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Hierarchical electrode architectures for electrical energy storage & conversion.

Description: The integration and stability of electrocatalytic nanostructures, which represent one level of porosity in a hierarchical structural scheme when combined with a three-dimensional support scaffold, has been studied using a combination of synthetic processes, characterization techniques, and computational methods. Dendritic platinum nanostructures have been covalently linked to common electrode surfaces using a newly developed chemical route; a chemical route equally applicable to a range of metals, oxides, and semiconductive materials. Characterization of the resulting bound nanostructure system confirms successful binding, while electrochemistry and microscopy demonstrate the viability of these electroactive particles. Scanning tunneling microscopy has been used to image and validate the short-term stability of several electrode-bound platinum dendritic sheet structures toward Oswald ripening. Kinetic Monte Carlo methods have been applied to develop an understanding of the stability of the basic nano-scale porous platinum sheets as they transform from an initial dendrite to hole containing sheets. Alternate synthetic strategies were pursued to grow dendritic platinum structures directly onto subunits (graphitic particles) of the electrode scaffold. A two-step photocatalytic seeding process proved successful at generating desirable nano-scale porous structures. Growth in-place is an alternate strategy to the covalent linking of the electrocatalytic nanostructures.
Date: January 1, 2012
Creator: Zavadil, Kevin Robert; Missert, Nancy A.; Shelnutt, John Allen & van Swol, Frank B.
Partner: UNT Libraries Government Documents Department

The effects of varying humidity on copper sulfide film formation.

Description: Detailed experiments involving extensive high resolution transmission electron microscopy (TEM) revealed significant microstructural differences between Cu sulfides formed at low and high relative humidity (RH). It was known from prior experiments that the sulfide grows linearly with time at low RH up to a sulfide thickness approaching or exceeding one micron, while the sulfide initially grows linearly with time at high RH then becomes sub-linear at a sulfide thickness less than about 0.2 microns, with the sulfidation rate eventually approaching zero. TEM measurements of the Cu2S morphology revealed that the Cu2S formed at low RH has large sized grains (75 to greater than 150 nm) that are columnar in structure with sharp, abrupt grain boundaries. In contrast, the Cu2S formed at high RH has small equiaxed grains of 20 to 50 nm in size. Importantly, the small grains formed at high RH have highly disordered grain boundaries with a high concentration of nano-voids. Two-dimensional diffusion modeling was performed to determine whether the existence of localized source terms at the Cu/Cu2S interface could be responsible for the suppression of Cu sulfidation at long times at high RH. The models indicated that the existence of static localized source terms would not predict the complete suppression of growth that was observed. Instead, the models suggest that the diffusion of Cu through Cu2S becomes restricted during Cu2S formation at high RH. The leading speculation is that the extensive voiding that exists at grain boundaries in this material greatly reduces the flux of Cu between grains, leading to a reduction in the rate of sulfide film formation. These experiments provide an approach for adding microstructural information to Cu sulfidation rate computer models. In addition to the microstructural studies, new micro-patterned test structures were developed in this LDRD to offer insight into the point defect structure ...
Date: February 1, 2004
Creator: Mayer, Thomas Michael; Missert, Nancy A.; Barbour, John Charles; Sullivan, John Patrick; Copeland, Robert Guild & Campin, Michael J. (International Sematech, Austin, TX)
Partner: UNT Libraries Government Documents Department

Low-Dislocation-Density GaN from a Single Growth on a Textured Substrate

Description: The density of threading dislocations (TD) in GaN grown directly on flat sapphire substrates is typically greater than 10{sup 9}/cm{sup 2}. Such high dislocation densities degrade both the electronic and photonic properties of the material. The density of dislocations can be decreased by orders of magnitude using cantilever epitaxy (CE), which employs prepatterned sapphire substrates to provide reduced-dimension mesa regions for nucleation and etched trenches between them for suspended lateral growth of GaN or AlGaN. The substrate is prepatterned with narrow lines and etched to a depth that permits coalescence of laterally growing III-N nucleated on the mesa surfaces before vertical growth fills the etched trench. Low dislocation densities typical of epitaxial lateral overgrowth (ELO) are obtained in the cantilever regions and the TD density is also reduced up to 1 micrometer from the edge of the support regions.
Date: July 31, 2000
Partner: UNT Libraries Government Documents Department

