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 Department: Department of Physics
A Search for Periodic and Quasi-Periodic Patterns in Select Proxy Data with a Goal to Understanding Temperature Variation
In this work over 200 temperature proxy data sets have been analyzed to determine if periodic and or quasi-periodic patterns exist in the data sets. References to the journal articles where data are recorded are provided. Chapter 1 serves an introduction to the problem of temperature determination in providing information on how various proxy data sources are derived. Examples are given of the techniques followed in producing proxy data that predict temperature for each method used. In chapter 2 temperature proxy data spanning the last 4000 years, from 2,000 BCE to 2,000 CE, are analyzed to determine if overarching patterns exist in proxy data sets. An average of over 100 proxy data sets was used to produce Figure 4. An overview of the data shows that several “peaks” can be identified. The data were then subjected to analysis using a series of frequency modulated cosine waves. This analysis led to a function that can be expressed by equation 3. The literature was examined to determine what mathematical models had been published to fit the experimental proxy data for temperature. A number of attempts have been made to fit data from limited data sets with some degree of success. Some other papers have used a sinusoidal function to best fit the changes in the temperature. After consideration of many published papers and reviewing long time streams of proxy data that appeared to have sine wave patterns, a new model was proposed for trial. As the patterns observed showed “almost” repeating sine cycles, a frequency modulated sine wave was chosen to obtain a best fit function. Although other papers have used a sinusoidal function to best fit the changes in the temperature, the “best fit” was limited. Thus, it was decided that a frequency modulated sine wave may be a better model that would provide a more precise fit. This proved to be the case and the more than 240 temperature proxy data sets were analyzed using Equation 3. In chapter 3 the time span for the proxy data was extended to cover the period of time 12,000 BCE to 2000 CE. The data were then tested by using the equation above to search for periodic/quasi-periodic patterns. These results are summarized under select conditions of time periods. In chapter 4 the interval of time is extended over 1,000,000 years of time to test for long period “periodic” changes in global temperature. These results are provided for overall analysis. The function f(x) as described above was used to test for periodic/quasi-periodic changes in the data. Chapter 5 provides an analysis of temperature proxy data for an interval of time of 3,000,000 years to establish how global temperature has varied during the last three million years. Some long-term quasi-periodic patterns are identified. Chapter 6 provides a summation of the model proposed for global temperature that can be expected if similar trends continue over future years as have prevailed for the past few million years. Data sets that were used in this work are tabulated in the appendices of this paper.
Quantum Coherent Control and Propagation in Lambda System
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Strong coherence in quasi-resonant laser driven system interferes with effective relaxations, resulting in behaviors like, coherent population trapping and Electromagnetically induced transparency. The Raman system can optimize this utilizing excited coherence in the lambda system when exposed to counter- intuitive pump-stokes pulses. The phenomenon can result in complete population transfer between vibrational levels called Stimulated Raman adiabatic passage(STIRAP). STIRAP and CHIRAP have been studied with Gaussian and chirped pulses. The optical propagation effects in dense medium for these phenomenon is studied to calculate the limitations and induced coherences. Further, the effect of rotational levels has been investigated. The molecular vibrational coherence strongly depends on the effect of rotational levels. The change in coherence interaction for ro-vibrational levels are reported and explained. We have considered the effects on the phase of radiation related to rotational mechanical motion of quantum system by taking advantages in ultra strong dispersion medium provided by quantum coherence in lambda system. The enhanced Fizeau effect on a single atom is observed.
Charged Particle Transport and Confinement Along Null Magnetic Curves and in Various Other Nonuniform Field Configurations for Applications in Antihydrogen Production
Comparisons between measurements of the ground-state hyperfine structure and gravitational acceleration of hydrogen and antihydrogen could provide a test of fundamental physical theories such as CPT (charge conjugation, parity, time-reversal) and gravitational symmetries. Currently, antihydrogen traps are based on Malmberg-Penning traps. The number of antiprotons in Malmberg-Penning traps with sufficiently low energy to be suitable for trappable antihydrogen production may be reduced by the electrostatic space charge of the positrons and/or collisions among antiprotons. Alternative trap designs may be needed for future antihydrogen experiments. A computational tool is developed to simulate charged particle motion in customizable magnetic fields generated by combinations of current loops and current lines. The tool is used to examine charged particle confinement in two systems consisting of dual, levitated current loops. The loops are coaxial and arranged to produce a magnetic null curve. Conditions leading to confinement in the system are quantified and confinement modes near the null curve and encircling one or both loops are identified. Furthermore, the tool is used to examine and quantify charged particle motion parallel to the null curve in the large radius limit of the dual, levitated current loops. An alternative to new trap designs is to identify the effects of the positron space in existing traps and to find modes of operation where the space charge is beneficial. Techniques are developed to apply the Boltzmann density relation along curved magnetic field lines. Equilibrium electrostatic potential profiles for a positron plasma are computed by solving Poisson's equation using a finite-difference method. Equilibria are computed in a model Penning trap with an axially varying magnetic field. Also, equilibria are computed for a positron plasma in a model of the ALPHA trap. Electric potential wells are found to form self-consistently. The technique is expanded to compute equilibria for a two-species plasma with an antiproton plasma confined by the positron space charge. The two-species equilibria are used to estimate timescales associated with three-body recombination, losses due to collisions between antiprotons, and temperature equilibration. An equilibrium where the three-body recombination rate is the smallest is identified.
