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The microorganisms that colonize the gastrointestinal tract have been recognized over the last several decades to have a significant bearing on the health trajectories of the hosts that harbor them. The collection of these gut microbes display links with acute and chronic disease, garnering substantial interest in leveraging the microbiome for improved health states. How these microbes assemble as a complex community and interact with each other, and the host depends on a multitude of factors. In adulthood, diet is one of the main moderators, having a significant influence on community composition and the functional output captured in the metabolites produced and/or modified by the gut microbiome. Thus, the assembly of microbes in the gut are tightly intertwined with health. In this dissertation, I examine the impact of diet and feeding behaviors on the gut microbiome and what features may be grounding or responsive under such pressures. Specifically, I first explore the avian gut microbiome as a barometer of nutritional and environmental influence on host health. Birds have continually displayed robust physiology under dietary pressures, placing them in an important, though underutilized, position within the translational science framework. Second, I describe the association of food insecurity on gut microbiome and metabolome profiles in a diverse college-based sample. Food insecurity provides its own set of unique pressures, such as unintentional calorie restriction, and inconsistent dietary intake and access to healthy food options. Third, I examine the effect of a one vs. two-consecutive days of intermittent fasting on the gut microbiome, the plasma metabolome, and associated clinical outcomes in overweight and obese adults. Growing in scientific and lay popularity, dietary fasting has been noted to induce changes in the diversity of gut microflora and gut motility, though different fasting lengths have not been assessed in the context of the human microbiome. Overall, this collection of work underscores that the community of microbes in the gut are individualized, resilient, and baseline composition and functioning are germane to how an individual may react to a particular dietary intervention.
ContributorsMohr, Alex (Author) / Sweazea, Karen L. (Thesis advisor) / Johnston, Carol S. (Committee member) / Sears, Dorothy D. (Committee member) / Whisner, Corrie M. (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Arizona State University (Publisher)
Created2022
Description
Trichloroethene (TCE) and hexavalent chromium (Cr (VI)) are ubiquitous subsurface contaminants affecting the water quality and threatening human health. Microorganisms capable of TCE and Cr (VI) reductions can be explored for bioremediation at contaminated sites. The goal of my dissertation research was to address challenges that decrease the efficiency of bioremediation in the subsurface. Specifically, I investigated strategies to (i) promote improve microbial reductive dechlorination extent through the addition of Fe0 and (ii) Cr (VI) bio-reduction through enrichment of specialized microbial consortia. Fe0 can enhance microbial TCE reduction by inducing anoxic conditions and generating H2 (electron donor). I first evaluated the effect of Fe0 on microbial reduction of TCE (with ClO4– as co-contaminant) using semi-batch soil microcosms. Results showed that high concentration of Fe0 expected during in situ remediation inhibited microbial TCE and ClO4– reduction when added together with Dehalococcoides mccartyi-containing cultures. A low concentration of aged Fe0 enhanced microbial TCE dechlorination to ethene and supported complete microbial ClO4– reduction. I then evaluated a decoupled Fe0 and biostimulation/bioaugmentation treatment approach using soil packed columns with continuous flow of groundwater. I demonstrated that microbial TCE reductive dechlorination to ethene can be benefitted by Fe0 abiotic reactions, when biostimulation and bioaugmentation are performed downstream of Fe0 addition. Furthermore, I showed that ethene production can be sustained in the presence of aerobic groundwater (after Fe0 exhaustion) by the addition of organic substrates. I hypothesized that some lessons learned from TCE Bioremediation can be applied also for other pollutants that can benefit from anaerobic reductions, like Cr (VI). Bioremediation of Cr (VI) has historically relied on biostimulation of native microbial communities, partially due to the lack of knowledge of the benefits of adding enriched consortia of specialized microorganisms (bioaugmentation). To determine the merits of a specialized consortium on bio-reduction of Cr (VI), I first enriched a culture on lactate and Cr (VI). The culture had high abundance of putative Morganella species and showed rapid and sustained Cr (VI) bio-reduction compared to a subculture grown with lactate only (without Morganella). Overall, this dissertation work documents possible strategies for synergistic abiotic and biotic chlorinated ethenes reduction, and highlights that specialized consortia may benefit Cr (VI) bio-reduction.
