Changes in transverse phonon sound velocity were measured during low temperature irradiation of amorphous Pd80Si20 with 3.5 MeV krypton ions. The sound velocity decreases as a function of the ion fluence and shows a tendency to saturate at large fluences at a relative change of -4.7%. The changes in sound velocity were used to determine the changes in shear elastic constant and in Debye temperature both of which were in reasonable agreement with the value reported in the literature.

The effect of Al ion irradiation on the mobility of Xe gas bubbles in Al thin films was investigated. Transmission electron microscopy was used to determine bubble diffusivities in films irradiated and/or annealed at 673,723 and 773 K. Irradiation increased bubble diffusivity by a factor of 2–9 over that due to thermal annealing alone. The Arrhenius behavior and dose rate dependence of bubble diffusivity are consistent with a radiation enhanced diffusion phenomenon affecting a volume diffusion mechanism of bubble transport.

ABSTRACTChanges induced by 1.5 MeV Kr ion irradiation of both U3Si and U3Si2 have been followed by in situ transmission electron microcopy. When irradiated at sufficiently low temperatures, both alloys transform from the crystalline to the amorphous state. When irradiated at temperatures above the temperature limit for ion-beam amorphization, both compounds disorder, with the Martensite twin structure in U3Si disappearing from view in TEM. Prolonged irradiation of the disordered crystalline phases results in nucleation of small crystallites within the initially large crystal grains. The new crystallites increase in number during continued irradiation until a fine grain structure is formed. Electron diffraction yields a powder-like diffraction pattern that indicates a random alignment of the small crystallites. During a second irradiation at lower temperatures, the small crystallizes retard amorphization. After 2 dpa at high temperatures, the amorphization dose is increased by over twenty times compared to that of initially unirradiated material.

We demonstrate the emission of nanometre-sized defect clusters from an isolated displacement cascade formed by irradiation of high-energy self-ions and their subsequent 1-D motion in Au at 50 K, using in situ electron microscopy. The small defect clusters emitted from a displacement cascade exhibited correlated back-and-forth 1-D motion along the [−1 1 0] direction and coalescence which results in their growth and reduction of their mobility. From the analysis of the random 1-D motion, the diffusivity of the small cluster was evaluated. Correlated 1-D motion and coalescence of clusters were understood via elastic interaction between small clusters. These results provide direct experimental evidence of the migration of small defect clusters and defect cascade evolution at low temperature.

Advantages and disadvantages of bulk nanocrystalline (nc)-oxides (UO2, ZrO2, ThO2) and suggestions for their potential use as nuclear fuels and inert matrix carriers are described in this work on the basis of a study with nc-4mol% Y2O3–ZrO2 bodies, which are envisaged to behave akin to highly exposed LWR-fuels with the High Burn-up Structure (HBS) also known as rim transformation. The main attributes of nc-fuels in-pile compared to conventional fuels will be the capacity to develop closed porosity retaining most of the fission gases, the ability to relax more efficiently the interaction stresses with the cladding (through much higher plasticity) and the enhanced resistance against radiation-damage thanks to their nanostructure. The present analysis comprises the long-term thermal stability of a porous nc-material, its property vs. porosity relations, the topology of the pore phase via X-ray synchrotron tomography, the behaviour under compressive stress and the performance under intense Xe-ions irradiation. Salient outcomes are the non-connectivity of the pore phase, the superplasticity of the nc-bodies and their high radiation–amorphisation resistance with negligible swelling under Xe-bombardment. Another important outcome of the present study is that deterioration of the thermal properties due to grain boundary effects (Kapitza resistance, melting point depression) can likely be avoided if the grain size is kept above 100nm and, emulating the real HBS material, preferably in the range between 200 and 300nm.

Xenon and krypton have been implanted into muscovite mica at room temperature and at liquid nitrogen temperature. The behavior of the implanted Xe and Kr was followed by low-temperature transmission electron microscopy and energy dispersive x-ray analysis. An electron diffraction pattern of diffuse bands is observed at room temperature due to the presence of fluid rare gas and to noncrystalline mica. Visible cavities with diameters 10–300 nm formed in the Xe-implanted mica. Visible cavities in room-temperature Kr-implanted mica ranged from 5–50 nm in diameter. The gas pressures at room temperature in the cavities are estimated, assuming all of the implanted gas precipitated in cavities to be ∼10 MPa for Xe and ∼20 MPa for Kr. These pressures are considerably lower than found for rare gases implanted in metals and ceramics, but sufficient to liquefy the rare gases at room temperature. The Xe and Kr were observed by dark-field microscopy to form fcc crystalline solids within the cavities at temperatures below their triple points, with lattice parameters of a (xe) = 0.630 ± 0.0015 nm and a (Kr) = 0.565 ± 0.005 nm. The solid Xe within bubbles was unstable under the electron beam of the transmission electron microscope at temperatures above 80 K, while the solid Kr within bubbles was unstable at temperatures as low as 35 K. The crystalline mica matrix undergoes a transformation from a crystalline structure to an amorphous structure as a result of implantation.