Nonlinear and Quantum Optics Near Nanoparticles
We study the behavior of electric fields in and around dielectric and metal nanoparticles, and prepare the ground for their applications to a variety of systems viz. photovoltaics, imaging and detection techniques, and molecular spectroscopy. We exploit the property of nanoparticles being able to focus the radiation field into small regions and study some of the interesting nonlinear, and quantum coherence and interference phenomena near them. The traditional approach to study the nonlinear light-matter interactions involves the use of the slowly varying amplitude approximation (SVAA) as it simplifies the theoretical analysis. However, SVVA cannot be used for systems which are of the order of the wavelength of the light. We use the exact solutions of the Maxwell's equations to obtain the fields created due to metal and dielectric nanoparticles, and study nonlinear and quantum optical phenomena near these nanoparticles. We begin with the theoretical description of the electromagnetic fields created due to the nonlinear wavemixing process, namely, second-order nonlinearity in an nonlinear sphere. The phase-matching condition has been revisited in such particles and we found that it is not satisfied in the sphere. We have suggested a way to obtain optimal conditions for any type and size of material medium. We have also studied the modifications of the electromagnetic fields in a collection of nanoparticles due to strong near field nonlinear interactions using the generalized Mie theory for the case of many particles applicable in photovoltaics (PV). We also consider quantum coherence phenomena such as modification of dark states, stimulated Raman adiabatic passage (STIRAP), optical pumping in $4$-level atoms near nanoparticles by using rotating wave approximation to describe the Hamiltonian of the atomic system. We also considered the behavior of atomic and the averaged atomic polarization in $7$-level atoms near nanoparticles. This could be used as a prototype to study any $n-$level atomic system experimentally in the presence of ensembles of quantum emitters. In the last chapter, we suggested a variant of a pulse-shaping technique applicable in stimulated Raman spectroscopy (SRS) for detection of atoms and molecules in multiscattering media. We used discrete-dipole approximation to obtain the fields created by the nanoparticles.
Fractional Calculus and Dynamic Approach to Complexity
Fractional calculus enables the possibility of using real number powers or complex number powers of the differentiation operator. The fundamental connection between fractional calculus and subordination processes is explored and affords a physical interpretation for a fractional trajectory, that being an average over an ensemble of stochastic trajectories. With an ensemble average perspective, the explanation of the behavior of fractional chaotic systems changes dramatically. Before now what has been interpreted as intrinsic friction is actually a form of non-Markovian dissipation that automatically arises from adopting the fractional calculus, is shown to be a manifestation of decorrelations between trajectories. Nonlinear Langevin equation describes the mean field of a finite size complex network at criticality. Critical phenomena and temporal complexity are two very important issues of modern nonlinear dynamics and the link between them found by the author can significantly improve the understanding behavior of dynamical systems at criticality. The subject of temporal complexity addresses the challenging and especially helpful in addressing fundamental physical science issues beyond the limits of reductionism.
Variational Calculations of Positronium Scattering with Hydrogen
Positronium-hydrogen (Ps-H) scattering is of interest, as it is a fundamental four-body Coulomb problem. We have investigated low-energy Ps-H scattering below the Ps(n=2) excitation threshold using the Kohn variational method and variants of the method with a trial wavefunction that includes highly correlated Hylleraas-type short-range terms. We give an elegant formalism that combines all Kohn-type variational methods into a single form. Along with this, we have also developed a general formalism for Kohn-type matrix elements that allows us to evaluate arbitrary partial waves with a single codebase. Computational strategies we have developed and use in this work will also be discussed.With these methods, we have computed phase shifts for the first six partial waves for both the singlet and triplet states. The 1S and 1P phase shifts are highly accurate results and could potentially be viewed as benchmark results. Resonance positions and widths for the 1S-, 1P-, 1D-, and 1F-waves have been calculated.We present elastic integrated, elastic differential, and momentum transfer cross sections using all six partial waves and note interesting features of each. We use multiple effective range theories, including several that explicitly take into account the long-range van der Waals interaction, to investigate scattering lengths for the 1,3S and 1,3P partial waves and effective ranges for the 1,3S-wave.
