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Metal hydride materials have been intensively studied for hydrogen storage applications. In addition to potential hydrogen economy applications, metal hydrides offer a wide variety of other interesting properties. For example, hydrogen-dominant materials, which are hydrides with the highest hydrogen content for a particular metal/semimetal composition, are predicted to display high-temperature

Metal hydride materials have been intensively studied for hydrogen storage applications. In addition to potential hydrogen economy applications, metal hydrides offer a wide variety of other interesting properties. For example, hydrogen-dominant materials, which are hydrides with the highest hydrogen content for a particular metal/semimetal composition, are predicted to display high-temperature superconductivity. On the other side of the spectrum are hydrides with small amounts of hydrogen (0.1 - 1 at.%) that are investigated as viable magnetic, thermoelectric or semiconducting materials. Research of metal hydride materials is generally important to gain fundamental understanding of metal-hydrogen interactions in materials. Hydrogenation of Zintl phases, which are defined as compounds between an active metal (alkali, alkaline earth, rare earth) and a p-block metal/semimetal, were attempted by a hot sintering method utilizing an autoclave loaded with gaseous hydrogen (< 9 MPa). Hydride formation competes with oxidative decomposition of a Zintl phase. The oxidative decomposition, which leads to a mixture of binary active metal hydride and p-block element, was observed for investigated aluminum (Al) and gallium (Ga) containing Zintl phases. However, a new phase Li2Al was discovered when Zintl phase precursors were synthesized. Using the single crystal x-ray diffraction (SCXRD), the Li2Al was found to crystallize in an orthorhombic unit cell (Cmcm) with the lattice parameters a = 4.6404(8) Å, b = 9.719(2) Å, and c = 4.4764(8) Å. Increased demand for materials with improved properties necessitates the exploration of alternative synthesis methods. Conventional metal hydride synthesis methods, like ball-milling and autoclave technique, are not responding to the demands of finding new materials. A viable alternative synthesis method is the application of high pressure for the preparation of hydrogen-dominant materials. Extreme pressures in the gigapascal ranges can open access to new metal hydrides with novel structures and properties, because of the drastically increased chemical potential of hydrogen. Pressures up to 10 GPa can be easily achieved using the multi-anvil (MA) hydrogenations while maintaining sufficient sample volume for structure and property characterization. Gigapascal MA hydrogenations using ammonia borane (BH3NH3) as an internal hydrogen source were employed in the search for new hydrogen-dominant materials. Ammonia borane has high gravimetric volume of hydrogen, and additionally the thermally activated decomposition at high pressures lead to a complete hydrogen release at reasonably low temperature. These properties make ammonia borane a desired hydrogen source material. The missing member Li2PtH6 of the series of A2PtH6 compounds (A = Na to Cs) was accessed by employing MA technique. As the known heavier analogs, the Li2PtH6 also crystallizes in a cubic K2PtCl6-type structure with a cell edge length of 6.7681(3) Å. Further gigapascal hydrogenations afforded the compounds K2SiH6 and Rb2SiH6 which are isostructural to Li2PtH6. The cubic K2SiH6 and Rb2SiH6 are built from unique hypervalent SiH62- entities with the lattice parameters of 7.8425(9) and 8.1572(4) Å, respectively. Spectroscopic analysis of hexasilicides confirmed the presence of hypervalent bonding. The Si-H stretching frequencies at 1550 cm-1 appeared considerably decreased in comparison with a normal-valent (2e2c) Si-H stretching frequencies in SiH4 at around 2200 cm-1. However, the observed stretching modes in hypervalent hexasilicides were in a reasonable agreement with Ph3SiH2- (1520 cm-1) where the hydrogen has the axial (3e4c bonded) position in the trigoal bipyramidal environment.
ContributorsPuhakainen, Kati (Author) / Häussermann, Ulrich (Thesis advisor) / Seo, Dong (Thesis advisor) / Kouvetakis, John (Committee member) / Wolf, George (Committee member) / Arizona State University (Publisher)
Created2013
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Description
Achievement of many long-term goals requires sustained practice over long durations. Examples include goals related to areas of high personal and societal benefit, such as physical fitness, which requires a practice of frequent exercise; self-education, which requires a practice of frequent study; or personal productivity, which requires a practice of

