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Description
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
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 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
ContributorsShi, Ge (Performer) / ASU Library. Music Library (Publisher)
Created2018-03-25
ContributorsShatuho, Kristina (Performer) / ASU Library. Music Library (Publisher)
Created2018-03-27
Description
Organic light emitting diodes (OLEDs) is a rapidly emerging technology based on organic thin film semiconductors. Recently, there has been substantial investment in their use in displays. In less than a decade, OLEDs have grown from a promising academic curiosity into a multi-billion dollar global industry. At the heart of an OLED are emissive molecules that generate light in response to electrical stimulation. Ideal emitters are efficient, compatible with existing materials, long lived, and produce light predominantly at useful wavelengths. Developing an understanding of the photophysical processes that dictate the luminescent properties of emissive materials is vital to their continued development. Chapter 1 and Chapter 2 provide an introduction to the topics presented and the laboratory methods used to explore them. Chapter 3 discusses a series of tridentate platinum complexes. A synthetic method utilizing microwave irradiation was explored, as well as a study of the effects ligand structure had on the excited state properties. Results and techniques developed in this endeavor were used as a foundation for the work undertaken in later chapters. Chapter 4 introduces a series of tetradentate platinum complexes that share a phenoxy-pyridyl (popy) motif. The new molecular design improved efficiency through increased rigidity and modification of the excited state properties. This class of platinum complexes were markedly more efficient than those presented in Chapter 3, and devices employing a green emitting complex of the series achieved nearly 100% electron-to-photon conversion efficiency in an OLED device. Chapter 5 adapts the ligand structure developed in Chapter 4 to palladium. The resulting complexes exceed reported efficiencies of palladium complexes by an order of magnitude. This chapter also provides the first report of a palladium complex as an emitter in an OLED device. Chapter 6 discusses the continuation of development efforts to include carbazolyl components in the ligand. These complexes possess interesting luminescent properties including ultra-narrow emission and metal assisted delayed fluorescence (MADF) emission.
ContributorsTurner, Eric (Author) / Li, Jian (Thesis advisor) / Adams, James (Committee member) / Alford, Terry (Committee member) / Arizona State University (Publisher)
Created2014
Description
Redox reactions are crucial to energy transduction in biology. Protein film electrochemistry (PFE) is a technique for studying redox proteins in which the protein is immobilized at an electrode surface so as to allow direct exchange of electrons. Establishing a direct electronic connection eliminates the need for redoxactive mediators, thus allowing for interrogation of the redox protein of interest. PFE has proven a versatile tool that has been used to elucidate the properties of many technologically relevant redox proteins including hydrogenases, laccases, and glucose oxidase.
This dissertation is comprised of two parts: extension of PFE to a novel electrode material and application of PFE to the investigation of a new type of hydrogenase. In the first part, mesoporous antimony-doped tin oxide (ATO) is employed for the first time as an electrode material for protein film electrochemistry. Taking advantage of the excellent optical transparency of ATO, spectroelectrochemistry of cytochrome c is demonstrated. The electrochemical and spectroscopic properties of the protein are analogous to those measured for the native protein in solution, and the immobilized protein is stable for weeks at high loadings. In the second part, PFE is used to characterize the catalytic properties of the soluble hydrogenase I from Pyrococcus furiosus (PfSHI). Since this protein is highly thermostable, the temperature dependence of catalytic properties was investigated. I show that the preference of the enzyme for reduction of protons (as opposed to oxidation of hydrogen) and the reactions with oxygen are highly dependent on temperature, and the enzyme is tolerant to oxygen during both oxidative and reductive catalysis.
This dissertation is comprised of two parts: extension of PFE to a novel electrode material and application of PFE to the investigation of a new type of hydrogenase. In the first part, mesoporous antimony-doped tin oxide (ATO) is employed for the first time as an electrode material for protein film electrochemistry. Taking advantage of the excellent optical transparency of ATO, spectroelectrochemistry of cytochrome c is demonstrated. The electrochemical and spectroscopic properties of the protein are analogous to those measured for the native protein in solution, and the immobilized protein is stable for weeks at high loadings. In the second part, PFE is used to characterize the catalytic properties of the soluble hydrogenase I from Pyrococcus furiosus (PfSHI). Since this protein is highly thermostable, the temperature dependence of catalytic properties was investigated. I show that the preference of the enzyme for reduction of protons (as opposed to oxidation of hydrogen) and the reactions with oxygen are highly dependent on temperature, and the enzyme is tolerant to oxygen during both oxidative and reductive catalysis.