ContributorsMohana Rangan, Srivatsan (Author) / Krajmalnik-Brown, Rosa (Thesis advisor) / Delgado, Anca G (Thesis advisor) / Torres, César I (Committee member) / van Paassen, Leon (Committee member) / Arizona State University (Publisher)
Created2022
Description
This dissertation encompasses the interaction of antimicrobial chemicals and emerging contaminants with multi-drug resistant (MDR) bacteria and their implications in engineered systems. The aim is to investigate the effect of combination antimicrobials on MDR bacteria E. coli, evaluate the extent of synergism and antagonism of utilizing two distinct biocidal chemicals, and evaluate the influence of endocrine-disrupting chemicals (EDCs) on protein production in response to stressors. Resistance mechanisms of bacteria such as E. coli include the use of protein systems that efflux excess nutrients or toxic compounds. These efflux proteins activate in response to environmental stressors such as contaminants and antimicrobials to varying degrees and are major contributors to antibiotic resistance in pathogenic bacteria. As is the case with engineered microbial environments, large quantities of emerging contaminants interact with bacteria, influencing antibiotic resistance and attenuation of these chemicals to an unknown degree. Interactions of antimicrobials on MDR bacteria such as E. coli have been extensively studied for pathogens, including synergistic combinations. Despite these studies in this field, a fundamental understanding of how chemicals influence antibiotic resistance in biological processes typical of engineered microbial environments is still ongoing. The impacts of EDCs on antibiotic resistance in E. coli were investigated by the characterization of synergism for antimicrobial therapies and the extrapolation of these metrics to the cycling of EDCs in engineered systems to observe the extent of antibiotic resistance proteins to the EDCs. The impact of this work provides insight into the delicate biochemistry and ongoing resistance phenomena regarding engineered systems.
ContributorsNovoa, Diego Erick (Author) / Conroy-Ben, Otakuye (Thesis advisor) / Abbazadegan, Morteza (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Arizona State University (Publisher)
Created2022
Description
In the last few decades, extensive research efforts have been focused on scaling down silicon-based complementary metal-oxide semiconductor (CMOS) technology to enable the continuation of Moore’s law. State-of-art CMOS includes fully depleted silicon-on-insulator (FDSOI) field-effect-transistors (FETs) with ultra-thin silicon channels (6 nm), as well as other three-dimensional (3D) device architectures like Fin-FETs, nanosheet FETs, etc. Significant research efforts have characterized these technologies towards various applications, and at different conditions including a wide range of temperatures from room temperature (300 K) down to cryogenic temperatures. Theoretical efforts have studied ultrascaled devices using Landauer theory to further understand their transport properties and predict their performance in the quasi-ballistic regime.Further scaling of CMOS devices requires the introduction of new semiconducting channel materials, as now established by the research community. Here, two-dimensional (2D) semiconductors have emerged as a promising candidate to replace silicon for next-generation ultrascaled CMOS devices. These emerging 2D semiconductors also have applications beyond CMOS, for example in novel memory, neuromorphic, and spintronic devices. Graphene is a promising candidate for spintronic devices due to its outstanding spin transport properties as evidenced by numerous studies in non-local lateral spin valve (LSV) geometries. The essential components of graphene-based LSV, such as graphene FETs, metal-graphene contacts, and tunneling barriers, were individually investigated as part of this doctoral dissertation.
In this work, several contributions were made to these CMOS and beyond CMOS technologies. This includes comprehensive characterization and modeling of FDSOI nanoscale FETs from room temperature down to cryogenic temperatures. Using Landauer theory for nanoscale transistors, FDSOI devices were analyzed and modeled under quasi-ballistic operation. This was extended towards a virtual-source modeling approach that accounts for temperature-dependent quasi-ballistic transport and back-gate biasing effects. Additionally, graphene devices with ultrathin high-k gate dielectrics were investigated towards FETs, non-volatile memory, and spintronic devices. New contributions were made relating to charge trapping effects and their impact on graphene device electrostatics (Dirac voltage shifts) and transport properties (impact on mobility and conductivity). This work also studied contact resistance and tunneling effects using transfer length method (TLM) graphene FET structures and magnetic tunneling junction (MTJ) towards graphene-based LSV.