Achievement of many long-term goals requires sustained practice over long durations. Examples include goals related to areas of high personal and societal benefit, such as physical fitness, which requires a practice of frequent exercise; self-education, which requires a practice of frequent study; or personal productivity, which requires a practice of performing work. Maintaining these practices can be difficult, because even though obvious benefits come with achieving these goals, an individual's willpower may not always be sufficient to sustain the required effort. This dissertation advocates addressing this problem by designing novel interfaces that provide people with new practices that are fun and enjoyable, thereby reducing the need for users to draw upon willpower when pursuing these long-term goals. To draw volitional usage, these practice-oriented interfaces can integrate key characteristics of existing activities, such as music-making and other hobbies, that are already known to draw voluntary participation over long durations. This dissertation makes several key contributions to provide designers with the necessary tools to create practice-oriented interfaces. First, it consolidates and synthesizes key ideas from fields such as activity theory, self-determination theory, HCI design, and serious leisure. It also provides a new conceptual framework consisting of heuristics for designing systems that draw new users, plus heuristics for making systems that will continue drawing usage from existing users over time. These heuristics serve as a collection of useful ideas to consider when analyzing or designing systems, and this dissertation postulates that if designers build these characteristics into their products, the resulting systems will draw more volitional usage. To demonstrate the framework's usefulness as an analytical tool, it is applied as a set of analytical lenses upon three previously-existing experiential media systems. To demonstrate its usefulness as a design tool, the framework is used as a guide in the development of an experiential media system called pdMusic. This system is installed at public events for user studies, and the study results provide qualitative support for many framework heuristics. Lastly, this dissertation makes recommendations to scholars and designers on potential future ways to examine the topic of volitional usage.
ContributorsWallis, Isaac (Author) / Ingalls, Todd (Thesis advisor) / Coleman, Grisha (Committee member) / Sundaram, Hari (Committee member) / Arizona State University (Publisher)
Created2013
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Description
This document is intended to show the various kinds of stylistically appropriate melodic and rhythmic ornamentation that can be used in the improvisation of the Sarabandes by J.S. Bach. Traditional editions of Bach's and other Baroque-era keyboard works have reflected evolving historical trends. The historical performance movement and other attempts

This document is intended to show the various kinds of stylistically appropriate melodic and rhythmic ornamentation that can be used in the improvisation of the Sarabandes by J.S. Bach. Traditional editions of Bach's and other Baroque-era keyboard works have reflected evolving historical trends. The historical performance movement and other attempts to "clean up" pre-1950s romanticized performances have greatly limited the freedom and experimentation that was the original intention of these dances. Prior to this study, few ornamented editions of these works have been published. Although traditional practices do not necessarily encourage classical improvisation in performance I argue that manipulation of the melodic and rhythmic layers over the established harmonic progressions will not only provide diversity within the individual dance movements, but also further engage the ears of the performer and listener which encourages further creative exploration. I will focus this study on the ornamentation of all six Sarabandes from J.S. Bach's French Suites and show how various types of melodic and rhythmic variation can provide aurally pleasing alternatives to the composed score without disrupting the harmonic fluency. The author intends this document to be used as a pedagogical tool and the fully ornamented Sarabandes from J.S. Bach's French Suites are included with this document.
ContributorsOakley, Ashley (Author) / Meir, Baruch (Thesis advisor) / Campbell, Andrew (Committee member) / Norton, Kay (Committee member) / Pagano, Caio (Committee member) / Ryan, Russell (Committee member) / Arizona State University (Publisher)
Created2013
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Description
The repertoire of the saxophone has advanced significantly since its invention circa 1840. Performers are required to adapt to the demands of composers - many of whom are exploring new and unconventional sounds and techniques. Numerous texts exist to identify and explain these so-called "extended" techniques, but there are very

