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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, (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
Description
Rapid processing and reduced end-of-range diffusion effects demonstrate that susceptor-assisted microwave annealing is an efficient processing alternative for electrically activating dopants and removing ion-implantation damage in ion-implanted semiconductors. Sheet resistance and Hall measurements provide evidence of electrical activation. Raman spectroscopy and ion channeling analysis monitor the extent of ion implantation damage and recrystallization. The presence of damage and defects in ion implanted silicon, and the reduction of the defects as a result of annealing, is observed by Rutherford backscattering spectrometry, moreover, the boron implanted silicon is further investigated by cross-section transmission electron microscopy. When annealing B+ implanted silicon, the dissolution of small extended defects and growth of large extended defects result in reduced crystalline quality that hinders the electrical activation process. Compared to B+ implanted silicon, phosphorus implanted samples experience more effective activation and achieve better crystalline quality. Comparison of end-of-range dopants diffusion resulting from microwave annealing and rapid thermal annealing (RTA) is done using secondary ion mass spectroscopy. Results from microwave annealed P+ implanted samples show that almost no diffusion occurs during time periods required for complete dopant activation and silicon recrystallization. The relative contributions to heating of the sample, by a SiC susceptor, and by Si self-heating in the microwave anneal, were also investigated. At first 20s, the main contributor to the sample's temperature rise is Si self-heating by microwave absorption.
ContributorsZhao, Zhao (Author) / Alford, Terry Lynn (Thesis advisor) / Theodore, David (Committee member) / Krause, Stephen (Committee member) / Arizona State University (Publisher)
Created2013
Description
Microwave (MW), thermal, and ultraviolet (UV) annealing were used to explore the response of Ag structures on a Ge-Se chalcogenide glass (ChG) thin film as flexible radiation sensors, and Te-Ti chalcogenide thin films as a material for diffusion barriers in microelectronics devices and processing of metallized Cu. Flexible resistive radiation sensors consisting of Ag electrodes on a Ge20Se80 ChG thin film and polyethylene naphthalate substrate were exposed to UV radiation. The sensors were mounted on PVC tubes of varying radii to induce bending strains and annealed under ambient conditions up to 150 oC. Initial sensor resistance was measured to be ~1012 Ω; after exposure to UV radiation, the resistance was ~104 Ω. Bending strain and low temperature annealing had no significant effect on the resistance of the sensors. Samples of Cu on Te-Ti thin films were annealed in vacuum for up to 30 minutes and were stable up to 500 oC as revealed using Rutherford backscattering spectrometry (RBS) and four-point-probe analysis. X-ray diffractometry (XRD) indicates Cu grain growth up to 500 oC and phase instability of the Te-Ti barrier at 600 oC. MW processing was performed in a 2.45-GHz microwave cavity on Cu/Te-Ti films for up to 30 seconds to induce oxide growth. Using a calibrated pyrometer above the sample, the temperature of the MW process was measured to be below a maximum of 186 oC. Four-point-probe analysis shows an increase in resistance with an increase in MW time. XRD indicates growth of CuO on the sample surface. RBS suggests oxidation throughout the Te-Ti film. Additional samples were exposed to 907 J/cm2 UV radiation in order to ensure other possible electromagnetically induced mechanisms were not active. There were no changes observed using XRD, RBS or four point probing.
ContributorsRoos, Benjamin, 1990- (Author) / Alford, Terry L. (Thesis advisor) / Theodore, David (Committee member) / Kozicki, Michael (Committee member) / Arizona State University (Publisher)
Created2013
Description
There has been much interest in photoelectrochemical conversion of solar energy in recent years due to its potential for low-–cost, sustainable and renewable production of fuels. Despite the huge potential, there are still a number of technical barriers due to the many constraints needed in order to drive photoelectrochemical reactions such as overall water splitting and the identification of efficient and effective semiconductor materials. To this end, the search for novel semiconductors that can act as light absorbers is still needed. The copper hydroxyphosphate mineral libethenite (CHP), which has a chemical formula of Cu2(OH)PO4, has been recently shown to be active for photocatalytic degradation of methylene blue under UV-–irradiation, indicating that photo-excited electrons and holes can effectively be generated and separated in this material. However, CHP has not been well studied and many of its fundamental electrochemical and photoelectrochemical properties are still unknown. In this work, the synthesis of different morphologies of CHP using hydrothermal synthesis and precipitation methods were explored. Additionally, a preliminary investigation of the relevant fundamental characteristics such as the bandgap, flatband potential, band diagram, electrochemical and photoelectrochemical properties for CHP was performed. Better understanding of the properties of this material may lead to the development of improved catalysts and photocatalysts from natural sources.
