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Thin-film Lithium Niobate Photonics for Electro-optics, Nonlinear Optics, and Quantum Optics on Silicon
Title
Thin-film Lithium Niobate Photonics for Electro-optics, Nonlinear Optics, and Quantum Optics on Silicon.
Creator
Rao, Ashutosh, Fathpour, Sasan, Delfyett, Peter, Li, Guifang, Thomas, Jayan, University of Central Florida
Abstract / Description
Ion-sliced thin-film lithium niobate (LN) compact waveguide technology has facilitated the resurgence of integrated photonics based on lithium niobate. These thin-film LN waveguides offer over an order of magnitude improvement in optical confinement, and about two orders of magnitude reduction in waveguide bending radius, compared to conventional LN waveguides. Harnessing the improved confinement, a variety of miniaturized and efficient photonic devices are demonstrated in this work. First,...
Show moreIon-sliced thin-film lithium niobate (LN) compact waveguide technology has facilitated the resurgence of integrated photonics based on lithium niobate. These thin-film LN waveguides offer over an order of magnitude improvement in optical confinement, and about two orders of magnitude reduction in waveguide bending radius, compared to conventional LN waveguides. Harnessing the improved confinement, a variety of miniaturized and efficient photonic devices are demonstrated in this work. First, two types of compact electrooptic modulators are presented (-) microring modulators, and Mach-Zehnder modulators. Next, two distinct approaches to nonlinear optical frequency converters are implemented (-) periodically poled lithium niobate, and mode shape modulation (grating assisted quasi-phase matching). Following this, stochastic variations are added to the mode shape modulation approach to demonstrate random quasi-phase matching. Afterward, broadband photon-pair generation is demonstrated in the miniaturized periodically poled lithium niobate, and spectral correlations of the biphoton spectrum are reported. Finally, extensions of the aforementioned results suitable for future work are discussed.
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Date Issued
2018
Identifier
CFE0007085, ucf:52013
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0007085
A Theoretical Investigation of Small Organic Molecules on Transition Metal Surfaces
Title
A Theoretical Investigation of Small Organic Molecules on Transition Metal Surfaces.
Creator
Malone, Walter, Kara, Abdelkader, Stolbov, Sergey, Kaden, William, Thomas, Jayan, University of Central Florida
Abstract / Description
With the ever growing number of proposed desnity functional theory (DFT) functionals it becomes necessary to thoroughly screen any new method to determine its merit. Especially relevant methods include a proper description of the van der Waals (vdW) interaction, which can prove vital to a correct description of a myriad of systems of technological importance. The first part of this dissertation explores the utility of several vdW-inclusive DFT functionals including optB86b-vdW, optB88-vdW,...
Show moreWith the ever growing number of proposed desnity functional theory (DFT) functionals it becomes necessary to thoroughly screen any new method to determine its merit. Especially relevant methods include a proper description of the van der Waals (vdW) interaction, which can prove vital to a correct description of a myriad of systems of technological importance. The first part of this dissertation explores the utility of several vdW-inclusive DFT functionals including optB86b-vdW, optB88-vdW, optPBE-vdW, revPBE-vdW, rPW86-vdW2, and SCAN+rVV10 by applying them to model systems of small organic molecules, pyridine and thiophene, on transition metal surfaces. Overall, we find the optB88-vdW functional gives the best, most balanced description of both thiophene and pyridine on transition metal surfaces while revPBE-vdW, rPW86-vdW2, and SCAN+rVV10 functionals perform especially poorly for these systems. In the second part of this dissertation we change our focus to potential applications of DFT. Specifically, we study the hydrodesulfurization (HDS) process and molecules that could be used in molecular electronics. The removal of sulfur containing molecules from petrochemicals through HDS is an exceptionally important process economically, and the field of molecular electronics is rapidly developing with hopes of competing with and replacing their silicon analogues. First we investigate the hydrodesulfurization of thiophene. In this dissertation we manage to map the HDS rate of thiophene in realistic reaction conditions to the charge transfer and adsorption energy of thiophene on bare transition metal surfaces in hopes of predicting ever more active HDS catalysis. Finally we look at the adsorption of polythiophenes and 5,14-dihydro-5,7,12,14-tetraazapentacene (DHTAP) on Au(111) and Cu(110). We find that polythiophenes may dissociate of Au(111), presenting an issue for their use in molecular electronics. DHTAP, in contrast, proves to a suitable candidate for use practical devices.