The repertoire of the saxophone has advanced significantly since its invention circa 1840. Performers are required to adapt to the demands of composers - many of whom are exploring new and unconventional sounds and techniques. Numerous texts exist to identify and explain these so-called "extended" techniques, but there are very few resources for the initial stages of performance. In order to offer performers a resource, the author of this text composed forty original etudes (or studies) that incorporate extended techniques in a variety of ways. After identifying common extended techniques that a performer might face, the author focused on four different ways each individual technique might appear in actual repertoire. The resulting work is entitled Pushing Boundaries: Forty Etudes on Extended Techniques. Each etude offers a practical approach to what is generally a single extended technique. Although this text is not pedagogical in the sense of identifying the mechanics and anatomical requirements of each technique, it does contain a performance analysis of each etude. This analysis identifies areas where performers might struggle and offers helpful suggestions. To this end, the etudes accompanied by performance analysis provide a paced, systematic approach to the mastery of each technique.
ContributorsMurphy, Patrick Joseph (Author) / Hill, Gary (Thesis advisor) / Spring, Robert (Committee member) / McAllister, Timothy (Committee member) / Micklich, Albie (Committee member) / DeMars, James (Committee member) / Arizona State University (Publisher)
Created2013
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Description
Digital sound synthesis allows the creation of a great variety of sounds. Focusing on interesting or ecologically valid sounds for music, simulation, aesthetics, or other purposes limits the otherwise vast digital audio palette. Tools for creating such sounds vary from arbitrary methods of altering recordings to precise simulations of vibrating

Digital sound synthesis allows the creation of a great variety of sounds. Focusing on interesting or ecologically valid sounds for music, simulation, aesthetics, or other purposes limits the otherwise vast digital audio palette. Tools for creating such sounds vary from arbitrary methods of altering recordings to precise simulations of vibrating objects. In this work, methods of sound synthesis by re-sonification are considered. Re-sonification, herein, refers to the general process of analyzing, possibly transforming, and resynthesizing or reusing recorded sounds in meaningful ways, to convey information. Applied to soundscapes, re-sonification is presented as a means of conveying activity within an environment. Applied to the sounds of objects, this work examines modeling the perception of objects as well as their physical properties and the ability to simulate interactive events with such objects. To create soundscapes to re-sonify geographic environments, a method of automated soundscape design is presented. Using recorded sounds that are classified based on acoustic, social, semantic, and geographic information, this method produces stochastically generated soundscapes to re-sonify selected geographic areas. Drawing on prior knowledge, local sounds and those deemed similar comprise a locale's soundscape. In the context of re-sonifying events, this work examines processes for modeling and estimating the excitations of sounding objects. These include plucking, striking, rubbing, and any interaction that imparts energy into a system, affecting the resultant sound. A method of estimating a linear system's input, constrained to a signal-subspace, is presented and applied toward improving the estimation of percussive excitations for re-sonification. To work toward robust recording-based modeling and re-sonification of objects, new implementations of banded waveguide (BWG) models are proposed for object modeling and sound synthesis. Previous implementations of BWGs use arbitrary model parameters and may produce a range of simulations that do not match digital waveguide or modal models of the same design. Subject to linear excitations, some models proposed here behave identically to other equivalently designed physical models. Under nonlinear interactions, such as bowing, many of the proposed implementations exhibit improvements in the attack characteristics of synthesized sounds.
ContributorsFink, Alex M (Author) / Spanias, Andreas S (Thesis advisor) / Cook, Perry R. (Committee member) / Turaga, Pavan (Committee member) / Tsakalis, Konstantinos (Committee member) / Arizona State University (Publisher)
Created2013
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Description
This project sheds light on trombonist Andy Martin's improvisation and provides tools for further learning. A biographical sketch gives background on Martin, establishing him as a newer jazz master. Through the transcription and analysis of nine improvised solos, Martin's improvisational voice and vocabulary is deciphered and presented as a series

This project sheds light on trombonist Andy Martin's improvisation and provides tools for further learning. A biographical sketch gives background on Martin, establishing him as a newer jazz master. Through the transcription and analysis of nine improvised solos, Martin's improvisational voice and vocabulary is deciphered and presented as a series of seven thematic hooks. These patterns, rhythms, and gestures are described, analyzed, and presented as examples of how each is used in the solos. The hooks are also set as application exercises for learning jazz style and improvisation. These exercises demonstrate how to use Martin's hooks as a means for furthering one's own improvisation. A full method for successful transcription is also presented, along with the printed transcriptions and their accompanying information sheets.
ContributorsWilkinson, Michael Scott (Author) / Ericson, John (Thesis advisor) / Kocour, Michael (Committee member) / Solis, Theodore (Committee member) / Arizona State University (Publisher)
Created2013
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Description
Bright Summer, a one-movement piece for orchestra, was composed in Arizona, and completed in February 2013. The piece is approximately twelve minutes long. The motivation for writing this piece was the death of my mother the year before, in 2012. The prevailing mood of this work is bright and pleasant,