ContributorsZhou, Guantong (Author) / Sanchez Esqueda, Ivan (Thesis advisor) / Vasileska, Dragica (Committee member) / Tongay, Sefaattin (Committee member) / Thornton, Trevor (Committee member) / Arizona State University (Publisher)
Created2023
Description
The research of alternative materials and new device architectures to exceed the limits of conventional silicon-based devices has been sparked by the persistent pursuit of semiconductor technology scaling. The development of tungsten diselenide (WSe2) and molybdenum disulfide (MoS2), well-known member of the transition metal dichalcogenide (TMD) family, has made great strides towards ultrascaled two-dimensional (2D) field-effect-transistors (FETs). The scaling issues facing silicon-based complementary metal-oxide-semiconductor (CMOS) technologies can be solved by 2D FETs, which show extraordinary potential.This dissertation provides a comprehensive experimental analysis relating to improvements in p-type metal-oxide-semiconductor (PMOS) FETs with few-layer WSe2 and high-κ metal gate (HKMG) stacks. Compared to this works improved methods, standard metallization (more damaging to underlying channel) results in significant Fermi-level pinning, although Schottky barrier heights remain small (< 100 meV) when using high work function metals. Temperature-dependent analysis reveals a dominant contribution to contact resistance from the damaged channel access region. Thus, through less damaging metallization methods combined with strongly scaled HKMG stacks significant improvements were achieved in contact resistance and PMOS FET overall performance. A clean contact/channel interface was achieved through high-vacuum evaporation and temperature-controlled stepped deposition. Theoretical analysis using a Landauer transport adapted to WSe2 Schottky barrier FETs (SB-FETs) elucidates the prospects of nanoscale 2D PMOS FETs indicating high-performance towards the ultimate CMOS scaling limit.
Next, this dissertation discusses how device electrical characteristics are affected by scaling of equivalent oxide thickness (EOT) and by adopting double-gate FET architectures, as well as how this might support CMOS scaling. An improved gate control over the channel is made possible by scaling EOT, improving on-off current ratios, carrier mobility, and subthreshold swing. This study also elucidates the impact of EOT scaling on FET gate hysteresis attributed to charge-trapping effects in high-κ-dielectrics prepared by atomic layer deposition (ALD). These developments in 2D FETs offer a compelling alternative to conventional silicon-based devices and a path for continued transistor scaling. This research contributes to ongoing efforts in 2D materials for future semiconductor technologies. Finally, this work introduces devices based on emerging Janus TMDs and bismuth oxyselenide (Bi2O2Se) layered semiconductors.
ContributorsPatoary, Md Naim Hossain (Author) / Sanchez Esqueda, Ivan (Thesis advisor) / Tongay, Sefaattin (Committee member) / Vasileska, Dragica (Committee member) / Goodnick, Stephen (Committee member) / Arizona State University (Publisher)
Created2023
Description
Doping is the cornerstone of Semiconductor technology, enabling the functionalities of modern digital electronics. Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have tunable direct bandgaps, strong many-body interactions, and promising applications in future quantum information sciences, optoelectronic, spintronic, and valleytronic devices. However, their wafer-scale synthesis and precisely controllable doping are challenging. Moreover, there is no fixed framework to identify the doping concentration, which impedes their process integration for future commercialization. This work utilizes the Neutron Transmutation Doping technique to control the doping uniformly and precisely in TMDCs. Rhenium and Tin dopants are introduced in Tungsten- and Indium-based Chalcogenides, respectively. Fine-tuning over 0.001% doping level is achieved. Precise analytical techniques such as Gamma spectroscopy and Secondary Ion Mass Spectrometry are used to quantify ultra-low doping levels ranging from 0.005-0.01% with minimal error. Dopants in 2D TMDCs often exhibit a broad stokes-shifted emission, with high linewidths, due to extrinsic effects such as substrate disorder and surface adsorbates. A well-defined bound exciton emission induced by Rhenium dopants in monolayer WSe2 and WS2 at liquid nitrogen temperatures is reported along with specific annealing regimes to minimize the defects induced in the Neutron Transmutation process. This work demonstrates a framework for Neutron Doping in 2D materials, which can be a scalable process for controlling doping and doping-induced effects in 2D materials.