Growth and Oxidation of Thin Film Al(2)Cu

Description: Al{sub 2}Cu thin films ({approx} 382 nm) are fabricated by melting and resolidifying Al/Cu bilayers in the presence of a {micro} 3 nm Al{sub 2}O{sub 3} passivating layer. X-ray Photoelectron Spectroscopy (XPS) measures a 1.0 eV shift of the Cu2p{sub 3/2} peak and a 1.6 eV shift of the valence band relative to metallic Cu upon Al{sub 2}Cu formation. Scanning Electron microscopy (SEM) and Electron Back-Scattered Diffraction (EBSD) show that the Al{sub 2}Cu film is composed of 30-70 {micro}m wide and 10-25 mm long cellular grains with (110) orientation. The atomic composition of the film as estimated by Energy Dispersive Spectroscopy (EDS) is 67 {+-} 2% Al and 33 {+-} 2% Cu. XPS scans of Al{sub 2}O{sub 3}/Al{sub 2}Cu taken before and after air exposure indicate that the upper Al{sub 2}Cu layers undergo further oxidation to Al{sub 2}O{sub 3} even in the presence of {approx} 5 nm Al{sub 2}O{sub 3}. The majority of Cu produced from oxidation is believed to migrate below the Al{sub 2}O{sub 3} layers, based upon the lack of evidence for metallic Cu in the XPS scans. In contrast to Al/Cu passivated with Al{sub 2}O{sub 3}, melting/resolidifying the Al/Cu bilayer without Al{sub 2}O{sub 3} results in phase-segregated dendritic film growth.
Date: January 18, 2000
Partner: UNT Libraries Government Documents Department

Electronic defects and interface potentials for Al oxide films on Al and their relationship to electrochemical properties

Description: The relative electronic defect densities and oxide interface potentials were determined for naturally-occurring and synthetic Al oxides on Al. In addition, the effect of electrochemical treatment on the oxide electrical properties was assessed. The measurements revealed (1) that the open circuit potential of Al in aqueous solution is inversely correlated with the oxide electronic defect density (viz., lower oxide conductivities are correlated with higher open circuit potentials), and (2) the electronic defect density within the Al oxide is increased upon exposure to an aqueous electrolyte at open circuit or applied cathodic potentials, while the electronic defect density is reduced upon exposure to slight anodic potentials in solution. This last result, combined with recent theoretical predictions, suggests that hydrogen may be associated with electronic defects within the Al oxide, and that this H may be a mobile species, diffusing as H{sup +}. The potential drop across the oxide layer when immersed in solution at open circuit conditions was also estimated and found to be 0.3 V, with the field direction attracting positive charge towards the Al/oxide interface.
Date: June 1, 2000
Partner: UNT Libraries Government Documents Department

A Combinatorial Approach to Determine Mechanisms of Atmospheric Copper Sulfidation

Description: Parallel microscopic experimentation (the combinatorial approach often used in solid-state science) was applied to characterize atmospheric copper corrosion behavior. Specifically, this technique permitted relative sulfidation rates to be determined for copper containing different levels of point defects and impurities (In, Al, O, and D). Corrosion studies are inherently difficult because of complex interactions between material interfaces and the environment. The combinatorial approach was demonstrated using micron-scale Cu lines that were exposed to a humid air environment containing sub-ppm levels of H{sub 2}S. The relative rate of Cu{sub 2}S growth was determined by measuring the change in resistance of the line. The data suggest that vacancy trapping by In and Al impurities slow the sulfidation rate. Increased sulfidation rates were found for samples containing excess point defects or deuterium. Furthermore, the sulfidation rate of 14 {micro}m wide Cu lines was increased above that for planar films.
Date: October 7, 1999
Partner: UNT Libraries Government Documents Department

Crevice Corrosion Initiation at Engineered Cu-Rich Defects in Al Thin Films

Description: Engineered Cu-rich islands were fabricated on an Al thin film to investigate pit initiation mechanisms at noble particles. X-ray photoelectron spectroscopy confirms that the thin film Cu-rich islands interdiffuse with the underlying Al substrate to form Al{sub 2}Cu islands. The defect arrays exhibit open circuit potential fluctuations whose magnitude and frequency increase as defect spacing decreases for constant island size and cathode/anode ratio. Post-exposure examination by energy dispersive spectroscopy (EDS) shows that the Al beneath the Cu-rich island dissolves with a crevice geometry. Engineered Al islands fabricated under identical conditions do not induce crevice corrosion in the vicinity of the Al defects. These results suggest that the Al dissolution is driven by the galvanic coupling between the noble island and matrix, and/or by a local change in chemistry, rather than by the presence of a defective oxide in the vicinity of the island.
Date: October 14, 1999
Partner: UNT Libraries Government Documents Department

Mechanisms of Atmospheric Copper Sulfidation and Evaluation of Parallel Experimentation Techniques

