Philip D. Edmondson

Effects of sequential tungsten and helium ion implantation on nano-indentation hardness of tungsten

To simulate neutron and helium damage in a fusion reactor first wall sequential self-ion implantation up to 13 dpa followed by helium-ion implantation up to 3000 appm was performed to produce damaged layers of ∼2 μm depth in pure tungsten. The hardness of these layers was measured using nanoindentation and was studied using transmission electron microscopy. Substantial hardness increases were seen in helium implanted regions, with smaller hardness increases in regions which had already been self-ion implanted, thus, containing pre-existing dislocation loops. This suggests that, for the same helium content, helium trapped in distributed vacancies gives stronger hardening than helium trapped in vacancies condensed into dislocation loops.

Structural modification of nanocrystalline ceria by ion beams

Exceptional size-dependent electronic-ionic conductivity of nanostructured ceria can significantly alter materials properties in chemical, physical, electronic and optical applications. Using energetic ions, we have demonstrated effective modification of interface volume and grain size in nanocrystalline ceria from a few nm up to ∼25 nm, which is the critical region for controlling size-dependent material property. The grain size increases and follows an exponential law as a function of ion fluence that increases with temperature, while the cubic phase is stable under the irradiation. The unique self-healing response of radiation damage at grain boundaries is utilized to control the grain size at the nanoscale. Structural modification by energetic ions is proposed to achieve desirable electronic-ionic conductivity.

The effect of electronic energy loss on irradiation-induced grain growth in nanocrystalline oxides

Grain growth of nanocrystalline materials is generally thermally activated, but can also be driven by irradiation at much lower temperature. In nanocrystalline ceria and zirconia, energetic ions deposit their energy to both atomic nuclei and electrons. Our experimental results have shown that irradiation-induced grain growth is dependent on the total energy deposited, where electronic energy loss and elastic collisions between atomic nuclei both contribute to the production of disorder and grain growth. Our atomistic simulations reveal that a high density of disorder near grain boundaries leads to locally rapid grain movement. The additive effect from both electronic excitation and atomic collision cascades on grain growth demonstrated in this work opens up new possibilities for controlling grain sizes to improve functionality of nanocrystalline materials.

Amorphization of crystalline Si due to heavy and light ion irradiation

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.

Thermodynamic and kinetic modeling of Mn-Ni-Si precipitates in low-Cu reactor pressure vessel steels

Abstract Formation of large volume fractions of Mn-Ni-Si precipitates (MNSPs) causes excess irradiation embrittlement of reactor pressure vessel (RPV) steels at high, extended-life fluences. Thus, a new and unique, semi-empirical cluster dynamics model was developed to study the evolution of MNSPs in low-Cu RPV steels. The model is based on CALPHAD thermodynamics and radiation enhanced diffusion kinetics. The thermodynamics dictates the compositional and temperature dependence of the free energy reductions that drive precipitation. The model treats both homogeneous and heterogeneous nucleation, where the latter occurs on cascade damage, like dislocation loops. The model has only four adjustable parameters that were fit to an atom probe tomography (APT) database. The model predictions are in semi-quantitative agreement with systematic Mn, Ni and Si composition variations in alloys characterized by APT, including a sensitivity to local tip-to-tip variations even in the same steel. The model predicts that heterogeneous nucleation plays a critical role in MNSP formation in lower alloy Ni contents. Single variable assessments of compositional effects show that Ni plays a dominant role, while even small variations in irradiation temperature can have a large effect on the MNSP evolution. Within typical RPV steel ranges, Mn and Si have smaller effects. The delayed but then rapid growth of MNSPs to large volume fractions at high fluence is well predicted by the model. For purposes of illustration, the effect of MNSPs on transition temperature shifts are presented based on well-established microstructure-property and property-property models.

Imaging of radiation damage using complementary field ion microscopy and atom probe tomography.

Radiation damage in tungsten and a tungsten-tantalum alloy, both of relevance to nuclear fusion research, has been characterized using a combination of field ion microscopy (FIM) imaging and atom probe tomography (APT). While APT provides 3D analytical imaging with sub-nanometer resolution, FIM is capable of imaging the arrangements of single atoms on a crystal lattice and has the potential to provide insights into radiation induced crystal damage, all the way down to its smallest manifestation--a single vacancy. This paper demonstrates the strength of combining these characterization techniques. In ion implanted tungsten, it was found that atomic scale lattice damage is best imaged using FIM. In certain cases, APT reveals an identifiable imprint in the data via the segregation of solute and impurities and trajectory aberrations. In a W-5at%Ta alloy, a combined APT-FIM study was able to determine the atomic distribution of tantalum inside the tungsten matrix. An indirect method was implemented to identify tantalum atoms inside the tungsten matrix in FIM images. By tracing irregularities in the evaporation sequence of atoms imaged with FIM, this method enables the benefit of FIMs atomic resolution in chemical distinction between the two species.