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Date Issued
2019
Identifier
CFE0007494, ucf:52653
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0007494
Graphene Induced Formation of Nanostructures in Composites
Title
Graphene Induced Formation of Nanostructures in Composites.
Creator
Shen, Chen, Zhai, Lei, Chen, Quanfang, Thomas, Jayan, Fang, Jiyu, Khondaker, Saiful, University of Central Florida
Abstract / Description
Graphene induced nanostructures in graphene-based composites and the performance of these composites have been explored in this study. For the metallic nanoparticles decorated graphene aerogels composites, the fabrication of hierarchically structured, reduced graphene oxide (rGO) aerogels with heavily metallic nanoparticles was realized. Higher loading of palladium nanoparticles in graphene aerogels leads to improved hydrogen gas sensing performance. For polymer derived ceramics (PDCs)...
Show moreGraphene induced nanostructures in graphene-based composites and the performance of these composites have been explored in this study. For the metallic nanoparticles decorated graphene aerogels composites, the fabrication of hierarchically structured, reduced graphene oxide (rGO) aerogels with heavily metallic nanoparticles was realized. Higher loading of palladium nanoparticles in graphene aerogels leads to improved hydrogen gas sensing performance. For polymer derived ceramics (PDCs) composites with anisotropic electrical properties, the fabrication of composites was realized by embedding anisotropic reduced graphene oxide aerogels (rGOAs) into the PDCs matrix. Raman spectroscopy and X-ray diffraction studies of PDCs composites with and without graphene indicate that graphene facilitates the transition from amorphous carbon to graphitic carbon in the PDCs. For composites composed of PDCs and edge functionalized graphene oxide (EFGO), bulk PDCs based composites with embedded graphene networks show high electrical conductivity, high thermal stability, and low thermal conductivity. For the study of poly(3-hexylthiophene) (P3HT) crystallization on graphitic substrates (i.e. carbon nanotubes, carbon fibers and graphene), different types of P3HT nanocrystals (i.e. nanowires, nanoribbons, and nanowalls) were observed. The type of nanocrystals grown from graphitic substrates depends on the curvature of graphitic substrates, the molecular weight of P3HT molecules, and the concentration of P3HT marginal solutions. Besides, both specific surface area and curvature of graphitic substrates have major effects on P3HT crystallization processes.
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Date Issued
2018
Identifier
CFE0007095, ucf:51961
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0007095
nanoengineered energy harvesting and storage devices
Title
nanoengineered energy harvesting and storage devices.
Creator
Li, Chao, Thomas, Jayan, Zhai, Lei, Yang, Yang, Gesquiere, Andre, Dong, Yajie, Sun, Wei, University of Central Florida
Abstract / Description
Organic and perovskite solar cells have recently attracted significant attention due to itsflexibility, ease of fabrication and excellent performance. In order to realize even betterperformance for organic and perovskite solar cells, rejuvenated effort towards developingnanostructured electrodes and high quality active layer is necessary.In this dissertation, several strategic directions of enhancing the performance of organicand perovskite solar cells are investigated. An introduction and...