ContributorsLi, Man (Author) / Chan, Candace K. (Thesis advisor) / O'Connell, Michael (Committee member) / Crozier, Peter (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
Description
In an effort to understand and improve interactions between homeless young adults and the nonprofit organizations that serve them, I engaged in a long-term, qualitative, participatory action project. My project involved input from homeless young adults, nonprofit organizations, volunteers/staff, and communication scholarship. While taking a community-engaged, participatory, and qualitative approach, I focused on the interactions between youth and the organizations. Particularly, I drew on homeless young adult experiences to inform services and illuminate compassion within the context of the nonprofit organizations. In the end, this project extends the individual model of compassion to include presence, identifies potential ruptures in the process of compassion, and models compassionate dynamics in organizations. It also articulates a method I call pragmatic fieldwork, a qualitative and pragmatic approach to participatory action research. Each of these outcomes speaks to varied community interests, from theoretically nuancing scholarly models of compassion to informing policy in the interest of more effectively and compassionately serving homeless youth.
ContributorsHuffman, Timothy (Author) / Trethewey, Angela (Thesis advisor) / Tracy, Sarah J. (Committee member) / Hagar, Mark (Committee member) / Arizona State University (Publisher)
Created2013
Description
Integrated photonics requires high gain optical materials in the telecom wavelength range for optical amplifiers and coherent light sources. Erbium (Er) containing materials are ideal candidates due to the 1.5 μm emission from Er3+ ions. However, the Er density in typical Er-doped materials is less than 1 x 1020 cm-3, thus limiting the maximum optical gain to a few dB/cm, too small to be useful for integrated photonics applications. Er compounds could potentially solve this problem since they contain much higher Er density. So far the existing Er compounds suffer from short lifetime and strong upconversion effects, mainly due to poor quality of crystals produced by various methods of thin film growth and deposition. This dissertation explores a new Er compound: erbium chloride silicate (ECS, Er3(SiO4)2Cl ) in the nanowire form, which facilitates the growth of high quality single crystals. Growth methods for such single crystal ECS nanowires have been established. Various structural and optical characterizations have been carried out. The high crystal quality of ECS material leads to a long lifetime of the first excited state of Er3+ ions up to 1 ms at Er density higher than 1022 cm-3. This Er lifetime-density product was found to be the largest among all Er containing materials. A unique integrating sphere method was developed to measure the absorption cross section of ECS nanowires from 440 to 1580 nm. Pump-probe experiments demonstrated a 644 dB/cm signal enhancement from a single ECS wire. It was estimated that such large signal enhancement can overcome the absorption to result in a net material gain, but not sufficient to compensate waveguide propagation loss. In order to suppress the upconversion process in ECS, Ytterbium (Yb) and Yttrium (Y) ions are introduced as substituent ions of Er in the ECS crystal structure to reduce Er density. While the addition of Yb ions only partially succeeded, erbium yttrium chloride silicate (EYCS) with controllable Er density was synthesized successfully. EYCS with 30 at. % Er was found to be the best. It shows the strongest PL emission at 1.5 μm, and thus can be potentially used as a high gain material.
ContributorsYin, Leijun (Author) / Ning, Cun-Zheng (Thesis advisor) / Chamberlin, Ralph (Committee member) / Yu, Hongbin (Committee member) / Menéndez, Jose (Committee member) / Ponce, Fernando (Committee member) / Arizona State University (Publisher)
Created2013
Description
Microwave dielectrics are widely used to make resonators and filters in telecommunication systems. The production of thin films with high dielectric constant and low loss could potentially enable a marked reduction in the size of devices and systems. However, studies of these materials in thin film form are very sparse. In this research, experiments were carried out on practical high-performance dielectrics including ZrTiO4-ZnNb2O6 (ZTZN) and Ba(Co,Zn)1/3Nb2/3O3 (BCZN) with high dielectric constant and low loss tangent. Thin films were deposited by laser ablation on various substrates, with a systematical study of growth conditions like substrate temperature, oxygen pressure and annealing to optimize the film quality, and the compositional, microstructural, optical and electric properties were characterized. The deposited ZTZN films were randomly oriented polycrystalline on Si substrate and textured on MgO substrate with a tetragonal lattice change at elevated temperature. The BCZN films deposited on MgO substrate showed superior film quality relative to that on other substrates, which grow epitaxially with an orientation of (001) // MgO (001) and (100) // MgO (100) when substrate temperature was above 500 oC. In-situ annealing at growth temperature in 200 mTorr oxygen pressure was found to enhance the quality of the films, reducing the peak width of the X-ray Diffraction (XRD) rocking curve to 0.53o and the χmin of channeling Rutherford Backscattering Spectrometry (RBS) to 8.8% when grown at 800oC. Atomic Force Microscopy (AFM) was used to study the topography and found a monotonic decrease in the surface roughness when the growth temperature increased. Optical absorption and transmission measurements were used to determine the energy bandgap and the refractive index respectively. A low-frequency dielectric constant of 34 was measured using a planar interdigital measurement structure. The resistivity of the film is ~3×1010 ohm·cm at room temperature and has an activation energy of thermal activated current of 0.66 eV.