Nanoscale Stoichiometric Analysis of a High-Temperature Superconductor by Atom Probe Tomography

The functional properties of the high-temperature superconductor Y1Ba2Cu3O7-δ (Y-123) are closely correlated to the exact stoichiometry and oxygen content. Exceeding the critical value of 1 oxygen vacancy for every five unit cells (δ>0.2, which translates to a 1.5 at% deviation from the nominal oxygen stoichiometry of Y7.7Ba15.3Cu23O54-δ ) is sufficient to alter the superconducting properties. Stoichiometry at the nanometer scale, particularly of oxygen and other lighter elements, is extremely difficult to quantify in complex functional ceramics by most currently available analytical techniques. The present study is an analysis and optimization of the experimental conditions required to quantify the local nanoscale stoichiometry of single crystal yttrium barium copper oxide (YBCO) samples in three dimensions by atom probe tomography (APT). APT analysis required systematic exploration of a wide range of data acquisition and processing conditions to calibrate the measurements. Laser pulse energy, ion identification, and the choice of range widths were all found to influence composition measurements. The final composition obtained from melt-grown crystals with optimized superconducting properties was Y7.9Ba10.4Cu24.4O57.2.

Influence of irradiation temperature on microstructure of EU batch of ODS Eurofer97 steel irradiated with neutrons

Abstract A TEM investigation of an EU batch of oxide dispersed strengthened (ODS) Eurofer97 steel specimens, irradiated to 1 and 3 dpa at 300, 450 and 550°C in high flux reactor at Petten, has been performed to understand the influence of irradiation temperature on the characteristics of irradiation defects and, eventually, on the resulting mechanical properties of this material. Specimens irradiated at 300°C revealed the presence of a high density of black dot damage and small self-interstitial atom (SIA) dislocation loops causing substantial hardening and embrittlement. In contrast, negligible black dot damage, low density of large SIA loops and networks of dislocations are observed in specimens irradiated at 450 and 550°C. The lath martensitic structure and ODS particles remain unaffected after irradiation in all specimens. These results are discussed in view of possible activation of defect annihilation mechanisms to explain the observed recovery of mechanical properties at high irradiation temperatures.

A Challenge to Multivariate Statistical Analysis: Spent Nuclear Fuel

Nuclear fission accounts for most of the non-polluting, non-fossil-fuel electrical power in the world. Higher burnup of fuel – that is, using a given fuel bundle for a longer time to produce more power – reduces the uranium resources needed, greatly enhances the economics of nuclear electricity, and reduces the amount of spent fuel for disposal. However, as the fuel burnup progresses, the fission process builds up large atomic fractions of fission products, consisting of most elements in the central region of the periodic table, in the fluorite UO2 matrix; and, a fuel/clad interaction (FCI) layer forms at the interface between the oxide fuel and the Zircaloy cladding. Providing a scientific basis for understating fuel behavior in the high burnup regime requires detailed characterization of high-burnup urania fuel. We have used X-ray spectrum imaging (SI) in SEM and STEM to analyze high-burnup (irradiated for 7 eighteen month long cycles to average burnup of 72 GWd/MTU) fuel from the H.B. Robinson pressurized water reactor. Multivariate statistical analysis (MVSA) is irreplaceable for understanding the extremely complex chemistry found.

Atomic Scale, 3-Dimensional Characterization of Radiation Effects in Tungsten for Fusion Applications

The refractory metal tungsten is a promising candidate material for plasma facing components (PFCs) in future fusion reactors due in part to its low sputter yield, good thermal conductivity and low activation under transmutation. However, tungsten suffers from a very high brittle-to-ductile transition temperature (BDTT) of 400-500 °C [1]. This inherent brittleness is only exacerbated under irradiation due to the irradiation-induced defects and the formation of second phase precipitates containing the transmutation products Re and Os. [2,3] Here, we discuss the use of novel field ion microscopy (FIM) and atom probe tomography (APT) techniques to investigate radiation effects in irradiated tungsten.