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ItemDesign, synthesis, characterization and application of rare-earth doped glass and glass ceramic scintillators(Georgia Institute of Technology, 2019-11-08) Struebing, ChristianSingle crystal scintillators have been the premier choice for gamma ray detecting applications due to their high luminescent efficiency and sharp energy resolutions. However, there remain downsides to the use of single crystal scintillators such as production expense, vulnerability to environmental factors, and rigid shaping. Industries have been searching for lower cost alternatives to single crystal scintillators in order to make more portable devices practical. Glass and glass-ceramic scintillators have gained attention for their lower production cost, scalability, and ease of shaping to fit complex geometries. By the nature of the glass matrix any crystalline phases within the material are self-encapsulated, which avoids the issue of hygroscopicity and reduces the impact of mechanical shock and high temperature exposure. The main issue holding back glass and glass-ceramic scintillators has been the low luminescent efficiency stemming from the inherent disorder in the non-crystalline glassy matrix. We believe this downside can be mitigated through increases to density, harnessing the innate energy transfer capabilities of constituent materials, and controlled nucleation of crystalline phases within the glass structure. Glass-ceramics combine the robust resilience of glass with the luminescent capabilities of crystalline nanoparticles by precipitating nano-sized crystals within the glass matrix. This study approaches the field of glass and glass-ceramic based scintillators with rare-earth rich, high density compositions modeled after known crystal systems in order to produce a glass ceramic scintillator that could compete with single crystals.
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ItemDesign and fabrication of multilayer structures in dynamic sensing and transparent nanocomposite scintillators for high energy detection(Georgia Institute of Technology, 2017-04-05) Lee, GyuhyonThe development and exploitation of materials science, such as chemical synthesis, physical processes such as diffusion and transport, and the understanding of the thermodynamics that drives these processes are the foundation of new materials and material structures. For example, novel approaches in growth and processing techniques combined with an understanding of quantum effects have led to the development of quantum dots and nanoparticles with unique electronic and optoelectronic properties. Subsequently, new applications have emerged in the field of quantum dot electronics, energy storage systems, and optical communication devices. In the present study, we have extended the principles of chemical synthesis to the solid phase regime to achieve the formation of nanoparticles of scintillating materials (BaGdF₅ and GdF₃) in different solid glass matrices to form novel transparent nanocomposite scintillators. Judicious manipulation of materials choice and thermal processing to drive diffusion and control solubility in the liquid-solid space has resulted in the selection of the robust host glass matrix and the high energy radiation absorbing material (aluminosilicate glass as the host for BaGdF₅:Tb nanoparticles). These nanocomposite and similar material systems offer a new approach to achieve large area, low-cost and efficient scintillators. As a result, we have achieved 2.4 times improvement in light output under gamma-ray excitation. To further enhance efficiency, we have investigated technologies for patterning 2D photonic crystal structures into the surface of the scintillators to improve light out-coupling into a photomultiplier tube (PMT). The potential of this embodiment has been demonstrated and resulted in a completely different and new opportunity for dynamic load sensing. During the investigation of 2D photonic crystal structures for dynamic loading sensing, it has become apparent that linearly deposited multilayer (1D photonic crystal) structures offer the best solution; therefore, optical microcavity (OMC) and distributed Bragg reflector (DBR) multilayer structures have been examined in greater detail. From a deeper understanding of the interplay between the optical and acoustic properties, highly sensitive devices (Ag/Al₂O₃/SiO₂/Al₂O₃/Ag asymmetrical OMC (AOMC) and SiOx₁/SiOx₂ DBR structures) have been successfully developed and extensively characterized. At a relatively low applied shock pressure of ~4 GPa, both structures have exhibited spectral peak shifts of ~14-24 nm with response time <3 ns, limited only by the acoustic properties of the optically active material. These devices demonstrate the unique attributes of high sensitivity to shock pressure, ultra- fast response and with the additional potential for 2D imaging which can further widen the understanding of materials behavior under extreme conditions.
