In recent years, continuum models of solvation have had exceptional success in materials simulations as well as condensed matter physics. They can easily capture the effects of disordered systems, such as neutral liquids or electrolytes solutions, on material interfaces without the need for expensive statistical sampling. The Environ library (www.quantum-environ.org) implements different continuum models and correction schemes, which is the focus of this presentation. Recently refactored into a stand-alone library, many changes have been introduced in Environ, making it more flexible and computationally efficient. Introduction of a double-cell formalism allows for faster ab initio DFT calculations while reparameterization of soft-sphere continuum model allows for smaller density cutoffs. Furthermore, Environ's periodic boundary conditions correction schemes have been expanded by including the AFC90 library, which allows for faster DFT calculations of partially periodic systems, such as slabs, wires, and isolated molecules. Finally, stand-alone Environ can now provide atomic and molecular descriptors, which can be used to characterize solvated interfaces, e.g. in machine learning applications. The specific details of the implementations are reviewed as well as their efficiency and some choice applications for different calculation setups and systems.

The Gemini Near Infrared Spectrograph - Distant Quasar Survey (GNIRS-DQS) is the largest uniform, homogeneous survey of its kind, covering 260 quasars at 1.5 ≤ z ≤ 3.5. This unique survey, coupled with data from the Sloan Digital Sky Survey (SDSS), enables new investigations into redshifts, supermassive black hole masses (MBH), and accretion rates at high redshift through spectroscopic coverage of important rest-frame UV-optical emission lines. The importance of this survey is highlighted in the fact that the optical emission lines provide more reliable measurements of these quasar parameters than their UV counterpart. With such a unique sample compiled here, I construct prescriptions to calibrate these quasar parameters derived from rest-frame UV emission lines to those derived from rest-frame optical emission lines. These prescriptions provide important insight into how these parameters depend on redshift and are potentially biased as we look out further into the universe. Additionally, all the work completed with this sample will help shape our understanding of how these quasars and their host galaxies co-evolve over cosmic time.

I present spectroscopic measurements for 260 sources from the Gemini Near Infrared Spectrograph–Distant Quasar Survey (GNIRS-DQS). Being the largest uniform, homogeneous survey of its kind, it represents a flux-limited sample of Sloan Digital Sky Survey (SDSS) quasars at 1.5 < z < 3.5. A combination of the GNIRS and SDSS spectra covers principal quasar diagnostic features, chiefly the C IV λ1549, Mg II λλ2798, 2803, Hβ λ4861, and [O III] λλ4959, 5007 emission lines, in each source. The spectral inventory is utilized primarily to develop prescriptions for obtaining more accurate and precise redshifts, black hole masses, and accretion rates for all quasars. Additionally, the measurements facilitate an understanding of the dependence of rest-frame ultraviolet–optical spectral properties of quasars on redshift, luminosity, and Eddington ratio, and test whether the physical properties of the quasar central engine evolve over cosmic time.

In this dissertation, I report the results of my research on twisted moiré photonic crystals which can be formed through multi-beam holographic interference without a physical rotation and later fabricated by electron-beam lithography. Their optical properties, such as photonic bandgaps, multiple resonance modes, and quality factor are presented. Randomized moire photonic crystals in lattice are also studied. The applications of moire photonic crystals in improving light extraction efficiency are simulated and verified in light emitting devices. Furthermore, I simulated the light extraction efficiency in OLED when the Al layer is patterned with a triangular GPSC, square moiré PhC with defects in the uniform area, and random locations of the photonic lattice, and obtain light extraction efficiency of 78.9%, 79.9%, 81.7%, respectively. Also, the ratios of photoluminescence intensity of LED integrated with twisted moiré PhCs and random moiré PhCs over that without moiré PhCs are measured to be (1.3-1.9) and 1.74, respectively, in a good agreement with simulated ratios of 1.69 and 1.8.

This thesis is a study of the structural, electrical and magnetic properties of indium antimonide (InSb) nanowires (NWs), that were synthesized by a template-assisted ordered growth technique via electrochemical deposition. InSb was chosen for this study because of its intrinsic properties that make it a material of choice for applications in high channel mobility, infrared (IR) sensing, thermoelectrics, and magnetoresistive sensing martials. This work has four main components: (i) Growth in commercially available anodic aluminum oxide (AAO) template, where hole-dominated conduction was observed, following NW growth in a low pH electrolyte. The challenge in using these AAO templates was in covering the back surface of the pores with a metal film. Uncovered pores resulted in electrolyte leakage and non-reproducible results. (ii) Growth in flexible polycarbonate membranes, where the flexibility of the membranes resulted in polycrystalline or high defect density NW growth. (iii) Fabrication of an AAO template, where the barrier layer thinning technique was found to be efficient in removal of the think aluminum oxide barrier that exists at the interface between the template and the aluminum metal. This allows for direct growth of NWs into the template pores without the need for metal evaporation. (iv) Fabrication of a heterostructure …