Complex Numbers in Quantum Theory
In 1927, Nobel prize winning physicist, E. Schrodinger, in correspondence with Ehrenfest, wrote the following about the new theory: “What is unpleasant here, and indeed directly to be objected to, is the use of complex numbers. Psi is surely fundamentally a real function.” This seemingly simple issue remains unexplained almost ninety years later. In this dissertation I elucidate the physical and theoretical origins of the complex requirement. I identify a freedom/constraint situation encountered by vectors when, employed in accordance with adopted quantum representational methodology, and representing angular momentum states in particular. Complex vectors, quite simply, provide more available adjustable variables than do real vectors. The additional variables relax the constraint situation allowing the theory’s representational program to carry through. This complex number issue, which lies at the deepest foundations of the theory, has implications for important issues located higher in the theory. For example, any unification of the classical and quantum accounts of the settled order of nature, will rest squarely on our ability to account for the introduction of the imaginary unit.
Synthesis and Characterization of Ion Beam Assisted Silver Nanosystems in Silicon Based Materials for Enhanced Photocurrent Collection Efficiency
In recent years a great deal of interest has been focused on the synthesis of transitional metal (e.g. Ag, Cu, Fe, Au) nanosystems at the surface to sub-surface regions of Si and SiO2 matrices for fundamental understanding of their structures as well as for development of technological applications with enhanced electronic and optical properties. The applications of the metal nanoparticle or nanocluster (NC) systems range from plasmonics, photovoltaic devices, medical, and biosensors. In all of these applications; the size, shape and distribution of the metallic NCs in the silicon matrix play a key role. Low energy ion implantation followed by thermal annealing (in vacuum or gas environment) is one of the most suitable methods for synthesis of NCs at near surfaces to buried layers below the surfaces of the substrates. This technique can provide control over depth and concentration of the implanted ions in the host matrix. The implanted low energy metal ions initially amorphizes the Si substrates while being distributed at a shallow depth near the substrate surface. When subject to thermal annealing, the implanted ions agglomerate to form clusters of different sizes at different depths depending upon the fluence. However, for the heavier ions implanted with high fluences (~1×1016 - 1×1017 atoms/cm2), there lies challenges for accurately predicting the distribution of the implanted ions due to sputtering of the surface as well as redistribution of the implants within the host matrix. In this dissertation, we report the investigation of the saturation of the concentration of the implanted ion species in the depth profiles with low energies (< 80 keV) metal ions (Ag and Au) in Si (100), while studying the dynamic changes during the ion implantation. Multiple low energies (30-80 keV) Ag ions with different fluences were sequentially implanted into commercially available Si wafers in order to facilitate the formation of Ag NCs with a wide ion distributions range. The light absorption profile according to different sizes of NCs at the near-surface layers in Si were investigated. We have investigated the formation of Ag NCs in the Si matrix as a function of implantation and thermal annealing parameters. The absorbance of light is increased in Ag implanted Si with a significant increase in the current collection in I-V (current-voltage) photo switching measurements. The experimental photovoltaic cells fabricated with the Ag implanted Si samples were optically characterized under AM (air mass) 1.5 solar radiation conditions (~1.0 kW/m2). An enhancement in the charge collection were measured in the annealed samples, where prominent Ag NCs were formed in the Si matrix compared to the as-implanted samples with the amorphous layer. The characterization techniques such as Rutherford Backscattering Spectroscopy, XPS-depth profiling, transmission electron microscopy, optical absorption, and I-V (current-voltage) photo switching measurements were employed to understand the underlying science in the observed properties. The results of these investigations are discussed in this research.
Electromagnetically Modulated Sonic Structures
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Phononic crystals are structures composed of periodically arranged scatterers in a background medium that affect the transmission of elastic waves. They have garnered much interest in recent years for their macro-scale properties that can be modulated by the micro-scale components. The elastic properties of the composite materials, the contrast in the elastic properties of the composite materials, and the material arrangement all directly affect how an elastic wave will behave as it propagates through the sonic structure. The behavior of an elastic wave in a periodic structure is revealed in its transmission bandstructure, and modification of any the elastic parameters will result in tuning of the band structure. In this dissertation, a phononic crystal with properties that can be modulated using electromagnetic radiation, and more specifically, radio-frequency (RF) light will be presented.
