Publications

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Preliminary evaluation of deep borehole disposal of high-level radioactive waste and spent nuclear fuel indicates the potential for excellent long-term safety performance at costs competitive with mined repositories. Significant fluid flow through basement rock is prevented, in part, by low permeabilities, poorly connected transport pathways, and overburden self-sealing. Deep fluids also resist vertical movement because they are density stratified. Thermal hydrologic calculations estimate the thermal pulse from emplaced waste to be small (less than 20 C at 10 meters from the borehole, for less than a few hundred years), and to result in maximum total vertical fluid movement of {approx}100 m. Reducing conditions will sharply limit solubilities of most dose-critical radionuclides at depth, and high ionic strengths of deep fluids will prevent colloidal transport. For the bounding analysis of this report, waste is envisioned to be emplaced as fuel assemblies stacked inside drill casing that are lowered, and emplaced using off-the-shelf oilfield and geothermal drilling techniques, into the lower 1-2 km portion of a vertical borehole {approx}45 cm in diameter and 3-5 km deep, followed by borehole sealing. Deep borehole disposal of radioactive waste in the United States would require modifications to the Nuclear Waste Policy Act and to applicable regulatory standards for long-term performance set by the US Environmental Protection Agency (40 CFR part 191) and US Nuclear Regulatory Commission (10 CFR part 60). The performance analysis described here is based on the assumption that long-term standards for deep borehole disposal would be identical in the key regards to those prescribed for existing repositories (40 CFR part 197 and 10 CFR part 63).

The chemistries of reactants, plasticizers, solvents and additives in an epoxy paint are discussed. Polyamide additives may play an important role in the absorption of molecular iodine by epoxy paints. It is recommended that the unsaturation of the polyamide additive in the epoxy cure be determined. Experimental studies of water absorption by epoxy resins are discussed. These studies show that absorption can disrupt hydrogen bonds among segments of the polymers and cause swelling of the polymer. The water absorption increases the diffusion coefficient of water within the polymer. Permanent damage to the polymer can result if water causes hydrolysis of ether linkages. Water desorption studies are recommended to ascertain how water absorption affects epoxy paint.

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The most energy efficient solid state white light source will likely be a combination of individually efficient red, green, and blue LED. For any multi-color approach to be successful the efficiency of deep green LEDs must be significantly improved. While traditional approaches to improve InGaN materials have yielded incremental success, we proposed a novel approach using group IIIA and IIIB nitride semiconductors to produce efficient green and high wavelength LEDs. To obtain longer wavelength LEDs in the nitrides, we attempted to combine scandium (Sc) and yttrium (Y) with gallium (Ga) to produce ScGaN and YGaN for the quantum well (QW) active regions. Based on linear extrapolation of the proposed bandgaps of ScN (2.15 eV), YN (0.8 eV) and GaN (3.4 eV), we expected that LEDs could be fabricated from the UV (410 nm) to the IR (1600 nm), and therefore cover all visible wavelengths. The growth of these novel alloys potentially provided several advantages over the more traditional InGaN QW regions including: higher growth temperatures more compatible with GaN growth, closer lattice matching to GaN, and reduced phase separation than is commonly observed in InGaN growth. One drawback to using ScGaN and YGaN films as the active regions in LEDs is that little research has been conducted on their growth, specifically, are there metalorganic precursors that are suitable for growth, are the bandgaps direct or indirect, can the materials be grown directly on GaN with a minimal defect formation, as well as other issues related to growth. The major impediment to the growth of ScGaN and YGaN alloys was the low volatility of metalorganic precursors. Despite this impediment some progress was made in incorporation of Sc and Y into GaN which is detailed in this report. Primarily, we were able to incorporate up to 5 x 10{sup 18} cm{sup -3} Y atoms into a GaN film, which are far below the alloy concentrations needed to evaluate the YGaN optical properties. After a no-cost extension was granted on this program, an additional more 'liquid-like' Sc precursor was evaluated and the nitridation of Sc metals on GaN were investigated. Using the Sc precursor, dopant level quantities of Sc were incorporated into GaN, thereby concluding the growth of ScGaN and YGaN films. Our remaining time during the no-cost extension was focused on pulsed laser deposition of Sc metal films on GaN, followed by nitridation in the MOCVD reactor to form ScN. Finally, GaN films were deposited on the ScN thin films in order to study possible GaN dislocation reduction.

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With no lattice matched substrate available, sapphire continues as the substrate of choice for GaN growth, because of its reasonable cost and the extensive prior experience using it as a substrate for GaN. Surprisingly, the high dislocation density does not appear to limit UV and blue LED light intensity. However, dislocations may limit green LED light intensity and LED lifetime, especially as LEDs are pushed to higher current density for high end solid state lighting sources. To improve the performance for these higher current density LEDs, simple growth-enabled reductions in dislocation density would be highly prized. GaN nucleation layers (NLs) are not commonly thought of as an application of nano-structural engineering; yet, these layers evolve during the growth process to produce self-assembled, nanometer-scale structures. Continued growth on these nuclei ultimately leads to a fully coalesced film, and we show in this research program that their initial density is correlated to the GaN dislocation density. In this 18 month program, we developed MOCVD growth methods to reduce GaN dislocation densities on sapphire from 5 x 10{sup 8} cm{sup -2} using our standard delay recovery growth technique to 1 x 10{sup 8} cm{sup -2} using an ultra-low nucleation density technique. For this research, we firmly established a correlation between the GaN nucleation thickness, the resulting nucleation density after annealing, and dislocation density of full GaN films grown on these nucleation layers. We developed methods to reduce the nuclei density while still maintaining the ability to fully coalesce the GaN films. Ways were sought to improve the GaN nuclei orientation by improving the sapphire surface smoothness by annealing prior to the NL growth. Methods to eliminate the formation of additional nuclei once the majority of GaN nuclei were developed using a silicon nitride treatment prior to the deposition of the nucleation layer. Nucleation layer thickness was determined using optical reflectance and the nucleation density was determined using atomic force microscopy (AFM) and Nomarski microscopy. Dislocation density was measured using X-ray diffraction and AFM after coating the surface with silicon nitride to delineate all dislocation types. The program milestone of producing GaN films with dislocation densities of 1 x 10{sup 8} cm{sup -2} was met by silicon nitride treatment of annealed sapphire followed by the multiple deposition of a low density of GaN nuclei followed by high temperature GaN growth. Details of this growth process and the underlying science are presented in this final report along with problems encountered in this research and recommendations for future work.

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