ContributorsKwan, Patrick Karchung (Author) / Jones, Anne K (Thesis advisor) / Francisco, Wilson (Committee member) / Moore, Thomas (Committee member) / Arizona State University (Publisher)
Created2014
ContributorsCarlisi, Daniel (Performer) / ASU Library. Music Library (Publisher)
Created2018-04-07
Description
Yannis Constantinidis was the last of the handful of composers referred to collectively as the Greek National School. The members of this group strove to create a distinctive national style for Greece, founded upon a synthesis of Western compositional idioms with melodic, rhyhmic, and modal features of their local folk traditions. Constantinidis particularly looked to the folk melodies of his native Asia Minor and the nearby Dodecanese Islands. His musical output includes operettas, musical comedies, orchestral works, chamber and vocal music, and much piano music, all of which draws upon folk repertories for thematic material. The present essay examines how he incorporates this thematic material in his piano compositions, written between 1943 and 1971, with a special focus on the 22 Songs and Dances from the Dodecanese. In general, Constantinidis's pianistic style is expressed through miniature pieces in which the folk tunes are presented mostly intact, but embedded in accompaniment based in early twentieth-century modal harmony. Following the dictates of the founding members of the Greek National School, Manolis Kalomiris and Georgios Lambelet, the modal basis of his harmonic vocabulary is firmly rooted in the characteristics of the most common modes of Greek folk music. A close study of his 22 Songs and Dances from the Dodecanese not only offers a valuable insight into his harmonic imagination, but also demonstrates how he subtly adapts his source melodies. This work also reveals his care in creating a musical expression of the words of the original folk songs, even in purely instrumental compositon.
ContributorsSavvidou, Dina (Author) / Hamilton, Robert (Thesis advisor) / Little, Bliss (Committee member) / Meir, Baruch (Committee member) / Thompson, Janice M (Committee member) / Arizona State University (Publisher)
Created2011
Description
This paper describes six representative works by twentieth-century Chinese composers: Jian-Zhong Wang, Er-Yao Lin, Yi-Qiang Sun, Pei-Xun Chen, Ying-Hai Li, and Yi Chen, which are recorded by the author on the CD. The six pieces selected for the CD all exemplify traits of Nationalism, with or without Western influences. Of the six works on the CD, two are transcriptions of the Han Chinese folk-like songs, one is a composition in the style of the Uyghur folk music, two are transcriptions of traditional Chinese instrumental music dating back to the eighteenth century, and one is an original composition in a contemporary style using folk materials. Two of the composers, who studied in the United States, were strongly influenced by Western compositional style. The other four, who did not study abroad, retained traditional Chinese style in their compositions. The pianistic level of difficulty in these six pieces varies from intermediate to advanced level. This paper includes biographical information for the six composers, background information on the compositions, and a brief analysis of each work. The author was exposed to these six pieces growing up, always believing that they are beautiful and deserve to be appreciated. When the author came to the United States for her studies, she realized that Chinese compositions, including these six pieces, were not sufficiently known to her peers. This recording and paper are offered in the hopes of promoting a wider familiarity with Chinese music and culture.
ContributorsLuo, Yali, D.M.A (Author) / Hamilton, Robert (Thesis advisor) / Campbell, Andrew (Committee member) / Pagano, Caio (Committee member) / Cosand, Walter (Committee member) / Rogers, Rodney (Committee member) / Arizona State University (Publisher)
Created2012
Description
The purpose of this project was to examine the lives and solo piano works of four members of the early generation of female composers in Taiwan. These four women were born between 1950 and 1960, began to appear on the Taiwanese musical scene after 1980, and were still active as composers at the time of this study. They include Fan-Ling Su (b. 1955), Hwei-Lee Chang (b. 1956), Shyh-Ji Pan-Chew (b. 1957), and Kwang-I Ying (b. 1960). Detailed biographical information on the four composers is presented and discussed. In addition, the musical form and features of all solo piano works at all levels by the four composers are analyzed, and the musical characteristics of each composer's work are discussed. The biography of a fifth composer, Wei-Ho Dai (b. 1950), is also discussed but is placed in the Appendices because her piano music could not be located. This research paper is presented in six chapters: (1) Prologue; the life and music of (2) Fan-Ling Su, (3) Hwei-Lee Chang, (4) Shyh-Ji Pan-Chew, and (5) Kwang-I Ying; and (6) Conclusion. The Prologue provides an overview of the development of Western classical music in Taiwan, a review of extant literature on the selected composers and their music, and the development of piano music in Taiwan. The Conclusion is comprised of comparisons of the four composers' music, including their personal interests and preferences as exhibited in their music. For example, all of the composers have used atonality in their music. Two of the composers, Fan-Ling Su and Kwang-I Ying, openly apply Chinese elements in their piano works, while Hwei-Lee Chang tries to avoid direct use of the Chinese pentatonic scale. The piano works of Hwei-Lee Chang and Shyh-Ji Pan-Chew are chromatic and atonal, and show an economical usage of material. Biographical information on Wei-Ho Dai and an overview of Taiwanese history are presented in the Appendices.
ContributorsWang, Jinding (Author) / Pagano, Caio (Thesis advisor) / Campbell, Andrew (Committee member) / Humphreys, Jere T. (Committee member) / Meyer-Thompson, Janice (Committee member) / Norton, Kay (Committee member) / Arizona State University (Publisher)
Created2011