Show moreOrganic and perovskite solar cells have recently attracted significant attention due to itsflexibility, ease of fabrication and excellent performance. In order to realize even betterperformance for organic and perovskite solar cells, rejuvenated effort towards developingnanostructured electrodes and high quality active layer is necessary.In this dissertation, several strategic directions of enhancing the performance of organicand perovskite solar cells are investigated. An introduction and background of organic andperovskite solar cells, which includes motivation, classification and working principles,nanostructured electrode materials and solvent effect on active materials, and devices fabrication,are presented. A facile method, called Spin-on Nanoprinting (SNAP), to fabricate highly orderedZnO-AgNW-ZnO electrode is introduced to enhance the performance of organic solar cell.Subsequently, a ternary solvent method is developed to fabricate high Voc thieno[3,4-b]thiophene/benzodithiophene (PTB7) and indene-C60 bisadduct (ICBA)solar cells. Theperformance of the devices improved about 20% compared to those made by binary solventmethod. In order to understand the fundamental properties of the materials ruling theperformance of the PSCs tested, AFM-based nanoscale characterization techniques includingPulsed-Force-Mode AFM (PFM-AFM) and Mode-Synthesizing AFM (MSAFM) are introduced.These methods are used to study the morphology and physical properties of the structuresconstitutive of the active layers of the PSCs. Conductive-AFM (cAFM) studies reveal localvariations in conductivity in the donor and acceptor phases as well as an increase in photocurrentmeasured in the PTB7:ICBA sample obtained with the ternary solvent processing technique.Moreover, efficient perovskite solar cells with good transparency in the visible wavelength rangehave been developed by a facile and low-temperature PCBM-assisted perovskite growth method.This method results in the formation of perovskite-PCBM hybrid material at the grain boundaries which is observed by EELS mapping and confirmed by steady-state photoluminescence (PL)spectra and transient photocurrent (TP) measurements. This method involves fewer steps andtherefore is less expensive and time consuming than other reported methods. In addition, wereport an all solid state, energy harvesting and storing (ENHANS) filament which integratesperovskite solar cell (PSC) on top of a symmetric supercapacitor (SSC) via a copper filamentwhich works as a shared electrode for direct charge transfer. Developing ENHANS on a copperfilament provides a low-cost solution for flexible self-sufficient energy systems for wearablesand other portable devices. Finally, a summary of this dissertation as well as some potentialfuture directions are presented.
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Date Issued
2016
Identifier
CFE0006693, ucf:51912
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0006693
Nanoscale Spectroscopy in Energy and Catalytic Applications
Title
Nanoscale Spectroscopy in Energy and Catalytic Applications.
Creator
Ding, Yi, Tetard, Laurene, Challapalli, Suryanarayana, Zhai, Lei, Thomas, Jayan, Lyakh, Arkadiy, Blair, Richard, University of Central Florida
Abstract / Description
Emerging societal challenges such as the need for more sustainable energy and catalysis are requiring more sensitive and versatile measurements at the nanoscale. This is the case in the design and optimization of new materials for energy harvesting (solar cells) and energy storage devices (batteries and capacitors), or for the development of new catalysts for carbon sequestration or other reactions of interest. Hence, the ability to advance spectroscopy with nanoscale spatial resolution and...
Show moreEmerging societal challenges such as the need for more sustainable energy and catalysis are requiring more sensitive and versatile measurements at the nanoscale. This is the case in the design and optimization of new materials for energy harvesting (solar cells) and energy storage devices (batteries and capacitors), or for the development of new catalysts for carbon sequestration or other reactions of interest. Hence, the ability to advance spectroscopy with nanoscale spatial resolution and high sensitivity holds great promises to meet the demands of deeper fundamental understanding to boost the development and deployment of nano-based devices for real applications. In this dissertation, the impact of nanoscale characterization on energy-related and catalytic materials is considered. Firstly an introduction of the current energy and environmental challenges and our motivations are presented. We discuss how revealing nanoscale properties of solar cell active layers and supercapacitor electrodes can greatly benefit the performance of devices, and ponder on the advantages over conventional characterization techniques. Next, we focus on two dimensional materials as promising alternative catalysts to replace conventional noble metals for carbon sequestration and its conversion to added-value products. Defect-laden hexagonal boron nitride (h-BN) has been identified as a good catalyst candidate for carbon sequestration. Theoretically, defects exhibit favorable properties as reaction sites. However, the detailed mechanism pathways cannot be readily probed experimentally, due to the lack of tools with sufficient sensitivity and time resolution. A comprehensive study of the design and material processes used to introduce defects in h-BN in view of improving the catalytic properties is presented. The processing-structure-property relationships are investigated using a combination of conventional characterization and advanced nanoscale techniques. In addition to identifying favorable conditions for defect creation, we also report on the first signs of local reactions at defect sites obtained with nanoscale spectroscopy. Next, we explore avenues to improve the sensitivity and time-resolution of nanoscale measurements using light-assisted AFM-based nanomechanical spectroscopy. For each configuration, we evaluate the new system by comparing its performance to the commercial capabilities.Lastly, we provide a perspective on the opportunities for state-of-the-art characterization to impact the fields of catalysis and sustainable energy, as well as the urge for highly sensitive functional capabilities and time-resolution for nanoscale studies.
