; no significant luminescence was detected in a range from approx. 1000 nm to approx. 5000 nm. These different bands either increased or decreased in intensity and shifted slightly in energy with decreasing temperature. Our measurements are explained in terms of simple disordered band theory models based on atomic-scale stochastic transport of electrons in highly disordered insulating materials. The theoretical models provide a fundamental basis for understanding the dependence of cathodoluminescence on irradiation time, incident flux and energy. and sample thickness and temperature. The observed luminescence occurs when an incident high energy electron excites a valence band electron into the conduction band. Following the excitation. a complex series of transitions take place between the extended conduction states and the long-lived localized trapped states (or chromophores) associated with structural or compositional defects in the dielectric materials. Thc transport equations and models of thc spatial and energy distribution of the trapped states below the mobility edge, their occupancy, and transitions provide microscopic scale insights into this macroscopic phenomenon. Our observations and theoretical models are also compared with similar previous room temperature studies of similar SiO2 films.

Dennison, J. R.↗

NASA NTRS2005

Protective effect of apigenin on radiation-induced chromosomal damage in human lymphocytes

The potential use of flavonoids as a radioprotector is of increasing interest because of their high antioxidant activity and abundance in the diet. The aim of this study is to examine genotoxic and radioprotective effects of one of the most common flavonoids, apigenin, on radiation-induced chromosome aberrations in human lymphocytes. The cytokinesis-block micronucleus (CBMN) assay was used to evaluate such effects of apigenin. Blood samples were collected from two non-smoking healthy male volunteers who had no history of previous exposure to other clastogenic agents. Isolated lymphocytes were cultured. There were two tubes per concentration for all treatments. To evaluate the genotoxicity of apigenin, cells were first treated with different concentrations of apigenin (0, 2.5, 5, 10 and 25 microg/mL) at 24 h after culture initiation, followed by cytochalasin-B (Cyt-B) treatment (3 microg/mL) and cell harvest at 44 and 72 h, respectively. Secondly, to investigate the radioprotective effect, cell cultures were exposed to different concentrations of apigenin as described above for 30 min before being irradiated to 2 Gy of 137Cs gamma rays (at a dose rate of 0.75 Gy/min). In all instances, the frequency of MN was scored in binucleated (BN) cells. The nuclear proliferation index also was calculated. We did not detect an increase in the frequency of MN in non-irradiated human lymphocyte cultures treated with 2.5, 5.0 or 10 microg/mL apigenin; although, we did observe an increase in cultures treated with 25 microg/mL apigenin (the highest concentration of apigenin used in our study). We also observed a significant increase in the frequency of MN in irradiated cells overall; however, the frequency was decreased as the concentration of apigenin increased, suggesting a radioprotective effect. These findings provide a basis for additional studies to help clarify the potential use and benefit of apigenin as a radioprotector.

NASA Discipline Radiation Health↗

DOE OSTI2025

Integral X-ray diffuse scattering for studying irradiation-induced dislocation loops in single crystals

Numerical diffuse scattering cross-section calculations are used to establish a rigorous basis for determining the concentration and size distribution of dislocation loops in irradiated single crystals from integral X-ray diffuse scattering (XRDS) measurements. Differential XRDS intensities for prismatic {111} type dislocation loops are numerically calculated as a function of loop radius R and wavevectors q relative to Bragg reflections in tungsten. The results show the well known 1/q 2 Huang scattering form at small q that transitions to a ∼1/q 4 dependence associated with the Stokes–Wilson approximation for q ≳ 1/R. More importantly, they show further that the 1/q 4 falloff is not the asymptotic large-q form of the diffuse scattering for small loops (R < 200 Å) as has often been assumed. Rather, for loop sizes as small as R ≃ 5 Å with strong curvature, the calculations show definitively that the scattering transitions to a robust 1/q 5 falloff at larger q that arises due to the local strains near the dislocation core defining the circumference of the dislocation loops. The presence of this 1/q 5 asymptotic form for both small and large loops is experimentally confirmed using an integral XRDS measurement around the 110 reflection on self-ion-irradiated tungsten combined with numerically calculated integral XRDS cross-sections. Accordingly, the historical two-region theoretical treatment of the cross-sections for integral XRDS is extended to a three-region model that has direct sensitivity to the (first-moment) dislocation line lengths of dislocation loops. In conclusion, these developments enable the use of both numerical and analytically modeled cross-sections to make accurate integral XRDS determinations of dislocation loop sizes and concentrations using modest-intensity laboratory X-ray sources.

42 ENGINEERING↗