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At least 649 records · Page 36

Mechanism of β-FeSi{sub 2} precipitates growth-and-dissolution and pyramidal defects' formation during oxidation of Fe-contaminated silicon wafers

Fe-implanted Si-wafers have been oxidized at 900 °C and 1100 °C in order to investigate the behaviour of Fe atoms at the growing SiO{sub 2}/Si interface and the impact on the integrity of microelectronic devices of an involuntary Fe contamination before or during the oxidation process. As-implanted and oxidized wafers have been characterized using secondary ion mass spectroscopy, atom probe tomography, and high-resolution transmission electron microscopy. Experimental results were compared to calculated implantation profiles and simulated images. Successive steps of iron disilicide precipitation and oxidation were evidenced during the silicon oxidation process. The formation of characteristic pyramidal-shaped defects, at the SiO{sub 2}/Si interface, was notably found to correlate with the presence of β-FeSi{sub 2} precipitates. Taking into account the competitive oxidation of these precipitates and of the surrounding silicon matrix, dynamic mechanisms are proposed to model the observed microstructural evolution of the SiO{sub 2}/Si interface, during the growth of the silicon oxide layer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Dissolution of Mg-enriched defects in implanted GaN and increased p-type dopant activation

Annealing Mg-implanted homoepitaxial GaN at temperatures above 1400 °C eliminates the formation of inversion domains and leads to improved dopant activation efficiency. Extended defects, in the form of inversion domains, contain electrically inactive Mg after post-implantation annealing at temperatures as high as 1300 °C (one GPa N 2 overpressure), which results in a low dopant activation efficiency. Triple-axis x-ray data reveal that implant-induced strain is fully relieved after annealing at 1300 °C for 10 min, indicating that strain-inducing point defects formed during implantation have reconfigured and inversion domains are formed. However, annealing at temperatures of 1400–1500 °C (one GPa N 2 overpressure) eliminates the presence of the inversion domains. While residual defects, such as dislocation loops, still exist after annealing at and above 1400 °C, chemical analysis at multiple dislocation loops shows no sign of Mg segregation. Meanwhile, an overall decreasing trend in the dislocation loop density is observed after annealing at the higher temperatures and longer times. Additionally, once inversion domains are formed and the samples are cooled to room temperature, they are shown to dissolve with subsequent annealing above 1400 °C. While such defects have been observed before, the important finding that such defects can be dissolved with a short, higher temperature step is key. Earlier work [Breckenridge et al., J. Appl. Phys. Lett. 118, 022101 (2021)] addressing electrical measurements of these types of samples showed that annealing at 1400 °C leads to a dopant activation efficiency that is an order of magnitude higher than that observed at 1300 °C. In conclusion, this work complements earlier work by identifying the inversion domains, which incorporate Mg, and points to the benefits, in terms of defect density and p-type dopant activation, of using higher temperature (>1400 °C) annealing cycles to activate Mg in GaN, even if the Mg-containing inversion domains had been formed during lower temperature annealing.

36 MATERIALS SCIENCE↗

Characterization of Fe and Cr Dissolution and Reaction Product Formation in Molten Chloride Salts With and Without Impurities

There is considerable interest in molten chloride salts for several applications including thermal storage and next-generation molten salt reactors (MSRs). Several studies have concluded that Cl salts are highly corrosive to structural materials. Using Oak Ridge National Laboratory’s established methodology, Cl salt compatibility was assessed for candidate Ni-based alloys 230, 600 and 740 H at 600°–800°C in static welded capsules and in flowing thermal convection loop (TCL) salt experiments. Simply drying commercial Cl salt at 550°–650°C and adding~0.05 wt.%Mg was able to produce small specimen mass changes and limited surface attack after 100–1000 h exposures. Intentional additions of H 2 O, NiCl 2 and undried salt were used to better understand the role of impurities and achieve the>50 µm levels of attack reported in other studies. Further, characterisation of Cr depletion and oxide formation in conjunction with pre- and post-test salt chemistry measurements are being used to understand salt compatibility of structural materials.