ContributorsLi, You (Author) / Newman, Nathan (Thesis advisor) / Alford, Terry (Committee member) / Singh, Rakesh (Committee member) / Arizona State University (Publisher)
Created2013
Description
This research emphasizes the use of low energy and low temperature post processing to improve the performance and lifetime of thin films and thin film transistors, by applying the fundamentals of interaction of materials with conductive heating and electromagnetic radiation. Single frequency microwave anneal is used to rapidly recrystallize the damage induced during ion implantation in Si substrates. Volumetric heating of the sample in the presence of the microwave field facilitates quick absorption of radiation to promote recrystallization at the amorphous-crystalline interface, apart from electrical activation of the dopants due to relocation to the substitutional sites. Structural and electrical characterization confirm recrystallization of heavily implanted Si within 40 seconds anneal time with minimum dopant diffusion compared to rapid thermal annealed samples. The use of microwave anneal to improve performance of multilayer thin film devices, e.g. thin film transistors (TFTs) requires extensive study of interaction of individual layers with electromagnetic radiation. This issue has been addressed by developing detail understanding of thin films and interfaces in TFTs by studying reliability and failure mechanisms upon extensive stress test. Electrical and ambient stresses such as illumination, thermal, and mechanical stresses are inflicted on the mixed oxide based thin film transistors, which are explored due to high mobilities of the mixed oxide (indium zinc oxide, indium gallium zinc oxide) channel layer material. Semiconductor parameter analyzer is employed to extract transfer characteristics, useful to derive mobility, subthreshold, and threshold voltage parameters of the transistors. Low temperature post processing anneals compatible with polymer substrates are performed in several ambients (oxygen, forming gas and vacuum) at 150 °C as a preliminary step. The analysis of the results pre and post low temperature anneals using device physics fundamentals assists in categorizing defects leading to failure/degradation as: oxygen vacancies, thermally activated defects within the bandgap, channel-dielectric interface defects, and acceptor-like or donor-like trap states. Microwave anneal has been confirmed to enhance the quality of thin films, however future work entails extending the use of electromagnetic radiation in controlled ambient to facilitate quick post fabrication anneal to improve the functionality and lifetime of these low temperature fabricated TFTs.
ContributorsVemuri, Rajitha (Author) / Alford, Terry L. (Thesis advisor) / Theodore, N David (Committee member) / Goryll, Michael (Committee member) / Arizona State University (Publisher)
Created2013
Description
The purpose of this dissertation was to develop a Compassionate Communication Scale (CCS) by conducting a series of studies. The first study used qualitative data to identify and develop initial scale items. A series of follow-up studies used exploratory factor analysis to investigate the underlying structure of the CCS. A three-factor structure emerged, which included: Compassionate conversation, such as listening, letting the distressed person disclose feelings, and making empathetic remarks; compassionate touch, such as holding someone's hand or patting someone's back; and compassionate messaging, such as posting an encouraging message on a social networking site or sending a sympathetic email. The next study tested convergent and divergent validity by determining how the three forms of compassionate communication associate with various traits. Compassionate conversation was positively related to compassion, empathetic concern, perspective taking, emotional intelligence, social expressivity, emotional expressivity and benevolence, and negatively related to verbal aggressiveness and narcissism. Compassionate touch was positively correlated with compassion, empathetic concern, perspective taking, emotional intelligence, social expressivity, emotional expressivity, and benevolence, and uncorrelated with verbal aggressiveness and benevolence. Finally, compassionate messaging was positively correlated with social expressivity, emotional expressivity, and uncorrelated with verbal aggressiveness and narcissism. The next study focused on cross-validation and criterion-related validity. Correlations showing that self-reports of a person's compassionate communication were positively related to a friend or romantic partner's report of that person's compassionate communication provided cross-validation. The test for criterion-related validity examined whether compassionate communication predicts relational satisfaction. Regression analyses revealed that people were more relationally satisfied when they perceived themselves to use compassionate conversation, when they perceived their partner to use compassionate conversation, and when their partner reported using compassionate conversation. This finding did not extend to compassionate touch or compassionate messaging. In fact, in one regression analysis, people reported more relational satisfaction when they perceived that their partners used high levels of compassionate conversation and low levels of compassionate touch. Overall, the analyses suggest that of the three forms of compassionate communication, compassionate conversation is most strongly related to relational satisfaction. Taken together, this series of studies provides initial evidence for the validity of the CCS.
ContributorsRamos Salazar, Leslie (Author) / Guerrero, Laura (Thesis advisor) / Roberto, Anthony (Committee member) / Millsap, Roger (Committee member) / Arizona State University (Publisher)
Created2013