Study on the dissolution of ß-precipitates in the Zr-1Nb alloy under the influence of Ne ion irradiation.

The stability of ß-precipitates in the Zr-1Nb alloy has been studied under Ne ion irradiation of energy 250 keV by insitu transmission electron microscope as a function of irradiation dose. The irradiation was carried out up to ∼136 dpa at 573 K. Microstructural investigations have shown that up to ∼38 dpa, precipitates showed an increase in size, and for irradiation doses >38 dpa, the size of the precipitates was noticed to reduce. Post-irradiation energy-dispersive spectrometry of the specimens revealed the Nb concentration throughout the matrix to be ∼0.8-1.5%. Three-dimensional atom probe tomography was also carried out for irradiated specimens to look for the presence of any nanoclusters. However, Nb clustering was not observed in the specimens. It is proposed that the dissolution of the precipitates may be facilitated by an increase in the solubility limit of Nb in Zr caused by irradiation. The solubility limit may increase by the introduction of defects generated by irradiation and by the destabilization of the ß-phase. This may result in back-diffusion of Nb atoms to the matrix by radiation-enhanced diffusion to lower the strain produced by the defects, resulting in the dissolution of the precipitates.

Understanding amorphization mechanisms using ion irradiation in situ a TEM and 3D damage reconstruction.

In this work, ion irradiations in-situ of a transmission electron microscope are performed on single-crystal germanium specimens with either xenon, krypton, argon, neon or helium. Using analysis of selected area diffraction patterns and a custom implementation of the Stopping and Range of Ions in Matter (SRIM) within MATLAB (which allows both the 3D reconstruction of the collision cascades and the calculation of the density of vacancies) the mechanisms behind amorphization are revealed. An intriguing finding regarding the threshold displacements per atom (dpa) required for amorphization results from this study: even though the heavier ions generate more displacements than lighter ions, it is observed that the threshold dpa for amorphization is lower for the krypton-irradiated specimens than for the xenon-irradiated ones. The 3D reconstructions of the collision cascades show that this counter-intuitive observation is the consequence of a heterogeneous amorphization mechanism. Furthermore, it is also shown that such a heterogeneous process occurs even for helium ions, which, on average induce only three recoils per ion in the specimen. It is revealed that at relatively high dpa, the stochastic nature of the collision cascade ensures complete amorphization via the accumulation of large clusters of defects and even amorphous zones generated by single-helium-ion strikes.

Effect of density and Z-contrast on the visibility of noble gas precipitates and voids with insights from Monte-Carlo simulations.

In this work, a detailed analysis of He, Ne, Ar, Kr and Xe precipitates in a complex borosilicate glass using transmission electron microscopy (TEM) with in-situ ion implantation is presented. With in-situ monitoring, the real-time dynamics of precipitate and void evolution under ion implantation was followed. Using appropriate equations of state and, Monte-Carlo simulations to supplement the TEM images, we then discuss in detail the possibility and ways of differentiating the precipitates of various noble gases from empty voids. It is shown that all the noble gases precipitate as inclusions of supercritical fluid. With the aid of the simulations, the crucial role played by the size and density of the precipitates and atomic number of the gas atoms in affecting the visibility of the precipitates is highlighted. The results show that the precipitates and voids can be unambiguously differentiated in the case of Xe and Kr whereas the precipitates of other lighter noble gases cannot be differentiated from the voids. However, the precipitate and void evolution under ion irradiation follow different dynamics, knowledge of which allows one to differentiate between the precipitates and voids even for lighter noble gases. Besides shedding light on the subject of noble gas precipitation and identification of the precipitates and voids, the study highlights the complexity in dissociating the behaviour of voids from the process of precipitate re-solution. This type of knowledge is pivotal in developing models describing the evolution of precipitates, voids and macroscopic porosity in a number of materials.

Xenon solubility and formation of supercritical xenon precipitates in glasses under non-equilibrium conditions.

Estimates of noble gas solubility in glasses and minerals are important to understand the origin of these gases, particularly xenon, in the atmosphere. However, technical difficulties and ambiguities in quantifying the dissolved gases introduce large uncertainties in the solubility estimates. We present here the use of transmission electron microscopy (TEM) with in-situ noble gas ion implantation as a non-equilibrium approach for noble gas solubility estimates. Using a suitable Xe equation of state and Monte-Carlo simulations of TEM images, a clear distinction between Xe filled precipitates and empty voids is made. Furthermore, implantation-induced changes in the solubility are estimated using molecular dynamics simulations. These studies allow us to evaluate the xenon solubility of irradiated and pristine silica glasses and monitor in-situ the diffusion-mediated dynamics between the precipitates and voids - otherwise impossible to capture. On exceeding the solubility limit, supercritical xenon precipitates, stable at least up to 1155 K, are formed. The results highlight the high capacity of silicates to store xenon and, predict higher solubility of radiogenic xenon due to the accompanying radiation damage.

Understanding and simulating the material behavior during multi-particle irradiations.

A number of studies have suggested that the irradiation behavior and damage processes occurring during sequential and simultaneous particle irradiations can significantly differ. Currently, there is no definite answer as to why and when such differences are seen. Additionally, the conventional multi-particle irradiation facilities cannot correctly reproduce the complex irradiation scenarios experienced in a number of environments like space and nuclear reactors. Therefore, a better understanding of multi-particle irradiation problems and possible alternatives are needed. This study shows ionization induced thermal spike and defect recovery during sequential and simultaneous ion irradiation of amorphous silica. The simultaneous irradiation scenario is shown to be equivalent to multiple small sequential irradiation scenarios containing latent damage formation and recovery mechanisms. The results highlight the absence of any new damage mechanism and time-space correlation between various damage events during simultaneous irradiation of amorphous silica. This offers a new and convenient way to simulate and understand complex multi-particle irradiation problems.

Self-healing capacity of nuclear glass observed by NMR spectroscopy.

Safe management of high level nuclear waste is a worldwide significant issue for which vitrification has been selected by many countries. There exists a crucial need for improving our understanding of the ageing of the glass under irradiation. While external irradiation by ions provides a rapid simulation of damage induced by alpha decays, short lived actinide doping is more representative of the reality. Here, we report radiological NMR experiments to compare the damage in International Simplified Glass (ISG) when irradiated by these two methods. In the 0.1 mole percent (244)Cm doped glass, accumulation of high alpha decay only shows small modifications of the local structure, in sharp contrast to heavy ion irradiation. These results reveal the ability of the alpha particle to partially repair the damage generated by the heavy recoil nuclei highlighting the radiation resistance of nuclear glass and the difficulty to accurately simulate its behaviour by single ion beam irradiations.