Description: A physics-based understanding of material aging mechanisms helps to increase reliability when predicting the lifetime of mechanical and electrical components. This report examines in detail the mechanisms of atmospheric copper sulfidation and evaluates new methods of parallel experimentation for high-throughput corrosion analysis. Often our knowledge of aging mechanisms is limited because coupled chemical reactions and physical processes are involved that depend on complex interactions with the environment and component functionality. Atmospheric corrosion is one of the most complex aging phenomena and it has profound consequences for the nation's economy and safety. Therefore, copper sulfidation was used as a test-case to examine the utility of parallel experimentation. Through the use of parallel and conventional experimentation, we measured: (1) the sulfidation rate as a function of humidity, light, temperature and O{sub 2} concentration; (2) the primary moving species in solid state transport; (3) the diffusivity of Cu vacancies through Cu{sub 2}S; (4) the sulfidation activation energies as a function of relative humidity (RH); (5) the sulfidation induction times at low humidities; and (6) the effect of light on the sulfidation rate. Also, the importance of various sulfidation mechanisms was determined as a function of RH and sulfide thickness. Different models for sulfidation-reactor geometries and the sulfidation reaction process are presented.
Date: March 1, 2002
Partner: UNT Libraries Government Documents Department

Materials physics and device development for improved efficiency of GaN HEMT high power amplifiers.

Description: GaN-based microwave power amplifiers have been identified as critical components in Sandia's next generation micro-Synthetic-Aperture-Radar (SAR) operating at X-band and Ku-band (10-18 GHz). To miniaturize SAR, GaN-based amplifiers are necessary to replace bulky traveling wave tubes. Specifically, for micro-SAR development, highly reliable GaN high electron mobility transistors (HEMTs), which have delivered a factor of 10 times improvement in power performance compared to GaAs, need to be developed. Despite the great promise of GaN HEMTs, problems associated with nitride materials growth currently limit gain, linearity, power-added-efficiency, reproducibility, and reliability. These material quality issues are primarily due to heteroepitaxial growth of GaN on lattice mismatched substrates. Because SiC provides the best lattice match and thermal conductivity, SiC is currently the substrate of choice for GaN-based microwave amplifiers. Obviously for GaN-based HEMTs to fully realize their tremendous promise, several challenges related to GaN heteroepitaxy on SiC must be solved. For this LDRD, we conducted a concerted effort to resolve materials issues through in-depth research on GaN/AlGaN growth on SiC. Repeatable growth processes were developed which enabled basic studies of these device layers as well as full fabrication of microwave amplifiers. Detailed studies of the GaN and AlGaN growth of SiC were conducted and techniques to measure the structural and electrical properties of the layers were developed. Problems that limit device performance were investigated, including electron traps, dislocations, the quality of semi-insulating GaN, the GaN/AlGaN interface roughness, and surface pinning of the AlGaN gate. Surface charge was reduced by developing silicon nitride passivation. Constant feedback between material properties, physical understanding, and device performance enabled rapid progress which eventually led to the successful fabrication of state of the art HEMT transistors and amplifiers.
Date: December 1, 2005
Creator: Kurtz, Steven Ross; Follstaedt, David Martin; Wright, Alan Francis; Baca, Albert G.; Briggs, Ronald D.; Provencio, Paula Polyak et al.
Partner: UNT Libraries Government Documents Department

Final report on grand challenge LDRD project : a revolution in lighting : building the science and technology base for ultra-efficient solid-state lighting.

Description: This SAND report is the final report on Sandia's Grand Challenge LDRD Project 27328, 'A Revolution in Lighting -- Building the Science and Technology Base for Ultra-Efficient Solid-state Lighting.' This project, which for brevity we refer to as the SSL GCLDRD, is considered one of Sandia's most successful GCLDRDs. As a result, this report reviews not only technical highlights, but also the genesis of the idea for Solid-state Lighting (SSL), the initiation of the SSL GCLDRD, and the goals, scope, success metrics, and evolution of the SSL GCLDRD over the course of its life. One way in which the SSL GCLDRD was different from other GCLDRDs was that it coincided with a larger effort by the SSL community - primarily industrial companies investing in SSL, but also universities, trade organizations, and other Department of Energy (DOE) national laboratories - to support a national initiative in SSL R&D. Sandia was a major player in publicizing the tremendous energy savings potential of SSL, and in helping to develop, unify and support community consensus for such an initiative. Hence, our activities in this area, discussed in Chapter 6, were substantial: white papers; SSL technology workshops and roadmaps; support for the Optoelectronics Industry Development Association (OIDA), DOE and Senator Bingaman's office; extensive public relations and media activities; and a worldwide SSL community website. Many science and technology advances and breakthroughs were also enabled under this GCLDRD, resulting in: 55 publications; 124 presentations; 10 book chapters and reports; 5 U.S. patent applications including 1 already issued; and 14 patent disclosures not yet applied for. Twenty-six invited talks were given, at prestigious venues such as the American Physical Society Meeting, the Materials Research Society Meeting, the AVS International Symposium, and the Electrochemical Society Meeting. This report contains a summary of these science and technology advances and ...
Date: June 1, 2004
Creator: Copeland, Robert Guild; Mitchell, Christine Charlotte; Follstaedt, David Martin; Lee, Stephen Roger; Shul, Randy John; Fischer, Arthur Joseph et al.
Partner: UNT Libraries Government Documents Department