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ItemNanocomposite glass-ceramic scintillators for radiation spectroscopy(Georgia Institute of Technology, 2012-10-24) Barta, Meredith BrookeIn recent years, the United States Departments of Homeland Security (DHS) and Customs and Border Protection (CBP) have been charged with the task of scanning every cargo container crossing domestic borders for illicit radioactive material. This is accomplished by using gamma-ray detection systems capable of discriminating between non-threatening radioisotopes, such as Cs-137, which is often used in nuclear medicine, and fissile material, such as U-238, that can be used to make nuclear weapons or "dirty" bombs. Scintillation detector systems, specifically thallium-doped sodium iodide (NaI(Tl)) single crystals, are by far the most popular choice for this purpose because they are inexpensive relative to other types of detectors, but are still able to identify isotopes with reasonable accuracy. However, increased demand for these systems has served as a catalyst for the research and development of new scintillator materials with potential to surpass NaI(Tl). The focus of a majority of recent scintillator materials research has centered on sintered transparent ceramics, phosphor-doped organic matrices, and the development of novel single crystal compositions. Some of the most promising new materials are glass-ceramic nanocomposites. By precipitating a dense array of nano-scale scintillating crystals rather than growing a single monolith, novel compositions such as LaBr₃(Ce) may be fabricated to useful sizes, and their potential to supersede the energy resolution of NaI(Tl) can be fully explored. Also, because glass-ceramic synthesis begins by casting a homogeneous glass melt, a broad range of geometries beyond the ubiquitous cylinder can be fabricated and characterized. Finally, the glass matrix ensures environmental isolation of the hygroscopic scintillating crystals, and so glass-ceramic scintillators show potential to serve as viable detectors in alpha- and neutron-spectroscopy in addition to gamma-rays. However, for the improvements promised by glass-ceramics to become reality, several material properties must be considered. These include the degree of control over precipitated crystallite size, the solubility limit of the glass matrix with respect to the scintillating compounds, the variation in maximum achievable light yield with composition, and the peak wavelength of emitted photons. Studies will focus on three base glass systems, sodium-aluminosilicate (NAS), sodium-borosilicate (NBS), and alumino-borosilicate (ABS), into which a cerium-doped gadolinium bromide (GdBr₃(Ce)) scintillating phase will be incorporated. Scintillator volumes of 50 cubic centimeters or greater will be fabricated to facilitate comparison with NaI(Tl) crystals currently available.
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ItemOptical properties of the square superlattice photonic crystal structure and optical invisibility cloaking(Georgia Institute of Technology, 2010-08-27) Blair, John L.The refraction properties of photonic crystal lattices offers methods to control the beam steering of light through use of non-linear dispersion contours. In this thesis new photonic crystal structures, such as the square and triangular superlattices, that provide novel refractive properties are analyzed. The property difference between rows in these structures is the hole radius Δr. The difference in hole sizes leads to observation of the superlattice effect, that is, a change in the refractive index Δn between opposite rows of holes. The index difference becomes a function of the size of the smaller r2 hole area or volume due to the addition of the higher index background material compared to the larger r1 holes. The difference in hole radii Δr = r1 - r2 is referred to as the static superlattice strength and is designated by the ratio of r2/r1. The superlattice strength increases as the ratio of r2/r1 decreases. The hole size modulation creates modified dispersion contours that can be used to fabricate advanced beam steering devices through the introduction of electro-optical materials and a controlled bias. A discussion of these superlattice structures and their optical properties will be covered, followed by both static and dynamic tunable device constructions utilizing these designs. Also, static tuning of the devices through the use of atomic layer deposition, as well as active tuning methods utilizing liquid crystal (LC) infiltration, sealed LC cells, and the addition of electro-optic material will be discussed. Also in this thesis we present designs to implement a simpler demonstration of cloaking, the carpet cloak, in which a curved reflective surface is compressed into a flat reflective surface, effectively shielding objects behind the curve from view with respect to the incoming radiation source. This approach eliminates the need for metallic resonant elements. These structures can now be fabricated using only high index dielectric materials by the use of electron beam lithography and standard cleanroom technologies. The design method, simulation analysis, device fabrication, and near field optical microscopy (NSOM) characterization results are presented for devices designed to operate in the 1400-1600nm wavelength range. Improvements to device performance by the deposition/infiltration of linear, and potentially non-linear optical materials, were investigated.