Twenty-five silicates were irradiated at ambient temperature conditions with 1.5 MeV Kr+. Critical doses of amorphization were monitored in situ with transmission electron microscopy. The doses required for amorphization are compared with the structures, bond-types, compositions, and physical properties of the silicates using simple correlation methods and more complex multivariate statistical analysis. These analyses were made in order to determine which properties most affect the critical amorphization dose. Simple two-variable correlations indicate that melting point, efficiency of atomic packing, the dimensionality of SiO4 polymerization (DOSP), and bond ionicity have a relationship with critical amorphization dose. However, these relationships are evident only in selected portions of the data set; that is, for silicate phases with a common structure type. A clearer relationship between the silicate properties and critical amorphization dose was determined for the entire data set with multiple linear regression. Several regression models are proposed which describe the variation in amorphization dose. All regression models contain the following properties: (i) melting point; (ii) a structural variable (DOSP, elastic modulus, and/or atomic packing); and (iii) the proportion of Si–O bonding (instead of bond ionicity). The regression models are equivalent, because they represent combinations of similar properties. Notably, density and atomic mass are not controlling properties for the critical amorphization dose. Melting and amorphization by ion irradiation are apparently related processes. Neither melting point nor critical amorphization dose can be predicted by considering only the structure, composition, or bonding of a particular phase. The Si–O bond is the most covalent bond in silicates, and is the “weak link” in the structure with respect to amorphization. Thus, DOSP is also an important property, as the topology of these ”weak links” influences a structure’s ability to accumulate amorphous regions. The efficiency of atomic packing is related to the process of defect self-recombination during amorphization. The bulk modulus and shear modulus are important variables within the regression models because of their direct relationship to atomic packing.

In this study, we simulated gas bubble formation in glasses by in-situ ion implantation. Alkali silicate glass and Na-borosilicate glass were implanted in situ with 50 keV Xe ions at temperatures at 200°C in a Hitachi-9000 electron microscope. Bubble formation was studied by transmission electron microscopy images taken during interruptions of the ion beam after discrete implanted-ion dose steps. We present a possible mechanism of bubble formation and growth based on amorphous network structures.

We compare damage evolution in U3Si produced by neutron irradiation at 30°C and 350°C and measured by neutron diffraction. Initial studies found that increasing neutron irradiation dose at 30°C results in monotonic expansion of the a-axis and contraction of the c-axis that transforms the crystal structure from tetragonal to cubic [1]. Additional irradiation results in amorphization. Neutron irradiation at 350°C results in little change to the a-axis and expansion of the caxis.The complete alteration in lattice dilatation during irradiation is interpreted as due to modification of surviving defect configurations at the higher temperature. The high temperature lattice dilations can be explained by defect loop formation in the a-b plane. Confinement of lattice strain to the c-axis during irradiation at 350°C may be the mechanism that prevents the total lattice dilatation from exceeding the critical level required for amorphization.

Single ion impacts have been observed using in-situ transmission electron microscopy during irradiation. In addition to internal defects, single-ion impacts create surface craters as large as 12 nm on In, Ag, Pb and Au. Crater formation rates have been determined from video recordings with a time-resolution of 33 milliseconds. The cratering rate for Xe ions increases linearly with increasing target mass density above a threshold density of approximately 7 g/cm3. The cratering rate increases as the ion mass is increased. These results suggest that cratering requires a high energy-density, near-surface displacement cascade. TRIM calculations have been made in an effort to establish a near-surface energydensity criterion for cratering.

The microstructure of a muscovite mica exposed to a rare gas ion beam has been studied by transmission electron microscopy. The investigation of damage without implantation was carried out using argon and helium ions of sufficient energy to traverse the 100–150 nm mica specimens. For 340 keV Ar++ irradiation, amorphization of mica occurred at a fluence as low as 3.5 × 1014 ions · cm−2, which corresponds to 0.29 dpa. Muscovite can be amorphized using 80 keV helium ions, but this requires a much higher fluence and damage production of 4.6 × 10−6 ions · cm−2 and 0.60 dpa, respectively. Since helium irradiation results principally in ionization energy loss, it indicates that amorphization of muscovite results mainly from nuclear interactions. Complete amorphization of muscovite mica is found to take place for all ions at approximately the same amount of nuclear energy transfer to energetic primary knock-on atoms, assuming a recoil energy greater than 500 eV. This suggests that amorphization occurs directly in dense displacement cascades. A significant amount of helium, 100 ppm, can be implanted into muscovite mica without destroying the crystal structure.

Vapor-deposited Zr-Fe multilayered thin films with various wavelengths and of overall composition either 50% Fe or Fe-rich up to 57 % Fe were either irradiated with 300 keV Kr ions at temperatures from 25K to 623 K to fluences up to 2 × 1016 cm−2, or simply annealed at 773Kin-situ in the Intermediate Voltage Electron Microscope at Argonne National Laboratory. Under irradiation, the final reaction product is the amorphous phase in all cases studied, but the dose to amorphization depends on the temperature and on the wavelength. In the purely thermal case (annealing at 773 K), the 50-50 composition produces the amorphous phase but for the Fe-rich multilayers the reaction products depend on the multilayer wavelength. For small wavelength, the amorphous phase is still formed, but at large wavelength the Zr-Fe crystalline intermetallic compounds appear. These results are discussed in terms of existing models of irradiation kinetics and phase selection during solid state reaction.