ContributorsLakhavade, Sushant Sambhaji (Author) / Tongay, Sefaattin (Thesis advisor) / Alford, Terry (Committee member) / Yang, Sui (Committee member) / Arizona State University (Publisher)
Created2023
Characterization and Manipulation of Microbiomes From Arid Landfills for Improved Methane Production
Description
Environmentally harmful byproducts from solid waste’s decomposition, including methane (CH4) emissions, are managed through standardized landfill engineering and gas-capture mechanisms. Yet only a limited number of studies have analyzed the development and composition of Bacteria and Archaea involved in CH4 production from landfills. The objectives of this research were to compare microbiomes and bioactivity from CH4-producing communities in contrasting spatial areas of arid landfills and to tests a new technology to biostimulate CH4 production (methanogenesis) from solid waste under dynamic environmental conditions controlled in the laboratory. My hypothesis was that the diversity and abundance of methanogenic Archaea in municipal solid waste (MSW), or its leachate, play an important role on CH4 production partially attributed to the group’s wide hydrogen (H2) consumption capabilities. I tested this hypothesis by conducting complementary field observations and laboratory experiments. I describe niches of methanogenic Archaea in MSW leachate across defined areas within a single landfill, while demonstrating functional H2-dependent activity. To alleviate limited H2 bioavailability encountered in-situ, I present biostimulant feasibility and proof-of-concepts studies through the amendment of zero valent metals (ZVMs). My results demonstrate that older-aged MSW was minimally biostimulated for greater CH4 production relative to a control when exposed to iron (Fe0) or manganese (Mn0), due to highly discernable traits of soluble carbon, nitrogen, and unidentified fluorophores found in water extracts between young and old aged, starting MSW. Acetate and inhibitory H2 partial pressures accumulated in microcosms containing old-aged MSW. In a final experiment, repeated amendments of ZVMs to MSW in a 600 day mesocosm experiment mediated significantly higher CH4 concentrations and yields during the first of three ZVM injections. Fe0 and Mn0 experimental treatments at mesocosm-scale also highlighted accelerated development of seemingly important, but elusive Archaea including Methanobacteriaceae, a methane-producing family that is found in diverse environments. Also, prokaryotic classes including Candidatus Bathyarchaeota, an uncultured group commonly found in carbon-rich ecosystems, and Clostridia; All three taxa I identified as highly predictive in the time-dependent progression of MSW decomposition. Altogether, my experiments demonstrate the importance of H2 bioavailability on CH4 production and the consistent development of Methanobacteriaceae in productive MSW microbiomes.
ContributorsReynolds, Mark Christian (Author) / Cadillo-Quiroz, Hinsby (Thesis advisor) / Krajmalnik-Brown, Rosa (Thesis advisor) / Wang, Xuan (Committee member) / Kavazanjian, Edward (Committee member) / Arizona State University (Publisher)
Created2022
Description
In the past decade, 2D materials especially transition metal dichalcogenides (TMDc), have been studied extensively for their remarkable optical and electrical properties arising from their reduced dimensionality. A new class of materials developed based on 2D TMDc that has gained great interest in recent years is Janus crystals. In contrast to TMDc, Janus monolayer consists of two different chalcogen atomic layers between which the transition metal layer is sandwiched. This structural asymmetry causes strain buildup or a vertically oriented electric field to form within the monolayer. The presence of strain brings questions about the materials' synthesis approach, particularly when strain begins to accumulate and whether it causes defects within monolayers.The initial research demonstrated that Janus materials could be synthesized at high temperatures inside a chemical vapor deposition (CVD) furnace. Recently, a new method (selective epitaxy atomic replacement - SEAR) for plasma-based room temperature Janus crystal synthesis was proposed. In this method etching and replacing top layer chalcogen atoms of the TMDc monolayer happens with reactive hydrogen and sulfur radicals. Based on Raman and photoluminescence studies, the SEAR method produces high-quality Janus materials. Another method used to create Janus materials was the pulsed laser deposition (PLD) technique, which utilizes the interaction of sulfur/selenium plume with monolayer to replace the top chalcogen atomic layer in a single step.
