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Lach, Timothy G.

Publications and source records attributed to Lach, Timothy G..

22 records · Page 2

Resolving atomic transport through iron oxide under irradiation using isotopic tracers

Structural materials in nuclear environments are exposed to complex and harsh conditions, including high temperatures, corrosive solutions, and irradiation. Material stability and likewise degradation are fundamentally controlled by atomic transport mechanisms. Here, we investigate the influence of radiation-induced, non-equilibrium point defect populations on mass transport within model oxide systems using isotopic tracers and atom probe tomography. An isotopically labelled hematite (a-Fe2O3) film was synthesized with 16O- and 18O-rich layers (>30nm and 10 nm, respectively) sequentially deposited via molecular beam epitaxy. One region of the film was proton irradiated to ~0.1 dpa at 450°C, and regions outside the beam spot provided a non-irradiated control of thermal annealing only. 3D APT was used to directly visualize the elemental and O-isotopic redistribution following both thermal and combined thermal and irradiation conditions. Complementary scanning transmission electron microscopy (STEM) was also employed to study the microstructural evolution. Error function fits of the 18O-concentration profiles enabled quantification of diffusion coefficients.

isotopic tracers, diffusion, proton irradiation, h↗

Precipitation-site competition in duplex stainless steels: Cu clusters vs spinodal decomposition interfaces as nucleation sites during thermal aging

Competing microstructural evolution mechanisms can exist simultaneously when duplex stainless steels are operating for several decades in a high temperature service environment. Such competition between different microstructural evolution pathways can be difficult to ascertain using simple model alloy systems necessitating detailed structural and compositional analysis of phase transformation mechanisms in complex alloys Thus, in this study duplex stainless steels with complex but well understood chemistries were used to investigate the relative importance of different heterogeneous nucleation sites – specifically spinodal decomposition and Cu clustering – on precipitation of Ni-Si-Mn particles during long term thermal aging. Precipitation of Ni-Si-Mn particles in duplex stainless steels and ferritic steels during thermal aging and irradiation is known to have profound effect on mechanical properties. Using duplex stainless steels with custom modified compositions along with atom probe tomography characterization and first-passage kinetic Monte Carlo (FPKMC) simulations it is revealed that while the interface between Cr and Fe formed during spinodal decomposition can be a pathway for diffusion of Ni, Si, Mn, and Cu, it is not a site that encourages precipitation of Ni-Si-Mn rich particles. Instead, the presence of a higher concentration of Cu in these steels leads to formation of small Cu clusters with high energy interfaces that act as nucleation sites for Ni-Si-Mn particles because of its strong interaction particularly with Ni increasing the chemical driving force for precipitation. These results will help inform predictive models for the use of duplex stainless steels and other precipitation-hardened alloys for extended operation at high temperatures.

Duplex stainless steel, Thermal aging, Precipitati↗

A new non-diffusional gas bubble production route in used nuclear fuel: Implications for fission gas release, cladding corrosion, and next generation fuel design

The relationship between noble metal phase particles and fission gas bubble production in used nuclear fuel is described. The majority of Te atoms within noble metal phase undergo radioactive decay to form stable Xe within a few hours after particle formation. This results in the production of clusters of Xe atoms contained within the solid metal matrix exhibiting an equivalent gas bubble pressure approaching 1 GPa. These high pressure bubbles are stabilized by the UO2 within the bulk of the fuel. However, when these bubbles form near the fuel / cladding interface, in combination with local and temporal damage caused by fission recoil, they are capable of overcoming the fracture strength of the UO2 and rupturing catastrophically. The force of the resulting bubble rupture is sufficient to eject noble metal phase particles several microns into the cladding. This proposed mechanism explains the observance of noble metal phase in cladding and is consistent with a host of morphological features found near the fuel / cladding interface.

Schwantes, Jon M.↗