The formation of amorphous silicon in crystalline silicon by bombardment with light (Si) and heavy (Xe) ions has been investigated by transmission electron microscopy with in situ ion irradiation. Experiments have been carried out at room temperature and low temperature (50K) and the results are compared to a simple numerical model for amorphization. The results indicate that the amorphization mechanisms for both irradiations are heterogeneous in nature and that numerous overlaps of the collision cascade are generally required to render the crystal amorphous. Following from this, the nature of the material within the confines of collision cascades will be discussed and it will be shown that the individual cascade volume is not necessarily amorphous as previously described in the scientific literature but contains varying degrees of damage depending on the energy deposited within the cascade.

Dynamic interaction of helium bubble with cascade damage in Fe–9Cr ferritic alloy has been studied using in situ irradiation and electron microscopy. During the irradiation of the alloy by 400keV Fe+ ions at temperatures where no thermal motion takes place, induced displacement of small helium bubbles was observed: the bubbles underwent sporadic and instant displacement. The displacement was of the order of a few nanometers. The experimentally determined displacement probability of helium bubbles is consistent with the calculated probability of their dynamic interaction with sub-cascades introduced by the irradiation. Furthermore, during the irradiation of the alloy at higher temperatures, both retarded and accelerated Brownian type motions were observed. These results are discussed on the basis of dynamic interaction of helium bubbles with point defects that survive through high-energy self-ion irradiation.

Brownian-type motion of helium bubbles in aluminum and its dynamical response to irradiation with 100-keV Al+ ions at high temperatures has been studied using in situ irradiation and transmission electron microscopy. It is found that, for most bubbles, the Brownian-type motion is retarded under irradiation, while the mobility returns when the irradiation is stopped. In contrast, under irradiation, a small number of bubbles display exceptionally rapid motion associated with the change in bubble size. These effects are discussed in terms of the dynamical interaction of helium bubbles with cascade damage formed by the high-energy self-ion irradiation.

The intermediate voltage electron microscope‐tandem user facility in the Electron Microscopy Center at Argonne National Laboratory is described. The primary purpose of this facility is electron microscopy with in situ ion irradiation at controlled sample temperatures. To illustrate its capabilities and advantages a few results of two outside user projects are presented. The motion of dislocation loops formed during ion irradiation is illustrated in video data that reveals a striking reduction of motion in Fe‐8%Cr over that in pure Fe. The development of extended defect structure is then shown to depend on this motion and the influence of nearby surfaces in the transmission electron microscopy thin samples. In a second project, the damage microstructure is followed to high dose (200 dpa) in an oxide dispersion strengthened ferritic alloy at 500°C, and found to be qualitatively similar to that observed in the same alloy neutron irradiated at 420°C. Microsc. Res. Tech., 2009. © 2009 Wiley‐Liss, Inc.

Oxide dispersion strengthened (ODS) steels are prime candidates for high-temperature, high-dose cladding in advanced nuclear reactors. When a 9Cr-ODS alloy was irradiated with 5 MeV nickel ions at temperatures of 500–700°C to doses up to 150 dpa, there was no significant change in the dislocation arrangement. For oxide particles, there is a small shrinkage in size and increase in density with increasing irradiation dose. This work confirms that oxide particles and the microstructure of the 9Cr-ODS show minimal changes under irradiation at temperatures up to 700°C and doses up to 150 dpa.

The experimental study of grain growth in nanocrystalline metallic foils under ion irradiation showed the existence of a low-temperature regime (below about 0.15–0.22Tm), where grain growth is independent of the irradiation temperature, and a thermally assisted regime where grain growth is enhanced with increasing irradiation temperature. A model is proposed to describe grain growth under irradiation in the temperature-independent regime, based on the direct impact of the thermal spikes on grain boundaries. In the model, grain-boundary migration occurs by atomic jumps, within the thermal spikes, biased by the local grain-boundary curvature driving. The jumps in the spike are calculated based on Vineyard’s analysis of thermal spikes and activated processes using a spherical geometry for the spike. The model incorporates cascade structure features such as subcascade formation, and the probability of subcascades occurring at grain boundaries. This results in a power law expression relating the average grain size with the ion dose with an exponent equal to 3, in agreement with the experimental observations. The model is applied to grain growth observed in situ in a transmission electron microscope in a wide range of doses, temperature, and irradiation conditions for four different pure metals, and shown to predict well the results in all applicable cases. Some discussions are also presented on the expansion of the model to the thermally assisted regime. The paper is organized in six sections. Section I gives background and literature review, while Secs. II and III review experimental methods and results for in situ grain growth under irradiation. Section IV derives the model proposed to find the grain-growth equation in the nonthermal regime, and in Sec. V the model is applied to the results. In Sec. VI grain growth in the thermally assisted regime is discussed and Sec. VII presents the conclusions.