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ItemA colloidal nanoparticle form of indium tin oxide: system development and characterization(Georgia Institute of Technology, 2009-04-06) Gilstrap, Richard Allen, Jr.A logical progression from the maturing field of colloidal semiconductor quantum dots to the emerging subclass of impurity-doped colloidal semiconductor nanoparticles is underway. To this end, the present work describes the formation and analysis of a new form of Tin-doped Indium Oxide (ITO). The form is that of a colloidal dispersion comprised of pure-phase, 4-6 nanometer ITO particles possessing an essentially single crystalline character. This system forms a non-agglomerated, optically clear solution in a variety of non-polar solvents and can remain in this state, at room temperature, for months and potentially, years. ITO is the most widely used member of the exotic materials family known as Transparent Conductive Oxides (TCOs) and is the primary enabling material behind a wide variety of opto-electronic device technologies. Material synthesis was achieved by initiating a series of interrelated nucleophilic substitution reactions that provided sufficient intensity to promote doping efficiencies greater than 90% for a wide range of tin concentrations. The optical clarity of this colloidal system allowed the intrinsic properties of single crystalline ITO particles to be evaluated prior to their use in thin-films or composite structures. Monitoring the temporal progression of n-type degeneracy by its effects on the optical properties of colloidal dispersions shed light on the fundamental issues of particle formation, band filling (Burstein-Moss) dynamics, and the very origin of n-type degeneracy in ITO. Central to these studies was the issue of excess electron character. The two limiting cases of entirely free and entirely confined electron motion were evaluated by application of bulk-like band dispersion analysis and the effective mass approximation, respectively. This provided a means to estimate the number of excess conduction band electrons present within an individual particle boundary. The ability to control and optimize the level of n-type degeneracy within the colloidal ITO nanoparticle form by compositional variation was also demonstrated. A key to the widespread adoption of a new material by industry is an ability to produce multi-gram and perhaps, kilogram quantities with no significant sacrifice in quality. Accordingly, a modified synthesis process was developed to allow for the mass production of high-quality colloidal ITO nanocrystals.
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ItemOptical Properties of Complex Periodic Media Structurally Modified by Atomic Layer Deposition(Georgia Institute of Technology, 2007-03-21) Gaillot, Davy PaulIn the late eighties, a new class of materials, known as photonic crystals (PCs), emerged enabling the propagation and generation of light to be potentially manipulated with unprecedented control. PCs consist of a periodic modulation of dielectric constant in one, two, or three dimensions, which can result in the formation of directional or omni-directional photonic band gaps (PBGs), spectral regions where light propagation is forbidden, and more remarkably, novel dispersion characteristics. Since PC properties scale with the dimension of the wavelength of interest, significant technological constraints must be fully addressed to manufacture 3D PBG materials for optical or infrared applications such as displays, lightning, and communications. PCs enable the unraveling of unique optical phenomena such as PBGs, spontaneous emission rate manipulation, sub-wavelength focusing, and superprism effects. This research focuses on the feasibility to achieve omni-directional PBGs in synthetic opal-based 3D PCs through precise nanoscale control to the original dielectric architecture. In particular, the optical response to the conformal deposition of dielectric layers using atomic layer deposition (ALD) within the porous template is strongly emphasized. Geometrical models were developed to faithfully model the manipulation of the synthetic opal architecture by ALD and then used in electromagnetic algorithms to predict the resulting optical properties. From these results, this research presents and investigates a scheme used to greatly enhance and adjust the PBG width and position, as well as simultaneously reducing the dielectric contrast threshold at which the PBG forms. This Thesis demonstrates that the unique opal architectures offered by ALD not only supports the formation of larger PBGs with high index materials; but also enables the use of optically transparent materials with reduced refractive index. Additionally, slight alteration of these structures facilitates the incorporation of non-linear (NL) electro-optical (EO) material for dynamic tuning capabilities and potentially offers a pathway for fabricating multi-functional photonic devices. Finally, low-temperature ALD was investigated as a means to manipulate band gaps and dispersion effects in 2D PC silicon slab waveguides and 3D organic biologically-derived templates. The results indicate the unique ability of ALD to achieve composite structures with desirable (large PBGs) or novel (slow light) optical properties.