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Date Issued
2018
Identifier
CFE0007751, ucf:52387
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0007751
Nanoarchitectured Energy Storage Devices
Title
Nanoarchitectured Energy Storage Devices.
Creator
Yu, Zenan, Thomas, Jayan, Seal, Sudipta, Zhai, Lei, Fang, Jiyu, Sundaram, Kalpathy, University of Central Florida
Abstract / Description
Supercapacitors, the devices that connect the gap between batteries and conventional capacitors, have recently attracted significant attention due to their high specific capacitance, substantially enhanced power and energy densities, and extraordinary cycle life. In order to realize even better performance with supercapacitors, rejuvenated effort towards developing nanostructured electrodes is necessary. In this dissertation, several strategic directions of nanoarchitecturing the electrodes...
Show moreSupercapacitors, the devices that connect the gap between batteries and conventional capacitors, have recently attracted significant attention due to their high specific capacitance, substantially enhanced power and energy densities, and extraordinary cycle life. In order to realize even better performance with supercapacitors, rejuvenated effort towards developing nanostructured electrodes is necessary. In this dissertation, several strategic directions of nanoarchitecturing the electrodes to enhance the performance of supercapacitors are investigated. An introduction and background of supercapacitors, which includes motivation, classification and working principles, recent nanostructured electrode materials studies, and devices fabrication, are initially presented. A facile method, called Spin-on Nanoprinting (SNAP), to fabricate highly ordered manganese dioxide (MnO2) nanopillars is introduced. The SNAP method that is further modified to develop carbon nanoarray electrodes is also discussed. Subsequently, a template-free method to develop high aspect ratio copper oxide nanowhiskers on copper substrate is presented, which boosts the surface area by 1000 times compared to non-nanostructured copper substrate. Electrochemically deposited MnO2 on the nanostructured substrate provided a specific capacitance of about 1379 F g-1 which is very close to the theoretical value (~ 1400 F g-1) due to this efficient nanostructure design. In addition, a novel method to decorate metal nanoparticles on graphene aerogel, which considerably enhances the electronic conductivity and the corresponding specific capacitance, is demonstrated. Moreover, ferric oxide (Fe2O3) nanorods prepared by a simple hydrothermal method is discussed. Asymmetric devices assembled based on Fe2O3 nanorods and MnO2 nanowhiskers show excellent electrochemical properties. The devices not only display the capability to store energy but also transmit electricity through the inner copper core. These two functions are independent and do not interfere with each other. Finally, a summary of this dissertation as well as some potential future directions are presented.
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Date Issued
2015
Identifier
CFE0006062, ucf:50995
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0006062
Nano and nanostructured materials for optical applications
Title
Nano and nanostructured materials for optical applications.
Creator
Chantharasupawong, Panit, Thomas, Jayan, Hagan, David, Kik, Pieter, Gaume, Romain, Chanda, Debashis, University of Central Florida
Abstract / Description
Nano and nanostructured materials offer unique physical and chemical properties that differ considerably from their bulk counterparts. For decades, due to their fascinating properties, they have been extensively explored and found to be beneficial in numerous applications. These materials are key components in many cutting-edge optic and photonic technologies, including photovoltaics, waveguides and sensors. In this dissertation, the uses of nano and nanostructured materials for optical...