This dissertation work is a study of positronium formation for positron-hydrogen and positron-helium collisions in the Ore gap (the energy region between the threshold for ground-state positronium formation and the first excitation level of the target atom) using variational K-matrices. We have fitted the K-matrices using multichannel effective range theories and using polynomials. Using the variational K-matrices and their fits, we have located zeros in the positronium-formation scattering amplitude and corresponding deep minima in the positronium-formation differential cross section. The zeros are related to the vortices in the extended velocity field associated with the positronium-formation scattering amplitude. For positron-hydrogen collisions, we have found two zeros in the positronium-formation scattering amplitude, and corresponding deep minima in the positronium-formation differential cross section, while we have obtained a zero in the positronium-formation scattering amplitude for positron-helium collisions. We have connected the zeros in the positronium-formation scattering amplitude to vortices in the extended velocity fields. Our work shows that vortices can occur for charge exchange in atomic collisions.

In this dissertation, we study the optical property of 2D graded photonic super-crystals (GPSCs) for photon management. We focused primarily on manipulation and control of light by using the newly discovered GPSCs which present great opportunity for electromagnetic wave control in photonic devices. The GPSC has been used to explore the superior capability of improving the light extraction efficiency of OLEDs. The enhancement of extraction efficiency has been explained in term of destructive interference of surface plasmon resonance and out-coupling of surface plasmon through phase matching provided by GPSC and verified by e-field intensity distributions. A large light extraction efficiency up to 75% into glass substrate has been predicted through simulation. We also study the light trapping enhancement in GPSCs. Broadband, wide incident angle, and polarization independent light trapping enhancement is achieved in silicon solar cells patterned with the GPSCs. In addition, novel 2D GPSCs were fabricated using holographic lithography through the interference lithography by two sets of multiple beams arranged in a cone geometry using a spatial light modulator (SLM). Finally, we also report a fabrication of GPSCs with a super-cell size of 12a×12a by using e-beam lithography. Diffraction pattern from GPSCs reveals unique diffraction properties. In an application …

The aim of this thesis is to develop both Yb and Tm fiber laser sources with all fiber cavities. Both wavelength ranges provide useful laser sources for optical pumping of helium. The goal is to develop Tm laser sources operating at 2058 nm to optically quench 3He (2058.63 nm) and 4He (2058.69 nm) singlets (21S0). We also have developed Yb laser sources at 1083 nm to optical pump the triplet states of helium and laser cool an atomic beam of helium.

In this dissertation work, the study focuses on large areal growth of MoS2 monolayers and a study of the structural, optical and electrical properties of such monolayers before and after transfer using a polymer-lift off technique. This work will discuss the issue of contact resistance and the effect of defects (both intrinsic and extrinsic) on the overall quality of the monolayer films. The significance of this dissertation work is that a reproducible strategy for monolayer MoS2 film growth and quantification of areal coverage as well as the detrimental effects of processing on device performance is presented.

An ion trap has been constructed that creates a potential well suitable for confining ions with the space charge of an electron cloud. The trap uses the concept of artificially structured boundaries, regions of overlapping electric and magnetic fields, to confine particles in a relatively field free volume. Measurements are presented from the build-up of ionized molecular hydrogen over time. Molecular hydrogen is introduced into the confinement volume by direct electron bombardment ionization of neutral background H2 leaked into the trap. Detailed analysis of the data is conducted using particle-in-cell simulations of trap operation and rate mechanics analysis. Pressure dependent estimates of ion lifetimes in the trap are on the order of milliseconds. Along with discussion of the trap a full introduction to the particle-in-cell technique is conducted through an original code implementation.

Propagation of a Gaussian beam in a layered periodic structure is studied analytically, numerically, and experimentally. It is demonstrated that for a special set of parameters the acoustic beam propagates without diffraction spreading. This propagation is also accompanied by negative refraction of the direction of phase velocity of the Bloch wave. In the study of two-dimensional viscous phononic crystals with asymmetrical solid inclusions, it was discovered that acoustic transmission is nonreciprocal. The effect of nonreciprocity in a static viscous environment is due to broken PT symmetry of the system as a whole. The difference in transmission is caused by the asymmetrical transmission and dissipation. The asymmetrical transmission is caused solely by broken mirror symmetry and could appear even in a lossless system. Asymmetrical dissipation of sound is a time-irreversible phenomenon that arises only if both energy dissipation and broken parity symmetry are present in the system. The numerical results for both types of phononic crystals were verified experimentally. Proposed devices could be exploited as collimation, rectification, and isolation acoustic devices.