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ItemSynthesis, Characterization and Application of Luminescent Quantum Dots and Microcrystalline Phosphors(Georgia Institute of Technology, 2006-11-20) Kang, ZhitaoSi QDs embedded in SiOx or SiNx thin films, which could emit light in the entire visible range from 440 nm to 840 nm by controlling their size and/or their matrix, were synthesized by evaporation or plasma enhanced chemical vapor deposition techniques. Various shades of white could be obtained from multi-layered SiNx film structures by controlling the size of Si QDs and layer thickness. It was shown that the combination of these films can produce white emission spectra with superior color rendering properties compared to conventional fluorescent tubes. Such Si-based QDs can be used as down-converting phosphors to coat a blue/UV LED to generate white light, providing a less expensive fabrication process to obtain advanced solid state lighting devices. As a supplement, free CdTe QDs with emission colors spanning 520~700 nm and quantum efficiency up to 54%, were synthesized using a colloidal chemical method for white LED applications. White PL and a range of emission colors were obtained from mixed CdTe QD samples excited by a 420 nm blue LED. Another part of this research was to develop a new x-ray powder phosphor, ZnTe:O, for biological imaging applications used in CCD-based synchrotron x-ray detectors. A unique dry synthesis process, including gaseous dry doping and etching procedures, was developed to synthesize ZnTe:O phosphors. The excellent x-ray luminescence results of oxygen doped ZnTe, including high efficiency, high resolution, fast decay, low afterglow and an improved spectral match to the CCD detector, indicated that ZnTe:O is a promising phosphor candidate for x-ray imaging applications.
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ItemLarge-Scale Patterned Oxide Nanostructures: Fabrication, Characterization and Applications(Georgia Institute of Technology, 2005-11-28) Wang, XudongNanotechnology is experiencing a flourishing development in a variety of fields covering all of the areas from science to engineering and to biology. As an active field in nanotechnology, the work presented in this dissertation is mostly focused on the fundamental study about the fabrication and assembly of functional oxide nanostructures. In particular, Zinc Oxide, one of the most important functional semiconducting materials, is the core objective of this research, from the controlled growth of nanoscale building blocks to understanding their properties and to how to organize these building blocks. Thermal evaporation process based on a single-zone tube furnace has been employed for synthesizing a range of 1D nanostructures. By controlling the experimental conditions, different morphologies, such as ultra-small ZnO nanobelts, mesoporous ZnO nanowires and core-shell nanowire were achieved. In order to pattern the nanostructures, a large-scale highly-ordered nanobowl structure based on the self-assembly of submicron spheres was created and utilized as patterning template. The growth and patterning techniques were thereafter integrated for aligning and patterning of ZnO nanowires. The aligning mechanisms and growth conditions were thoroughly studied so as to achieve a systematic control over the morphology, distribution and density. The related electronic and electromechanical properties of the aligned ZnO nanowires were investigated. The feasibility of some potential applications, such as photonic crystals, solar cells and sensor arrays, has also been studied. This research may set a foundation for many industrial applications from controlled synthesis to nanomanufacturing.