Show moreNano and nanostructured materials offer unique physical and chemical properties that differ considerably from their bulk counterparts. For decades, due to their fascinating properties, they have been extensively explored and found to be beneficial in numerous applications. These materials are key components in many cutting-edge optic and photonic technologies, including photovoltaics, waveguides and sensors. In this dissertation, the uses of nano and nanostructured materials for optical applications are investigated in the context of optical limiting, three dimensional displays, and optical sensing. Nanomaterials with nonlinear optical responses are promising candidates for self-activating optical limiters. In the first part of this study, optical limiting properties of unexplored nanomaterials are investigated. A photoacoustic detection technique is developed as an alternative characterization method for studying optical nonlinearities. This was done with an indigenously developed setup for measuring the photoacoustic signals generated from samples excited with a pulse laser. A theoretical model for understanding the experimental observations is presented. In addition, the advantages of this newly developed technique over the existing methods are demonstrated. Blending optical sensitizers with photoconducting polymers and chromophores results in a polymer composite that is able to record a light grating. This composite can be used as recording media in 3D holographic display technology. Here, 2D nano materials, like graphenes, are used as optical sensitizers to improve the response time of a photorefractive polymer. The addition of graphenes to a PATPD/ECZ/7-DCST composite results in a three-fold enhancement in response time and therefore faster recording speed of the medium. The faster build-up time is attributed to better charge generation and mobility due to the presence of graphenes in the composite. Lastly, a facile nanofabrication technique is developed to produce metallic nanostructures with a tunable plasmonic response. The enhancement of the light-matter interactions due to these nanostructures in sensing an analyte is demonstrated.
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Date Issued
2015
Identifier
CFE0006029, ucf:51016
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0006029
Advanced Metrology and Diagnostic Loss Analytics for Crystalline Silicon Photovoltaics.
Title
Advanced Metrology and Diagnostic Loss Analytics for Crystalline Silicon Photovoltaics.
Creator
Schneller, Eric, Schoenfeld, Winston, Thomas, Jayan, Fenton, James, Coffey, Kevin, Sundaram, Kalpathy, University of Central Florida
Abstract / Description
Characterization plays a key role in developing a comprehensive understanding of the structure and performance of photovoltaic devices. High quality characterization methods enable researchers to assess material choices and processing steps, ultimately giving way to improved device performance and reduced manufacturing costs. In this work, several aspects of advanced metrology for crystalline silicon photovoltaic are investigated including in-line applications for manufacturing, off-line...
Show moreCharacterization plays a key role in developing a comprehensive understanding of the structure and performance of photovoltaic devices. High quality characterization methods enable researchers to assess material choices and processing steps, ultimately giving way to improved device performance and reduced manufacturing costs. In this work, several aspects of advanced metrology for crystalline silicon photovoltaic are investigated including in-line applications for manufacturing, off-line applications for research and development, and module/system level applications to evaluate long-term reliability. A frame work was developed to assess the cost and potential value of metrology within a manufacturing line. This framework has been published to an on-line calculator in an effort to provide the solar industry with an intuitive and transparent method of evaluating the economics of in-line metrology. One important use of metrology is in evaluating spatial non-uniformities, as localized defects in large area solar cells often reduce overall device performance. Techniques that probe spatial uniformity were explored and analysis algorithms were developed that provide insights regarding process non-uniformity and its impact on device performance. Finally, a comprehensive suite of module level characterization was developed to accurately evaluate performance and identify degradation mechanisms in field deployed photovoltaic modules. For each of these applications, case-studies were used to demonstrate the value of these techniques and to highlight potential use cases.
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Date Issued
2016
Identifier
CFE0006499, ucf:51386
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0006499
Study of Surface Passivation Behavior of Crystalline Silicon Solar Cells
Title
Study of Surface Passivation Behavior of Crystalline Silicon Solar Cells.
Creator
Ali, Haider, Schoenfeld, Winston, Coffey, Kevin, Gaume, Romain, Thomas, Jayan, Chanda, Debashis, University of Central Florida
Abstract / Description
To achieve efficiencies approaching the theoretical limit of 29.4% for industrially manufactured solar cells based on crystalline silicon, it is essential to have very low surface recombination velocities at both the front and rear surfaces of the silicon substrate. Typically, the substrate surfaces feature contacted and uncontacted regions, and recombination should be limited for both to maximize the energy conversion efficiency.Uncontacted silicon surfaces are often passivated by the...