In the past two decades, myriad algorithms to elucidate the characteristics and dynamics of molecular systems have been developed for quantum computers. In this dissertation, we explore how these algorithms can be adapted to other fields, both to closely related subjects such as materials science, and more surprising subjects such as information theory. Special emphasis is placed on the Variational Quantum Eigensolver algorithm adapted to solve band structures of a periodic system; three distinct implementations are developed, each with its own advantages and disadvantages. We also see how unitary quantum circuits designed to model individual electron excitations within a molecule can be modified to prepare a quantum states strictly orthogonal to a space of known states, an important component to solve problems in thermodynamics and spectroscopy. Finally, we see how the core behavior in several quantum algorithms originally developed for quantum chemistry can be adapted to implement compressive sensing, a protocol in information theory for extrapolating large amounts of information from relatively few measurements. This body of work demonstrates that quantum algorithms developed to study molecules have immense interdisciplinary uses in fields as varied as materials science and information theory.

Electronic transport properties have been used to classify and characterize materials and describe their functionality. Recent surge in computational power has enabled computational modelling and accelerated theoretical studies to complement and accelerate experimental discovery of novel materials. This work looks at methods for theoretical calculations of electronic transport properties and addresses the limitations of a common approximation in the calculation of these properties, namely, the constant relaxation time approximation (CRTA). This work takes a look at the limitations of this approximation and introduces energy and temperature dependent relaxation times. This study is carried out on models and real systems and compared with experiments.

This work explores a continuum representation for diffuse layer models, thereby endowing continuum embedding models the ability to capture electrostatic phenomena in the environment such as the existence of electrolyte ions, and the nature of ionic liquids. It introduces a new field-aware continuum model that adjusts the size of the quantum regime per atom based on the distribution of charge in a system. The model accounts for the asymmetric nature of solvent distribution when applied to cations versus anions; it also overcomes the need to parameterize continuum interface models for different charged systems. The continuum representation of cavitation in water does not account for the tendency for water to form a hydrogen bonding network that is broken due to the formation of cavities. This effect is a major contributor to hydrophobic solvation and is an important precondition to the investigation of solvated proteins with continuum embedding. A new model inspired by machine learning advances is trained on molecular dynamics simulations due to the difficulty of isolating the cavitation energy term in experiment. Thermodynamic integration is used to calculate the energy from a step-like repulsive potential from cavities in TIP4P water, cavities ranging from small organic molecules, to small proteins. Predictions …

Magnetic nano-clusters in silicon involving iron and cobalt were synthesized using low energy (50 keV) ion implantation technique and post-implantation thermal annealing. Before the irradiation, multiple ion-solid interaction simulations were carried out to estimate optimal ion energy and fluence for each experiment. For high-fluence low-energy irradiation of heavy ions in a relatively lighter substrate, modeling the ion irradiation process using dynamic code SDTrimSP showed better agreement with the experimental results compared to the widely used static simulation code TRIM. A saturation in concentration (~ 48%) profile of the 50 keV Fe or Co implants in Si was seen at a fluence of ~ 2 × 1017 ions/cm2. Further study showed that for structures with a curved surface, particularly for nanowires, better simulation results could be extracted using a code "Iradina" as the curve geometry of the target surface can be directly defined in the input file. The compositional, structural, and magnetic properties were studied using Rutherford backscattering spectrometry, X-ray photoelectron spectroscopy, X-ray diffraction, atom probe tomography, and vibrating sample magnetometry. Irradiation of high-current (~ 2 μA/cm2) 50 keV Fe ions into Si at a fluence of 2 × 1017 ions/cm2 showed the formation of Fe5Si3 nano structures in the near-surface …

In this work, we have utilized an ion beam process known as gettering to migrate implanted Ni ions much deeper into the bulk substrate than their initial projected end of the range. The projected mean depth is known as Rp. The gettering effect is the most crucial part of the fabrication and we have found that for an H fluence of 3x 1016 cm-2 there is a threshold fluence of approximately 7.5 x 1015 cm-2 that cannot be surpassed if the gettering process is to be completed along with the substrate recovered to the high crystalline quality. This hard threshold is due to the gettering process relaxation induced mechanism that is responsible for migrating the Ni to the Rp/2 location while the H is vacating during the thermal annealing process. If the total number of vacancies produced by the H dissociation is not substantially larger than the total number of implanted Ni atoms the Ni will migrate to the Rp location of the Ni implantation at the amorphous and crystalline interface and toward the surface. When the gettering condition is not met the resulting magnetic responses vary from an exceptionally weak ferromagnetic response to not exhibiting a magnetic response. Additionally, …