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ItemOptical Properties of Superlattice Photonic Crystals(Georgia Institute of Technology, 2005-09-22) Neff, Curtis WaynePhotonic band gap materials, commonly referred to as photonic crystals (PCs), have been a topic of great interest for almost two decades due to their promise of unprecedented control over the propagation and generation of light. We report investigations of the optical properties of a new PC structure based upon a triangular lattice in which adjacent [i, j] rows of holes possess different properties, creating a superlattice (SL) periodicity. Symmetry arguments predicted and quot;band folding and quot; and band splitting behaviors, both of which are direct consequences of the new basis that converts the Brillouin zone from hexagonal (six-fold) to rectangular (two-fold). Plane wave expansion and finite-difference time-domain (FDTD) numerical calculations were used to explore the effects of the new structure on the photonic dispersion relationship of the SL PC. Electron beam lithography and inductively coupled plasma dry etching were used to fabricate 1 mm2 PC areas (lattice constant, a =358 nm and 480 nm) with hole radius ratios ranging from 1.0 (triangular) to 0.585 (r2/r1 = 73.26 nm/125.26 nm) on Silicon-on-insulator wafers. The effects of modifying structural parameters (such as hole size, lattice constant, and SL strength) were measured using the coupled resonant band technique, confirming the SL symmetry arguments and corroborating the band structure calculations. Analysis of the dispersion contours of the static SL (SSL) PC predicted both giant refraction (change in beam propagation angle of 110 for an 8 change in incident angle) and superprism behavior (change in beam propagation angle of 108 for a 12% change in normalized frequency) in these structures. Dynamic control of these refraction effects was also investigated by incorporating electro-optic and nonlinear materials into the SSL PC structure. Wave vector analyses on these structures predicted a change in beam propagation angle and gt;96 when the refractive index inside of the holes of the structure changed from n=1.5 to 1.7. Through this investigation, the first successful measurement of the band folding effect in multidimensional PCs as well as the first explicit measurement of the dielectric band of a 2D PC were reported. In addition, the SL PCs impact on new opto-electronic devices was explored.
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ItemUnraveling photonic bands: characterization of self-collimation effects in two-dimensional photonic crystals(Georgia Institute of Technology, 2005-06-15) Yamashita, TsuyoshiPhotonic crystals, periodic dielectric structures that control photons in a similar way that atomic crystals control electrons, present opportunities for the unprecedented control of light. Photonic crystals display a wide gamut of properties, such as the photonic band gap, negative index of refraction, slow or stationary modes, and anomalous refraction and propagation effects. This thesis investigates the modeling, simulation, fabrication, and measurement of two-dimensional square lattice photonic crystals. An effective index model was developed to describe the propagation of electromagnetic waves in the media and applied to characterize the behavior of self-collimated beams to discern the effect of the photonic crystal on the evolution of the amplitude and phase of the propagating beam. Potential applications include optical interconnects and stand alone devices such as filters and lasers. Based on design parameters from the simulations, two dimensional photonic crystals were fabricated on amorphous and single crystal silicon-on-insulator substrates utilizing electron beam lithography and inductively coupled plasma etching. A unique etching process utilizing a combination of Cl2 and C4F6 gases was developed and characterized which displayed a vertical profile with a sidewall angle of under 1 degree from vertical and very smooth sidewalls for features as small as 150 nm. The high quality of the etching was the key to obtaining extremely low loss, low noise structures, making feasible the fabrication of large area photonic crystal devices that are necessary to measure propagation phenomena. Reflectivity measurements were used to directly observe the photonic band structure with excellent correlation with theory. A device was designed and fabricated which successfully verified the prediction of the simulations through measurements of the self-collimation effect across a broad range of infrared wavelengths. A solid foundation for the necessary components (simulation, modeling, design, fabrication, and measurement) of two-dimensional photonic crystal has been demonstrated. Elements from solid state physics, materials science, optics, and electromagnetics were incorporated to further the understanding of the mechanism of beam propagation in photonic crystals and illuminating the vast potential of research in periodic media.