36 MATERIALS SCIENCE↗

Lattice Boltzmann method for diffusion-limited partial dissolution of fluids

A lattice Boltzmann model for two partially miscible fluids is developed. By partially miscible, we mean that although there is a definite interfacial region separating the two fluids with a surface tension force acting at all points of the transition region, each fluid can nonetheless accept molecules from the other fluid up to a set solubility limit. We allow each fluid to diffuse into the other with the solubility and diffusivity in each fluid being input parameters. The approach is to define two regions within the fluid. One interfacial region having finite width, across which most of the concentration change occurs, and in which a surface tension force and color separation step are allowed for. And one miscible fluid region where the concentration of the binary fluids follows an advection-diffusion equation and the mixture as a whole obeys the Navier-Stokes incompressible flow equations. Numerical examples are presented in which the algorithm produces results that are quantitatively compared to exact analytical results as well as qualitatively examined for their reasonableness. The model has the ability to simulate how bubbles of one fluid flow through another while dissolving their contents as well as to a range of practical invasion problems such as injecting supercritical CO 2 into a porous material saturated with water for sequestration purposes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Desorption and Co–Dissolution of Uranium–Bearing Solids During Alkalinity–Enhanced Flushing of Contaminated Sediments

Elevated uranium concentrations in groundwater remain a persistent challenge at contaminated sites. Several sites rely on natural flushing of uranium as a remediation strategy. Uncertainties in conceptual models can cause remediation strategies to underestimate timeframes required to reach remediation goals. In this study, laboratory experiments were conducted to investigate uranium flushing of sediments from a site with persistent groundwater contamination. Six columns were used to simulate alkalinity-enhanced flushing of uranium from sediments, by switching influent alkalinity after ~12 pore volumes. About 20% to 31% of sediment uranium was consistently flushed from the sediments. K d values varied greatly (5.3 to 117 L/kg) but were consistently lower (20% to 50%) during influents with elevated alkalinity. The mass of uranium recovered from the columns also was consistently higher (5% to 80%) during alkalinity-enhanced flushing periods. However, column experiments with sequentially increasing alkalinity showed diminishing returns in uranium elution at higher carbonate concentrations. The loss of flushing efficiency is attributed to significant calcite precipitation at higher alkalinities. Furthermore, the results show that alkalinity-enhanced flushing of uranium could be employed as a viable remediation scheme if calcite precipitation could be minimized in a field application.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Gas generation during waste treatment of acidic solutions from the dissolution of irradiated LEU targets for 99 Mo production

The goal of the Reduced Enrichment for Research and Test Reactors Program is to limit the use of high-enriched uranium (HEU) in research and test reactors by substituting low-enriched uranium (LEU) wherever possible. The work reported here documents our work to develop the calcining technologies and processes that will be needed for 99 Mo production using LEU foil targets and the Modified Cintichem Process. The primary concern with the conversion to LEU from HEU targets is that it would result in a five- to six-fold increase in the total uranium. This increase results in more liquid waste from the process. We have been working to minimize the increase in liquid waste and to minimize the impact of any change in liquid waste. Direct calcination of uranium-rich nitric acid solutions generates NO 2 gas and UO 3 solid. We have proposed two processes for treating the liquid waste from a Modified Cintichem Process with a LEU foil. One is an optimized direct calcination process that is similar to the process currently in use. The other is a uranyl oxalate precipitation process. The specific goal of the work reported here was to characterize and compare the chemical reactions that occur during these two processes. In particular, the amounts and compositions of the gaseous and solid products were of interest. A series of experiments was carried out to show the effects of temperature and the redox potential of the reaction atmosphere. The primary products of the direct calcination process were mixtures of U 3 O 8 and UO 3 solids and NO 2 gas. The primary products of the oxalate precipitation process were mixtures of U 3 O 8 and UO 2 solid and CO 2 gas. Higher temperature and a reducing atmosphere tended to favor quadrivalent over hexavalent uranium in the solid product. These data will help producers to decide between the two processes. In addition, the data can be used to design appropriate off-gas systems for pilot and production facilities.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