Show moreTo achieve efficiencies approaching the theoretical limit of 29.4% for industrially manufactured solar cells based on crystalline silicon, it is essential to have very low surface recombination velocities at both the front and rear surfaces of the silicon substrate. Typically, the substrate surfaces feature contacted and uncontacted regions, and recombination should be limited for both to maximize the energy conversion efficiency.Uncontacted silicon surfaces are often passivated by the deposition of silicon nitride (SiNx) or an aluminum oxide film with SiNx as capping layer (Al2O3/SiNx stack). Further, proper surface preparation and cleaning of Si wafers prior to deposition also plays an important role in minimizing surface recombination. In the present work, the effect of various cleans based on different combinations of HCl, HF, HNO3, and ozonated deionized water (DIO3) on surface passivation quality of boron-diffused and undiffused {100} n-type Cz Si wafers was studied. It was observed that for SiNx passivated Si, carrier lifetime was strongly influenced by cleaning variations and that a DIO3-last treatment resulted in higher lifetimes. Moreover, DIO3+HF+HCl?HF?DIO3 and HNO3?HF?HNO3 cleans emerged as potential low-cost alternatives to HCl/HF clean in the photovoltaics industry.Transmission electron microscopy (TEM) studies were carried out to get insight into the origin of variation in carrier lifetimes for different cleans. Changes in the surface cleans used were not found to have a significant impact on Al2O3/SiNx passivation stacks.ivHowever, an oxide-last cleaning step prior to deposition of SiNx passivation layers was found to create a 1-2 nm SiOx tunnel layer resulting in excellent carrier lifetimes.For contacted regions, low surface recombination can be achieved using passivated carrier selective contacts, which not only passivate the silicon surface and improve the open circuit voltage, but are also carrier selective. This means they only allow the majority carrier to be transported to the metal contacts, limiting recombination by reducing the number of minority carriers. Typically, carrier selectivity is achieved using a thin metal oxide layer, such as titanium oxide (TiO2) for electron-selective contacts and molybdenum oxide (MoOx) for hole-selective contacts. This is normally coupled with a very thin passivation layer (e.g., a-Si:H, SiOx) between the silicon wafer and the contact.In the present work, TiO2-based electron-selective passivated rear contacts were investigated for n-type c-Si solar cells. A low efficiency of 9.8% was obtained for cells featuring a-Si:H/TiO2 rear contact, which can be attributed to rapid degradation of surface passivation of a-Si:H upon FGA at 350(&)deg;C due to hydrogen evolution leading to generation of defect states which increases recombination and hence a much lower Voc of 365 mV is obtained. On the other hand, 21.6% efficiency for cells featuring SiO2/TiO2 rear contact is due to excellent passivation of SiO2/TiO2 stack upon FGA anneal, which can be attributed to the presence of 1-2 nm SiO2 layer whose passivation performance improves upon FGA at 350(&)deg;C whereas presence of large number of oxygen vacancies in TiO2-x reduces rear contact resistivity.vLikewise, MoOx-based contacts were investigated as hole-selective front contacts for an n-type cell with a boron-doped emitter. It has been previously reported that cell efficiencies up to 22.5% have been achieved with silicon heterojunction solar cells featuring a front contact wherein MoOx is inserted between a-Si:H(i) and hydrogenated indium oxide (IO:H). However, device performance and FF degrades upon annealing beyond 130(&)deg;C. In this work, contact resistivity measurements by TLM technique in combination with TEM studies revealed that degradation of device performance is due to oxygen diffusion into MoOx upon annealing in air which reduces concentration of oxygen vacancies in MoOx and increases contact resistivity. The increase in contact resistivity reduces FF resulting in deterioration of device performance.
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Date Issued
2017
Identifier
CFE0006554, ucf:51351
Format
Document (PDF)
PURL
http://purl.flvc.org/ucf/fd/CFE0006554