Bright Summer, a one-movement piece for orchestra, was composed in Arizona, and completed in February 2013. The piece is approximately twelve minutes long. The motivation for writing this piece was the death of my mother the year before, in 2012. The prevailing mood of this work is bright and pleasant, expressing my mother's cheerful personality when she was alive. It also portrays bright summer days which resemble my mother's spirit. Thus, soundscape plays an important role in this work. It depicts summer breeze, rustling sounds of leaves, and, to translate a Korean saying, "high blue skies." This soundscape opens the piece as well as closes it. In the middle section, the fast upbeat themes represent my mother's witty and optimistic personality. The piece also contains the presence of a hymn tune, The Love of God is Greater Far, which informs the motivic content and also functions as the climax of the piece. It was my mother's favorite hymn and we used to sing it together following her conversion to Christianity. The piece contains three main sections, which are held together by transitional material based on the soundscape and metric modulations. Unlike my earlier works, Bright Summer is tonal, with upper tertian harmonies prevailing throughout the piece. However, the opening and closing soundscapes do not have functional harmonies. For example, tertian chords appear and vanish silently, leaving behind some resonant sounds without any harmonic progression. Overall, the whole piece is reminiscent of my mother who lived a beautiful life.
ContributorsKim, JeeYeon (Composer) / DeMars, James (Thesis advisor) / Hackbarth, Glenn (Committee member) / Rogers, Rodney (Committee member) / Levy, Benjamin (Committee member) / Rockmaker, Jody (Committee member) / Arizona State University (Publisher)
Created2013
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Description
The thesis studies new methods to fabricate optoelectronic Ge1-ySny/Si(100) alloys and investigate their photoluminescence (PL) properties for possible applications in Si-based photonics including IR lasers. The work initially investigated the origin of the difference between the PL spectrum of bulk Ge, dominated by indirect gap emission, and the PL spectrum

The thesis studies new methods to fabricate optoelectronic Ge1-ySny/Si(100) alloys and investigate their photoluminescence (PL) properties for possible applications in Si-based photonics including IR lasers. The work initially investigated the origin of the difference between the PL spectrum of bulk Ge, dominated by indirect gap emission, and the PL spectrum of Ge-on-Si films, dominated by direct gap emission. It was found that the difference is due to the supression of self-absorption effects in Ge films, combined with a deviation from quasi-equilibrium conditions in the conduction band of undoped films. The latter is confirmed by a model suggesting that the deviation is caused by the shorter recombination lifetime in the films relative to bulk Ge. The knowledge acquired from this work was then utilized to study the PL properties of n-type Ge1-ySny/Si (y=0.004-0.04) samples grown via chemical vapor deposition of Ge2H6/SnD4/P(GeH3)3. It was found that the emission intensity (I) of these samples is at least 10x stronger than observed in un-doped counterparts and that the Idir/Iind ratio of direct over indirect gap emission increases for high-Sn contents due to the reduced gamma-L valley separation, as expected. Next the PL investigation was expanded to samples with y=0.05-0.09 grown via a new method using the more reactive Ge3H8 in place of Ge2H6. Optical quality, 1-um thick Ge1-ySny/Si(100) layers were produced using Ge3H10/SnD4 and found to exhibit strong, tunable PL near the threshold of the direct-indirect bandgap crossover. A byproduct of this study was the development of an enhanced process to produce Ge3H8, Ge4H10, and Ge5H12 analogs for application in ultra-low temperature deposition of Group-IV semiconductors. The thesis also studies synthesis routes of an entirely new class of semiconductor compounds and alloys described by Si5-2y(III-V)y (III=Al, V= As, P) comprising of specifically designed diamond-like structures based on a Si parent lattice incorporating isolated III-V units. The common theme of the two thesis topics is the development of new mono-crystalline materials on ubiquitous silicon platforms with the objective of enhancing the optoelectronic performance of Si and Ge semiconductors, potentially leading to the design of next generation optical devices including lasers, detectors and solar cells.
ContributorsGrzybowski, Gordon (Author) / Kouvetakis, John (Thesis advisor) / Chizmeshya, Andrew (Committee member) / Menéndez, Jose (Committee member) / Arizona State University (Publisher)
Created2013
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Description
Nitrate is the most prevalent water pollutant limiting the use of groundwater as a potable water source. The overarching goal of this dissertation was to leverage advances in nanotechnology to improve nitrate photocatalysis and transition treatment to the full-scale. The research objectives were to (1) examine commercial and synthesized photocatalysts,