The goal of this analysis is to characterize microscale defects that appear in 2D Janus materials after they are synthesized using SEAR and PLD techniques. Various microscopic techniques were used for this purpose, as well as to understand the
mechanism of defect formation. The main mechanism of defect formation was proposed to be strain release phenomena. Furthermore, different chalcogen atom positions within the monolayer result in different types of defects, such as the appearance of cracks or wrinkles across monolayers. In addition to investigating sample topography, Kelvin probe force microscopy (KPFM) was used to examine its electrical properties to see if the formation of defects impacts work function. Further study directions have been suggested for identifying and characterizing defects and their formation mechanism in the Janus crystals to understand their fundamental properties.
ContributorsSinha, Shantanu (Author) / Tongay, Sefaattin (Thesis advisor) / Alford, Terry (Committee member) / Yang, Sui (Committee member) / Arizona State University (Publisher)
Created2022
Description
This study investigated the difference in biofilm growth on pristine and aged polypropylene microplastics exposed to Tempe Town Lake water for 8 weeks. The research question here is, does the aging of microplastic (MPs) change the biofilm formation rate and composition of the biofilm in comparison with the pristine MPs. To answer this question, the biofilm formation was quantified using different methods over time for both pristine polypropylene and aged polypropylene using agar plate counts and crystal violet staining. Colony counts based on agar plating showed an increase in microbial growth over the 8 weeks of treatment, with the aged MPs accumulating higher microbial counts than the pristine MPs. The diversity of the biofilm decreased over time for both MPs and the aged MPs had overall less diversity in biofilm, based on phenotype enumeration, in comparison with the pristine MPs. Higher biofilm growth on aged MPs was confirmed using crystal violet staining, which stains the negatively charged biological compounds such as proteins and the extracellular polymeric substance matrix of the biofilm. Using this complementary approach to colony counting, the same trend of higher biofilm growth on aged MPs was found. Further studies will focus on confirming the phenotype findings using microbiome analysis following DNA extraction. This project created a methodology to quantify biofilm formation on MPs, which was used to show that MPs may accumulate more biofilms in the environment as they age under sunlight.
ContributorsMushro, Noelle (Author) / Perreault, Francois (Thesis advisor) / Hamilton, Kerry (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Arizona State University (Publisher)
Created2022
Description
Complex perovskite materials, including Ba(Zn1/3Ta2/3)O3 (BZT), are commonly used to make resonators and filters in communication systems because of their low dielectric loss and high-quality factors (Q). Transition metal additives are introduced (i.e., Ni2+, Co2+, Mn2+) to act as sintering agents and tune their temperature coefficient to zero or near-zero. However, losses in these commercial dielectric materials at cryogenic temperatures increase markedly due to spin-excitation resulting from the presence of paramagnetic defects. Applying a large magnetic field (e.g., 5 Tesla) quenches these losses and has allowed the study of other loss mechanisms present at low temperatures. Work was performed on Fe3+ doped LaAlO3. At high magnetic fields, the residual losses versus temperature plots exhibit Debye peaks at ~40 K, ~75 K, and ~215 K temperature and can be tentatively associated with defect reactions O_i^x+V_O^x→O_i^'+V_O^•, Fe_Al^x+V_Al^"→Fe_Al^'+V_Al^' and Al_i^x+Al_i^(••)→〖2Al〗_i^•, respectively. Peaks in the loss tangent versus temperature graph of Zn-deficient BZT indicate a higher concentration of defects and appear to result from conduction losses.Guided by the knowledge gained from this study, a systematic study to develop high-performance microwave materials for ultra-high performance at cryogenic temperatures was performed. To this end, the production and characterization of perovskite materials that were either undoped or contained non-paramagnetic additives were carried out. Synthesis of BZT ceramic with over 98% theoretical density was obtained using B2O3 or BaZrO3 additives. At 4 K, the highest Q x f product of 283,000 GHz was recorded for 5% BaZrO3 doped BZT.
A portable, inexpensive open-air spectrometer was designed, built, and tested to make the electron paramagnetic resonance (EPR) technique more accessible for high-school and university lab instruction. In this design, the sample is placed near a dielectric resonator and does not need to be enclosed in a cavity, as is used in commercial EPR spectrometers. Permanent magnets used produce fields up to 1500 G, enabling EPR measurements up to 3 GHz.
ContributorsGajare, Siddhesh Girish (Author) / Newman, Nathan (Thesis advisor) / Alford, Terry (Committee member) / Tongay, Sefaattin (Committee member) / Chamberlin, Ralph (Committee member) / Arizona State University (Publisher)
Created2022