Nitrate is the most prevalent water pollutant limiting the use of groundwater as a potable water source. The overarching goal of this dissertation was to leverage advances in nanotechnology to improve nitrate photocatalysis and transition treatment to the full-scale. The research objectives were to (1) examine commercial and synthesized photocatalysts, (2) determine the effect of water quality parameters (e.g., pH), (3) conduct responsible engineering by ensuring detection methods were in place for novel materials, and (4) develop a conceptual framework for designing nitrate-specific photocatalysts. The key issues for implementing photocatalysis for nitrate drinking water treatment were efficient nitrate removal at neutral pH and by-product selectivity toward nitrogen gases, rather than by-products that pose a human health concern (e.g., nitrite). Photocatalytic nitrate reduction was found to follow a series of proton-coupled electron transfers. The nitrate reduction rate was limited by the electron-hole recombination rate, and the addition of an electron donor (e.g., formate) was necessary to reduce the recombination rate and achieve efficient nitrate removal. Nano-sized photocatalysts with high surface areas mitigated the negative effects of competing aqueous anions. The key water quality parameter impacting by-product selectivity was pH. For pH < 4, the by-product selectivity was mostly N-gas with some NH4+, but this shifted to NO2- above pH = 4, which suggests the need for proton localization to move beyond NO2-. Co-catalysts that form a Schottky barrier, allowing for localization of electrons, were best for nitrate reduction. Silver was optimal in heterogeneous systems because of its ability to improve nitrate reduction activity and N-gas by-product selectivity, and graphene was optimal in two-electrode systems because of its ability to shuttle electrons to the working electrode. "Environmentally responsible use of nanomaterials" is to ensure that detection methods are in place for the nanomaterials tested. While methods exist for the metals and metal oxides examined, there are currently none for carbon nanotubes (CNTs) and graphene. Acknowledging that risk assessment encompasses dose-response and exposure, new analytical methods were developed for extracting and detecting CNTs and graphene in complex organic environmental (e.g., urban air) and biological matrices (e.g. rat lungs).
ContributorsDoudrick, Kyle (Author) / Westerhoff, Paul (Thesis advisor) / Halden, Rolf (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2013
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Description
The overall objective of this project is to optimize the development of magnetic ferrite thin films targeted for enabling low-loss broadband communication devices, miniaturized low-microwave inductors and electromagnetic noise suppressors. The focus of this objective is to design and build a reactor and improve the spin-spray process. Each film is

The overall objective of this project is to optimize the development of magnetic ferrite thin films targeted for enabling low-loss broadband communication devices, miniaturized low-microwave inductors and electromagnetic noise suppressors. The focus of this objective is to design and build a reactor and improve the spin-spray process. Each film is then characterized and optimized to have a high permeability and high frequency in the range of 500 MHz - 3 GHz. Films produced by the µ-droplet deposition regime yields a higher Snoek's product than the continuous liquid layer regime. The highest Snoek's product occurs when it is deposited at an oxidant pH of 8.28. The Ni-Zn-Co ferrite magnetic domains were imaged using the Lorentz TEM in which multi-grain domains are experimentally observed for the first time.
ContributorsRay, Nicole M (Author) / Petuskey, William T. (Thesis advisor) / Diaz, Rodolfo E. (Committee member) / Chamberlin, Ralph V. (Committee member) / Arizona State University (Publisher)
Created2013