Highly Efficient Single Frequency Blue Laser Generation by Second Harmonic Generation of Infrared Lasers Using Quasi Phase Matching in Periodically Poled Ferroelectric Crystals
Performance and reliability of solid state laser diodes in the IR region exceeds those in the visible and UV part of the light spectrum. Single frequency visible and UV laser diodes with higher than 500 mW power are not available commercially. However we successfully stabilized a multi-longitudinal mode IR laser to 860 mW single frequency. This means high efficiency harmonic generation using this laser can produce visible and UV laser light not available otherwise. In this study we examined three major leading nonlinear crystals: PPMgO:SLN, PPKTP and PPMgO:SLT to generate blue light by second harmonic generation. We achieved record high net conversion efficiencies 81.3% using PPMgO:SLT (~500 mW out), and 81.1% using PPKTP (~700 mW out). In both these cases an external resonance buildup cavity was used. We also studied a less complicated single pass waveguide configuration (guided waist size of ~ 5 um compared to ~60 um) to generate blue. With PPMgO:SLN we obtained net 40.4% and using PPKT net 6.8% (110mW and 10.1 mW respectively).
Interaction of Plasmons and Excitons for Low-Dimension Semiconductors
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The effects of surface plasmon for InGaN/GaN multi-quantum wells and ZnO nanoparticles optical linear and nonlinear emission efficiency had been experimentally studied. Due to the critical design for InGaN MQWs with inverted hexagonal pits based on GaN, both contribution of surface plasmon effect and image charge effect at resonant and off resonant frequencies were experimentally and theoretically investigated. With off- resonant condition, the InGaN MQWs emission significantly enhanced by metal nanoparticles. This enhancement was caused by the image charge effect, due to the accumulation of carriers to NPs region. When InGaN emission resonated with metal particles SP modes, surface Plasmon effect dominated the emission process. We also studied the surface plasmon effect for ZnO nanoparticles nonlinear optical processes, SHG and TPE. Defect level emission had more contribution at high incident intensity. Emissions are different for pumping deep into the bulk and near surface. A new assumption to increase the TPE efficiency was studied. We thought by using Au nanorods localized surface plasmon mode to couple the ZnO virtual state, the virtual state’s life time would be longer and experimentally lead the emission enhancement. We studied the TPE phenomena at high and near band gap energy. Both emission intensity and decay time results support our assumption. Theoretically, the carriers dynamic mechanism need further studies.
Temporal Complexity and Stochastic Central Limit Theorem
Complex processes whose evolution in time rests on the occurrence of a large and random number of intermittent events are the systems under study. The mean time distance between two consecutive events is infinite, thereby violating the ergodic condition and activating at the same time a stochastic central limit theorem that explains why the Mittag-Leffler function is a universal property of nature. The time evolution of these complex systems is properly generated by means of fractional differential equations, thus leading to the interpretation of fractional trajectories as the average over many random trajectories, each of which fits the stochastic central limit theorem and the condition for the Mittag-Leffler universality. Additionally, the effect of noise on the generation of the Mittag-Leffler function is discussed. Fluctuations of relatively weak intensity can conceal the asymptotic inverse power law behavior of the Mittag-Leffler function, providing a reason why stretched exponentials are frequently found in nature. These results afford a more unified picture of complexity resting on the Mittag-Leffler function and encompassing the standard inverse power law definition.
Enhancement of Mechanical, Thermal Stability, and Tribological Properties by Addition of Functionalized Reduced Graphene Oxide in Epoxy
The effects of octadecylamine-functionalized reduced graphene oxide (FRGO) on the frictional and wear properties of diglycidylether of bisphenol-A (DGEBA) epoxy are studied using a pin-on-disk tribometer. It was observed that the addition of FRGO significantly improves the tribological, mechanical, and thermal properties of epoxy matrix. Graphene oxide (GO) was functionalized with octadecylamine (ODA), and then reduction of oxygen-containing functional groups was carried out using hydrazine monohydrate. The Raman and x-ray photoelectron spectroscopy studies confirm significant reduction in oxygen-containing functional groups and formation of ODA functionalized reduced GO. The nanocomposites are prepared by adding 0.1, 0.2, 0.5 and 1.0 wt % of FRGO to the epoxy. The addition of FRGO increases by more than an order of magnitude the sliding distance during which the dynamic friction is ≤ 0.1. After this distance, the friction sharply increases to the range of 0.4 - 0.5. We explain the increase in sliding distance during which the friction is low by formation of a transfer film from the nanocomposite to the counterface. The wear rates in the low and high friction regimes are approximately 1.5 x 10-4 mm3/N·m and 5.5 x 10-4 mm3/N·m, respectively. The nanocomposites exhibit a 74 % increase in Young’s modulus with 0.5 wt. % of FRGO, and an increase in glass transition and thermal degradation temperatures.
Analysis of Biological Materials Using a Nuclear Microprobe
The use of nuclear microprobe techniques including: Particle induced x-ray emission (PIXE) and Rutherford backscattering spectrometry (RBS) for elemental analysis and quantitative elemental imaging of biological samples is especially useful in biological and biomedical research because of its high sensitivity for physiologically important trace elements or toxic heavy metals. The nuclear microprobe of the Ion Beam Modification and Analysis Laboratory (IBMAL) has been used to study the enhancement in metal uptake of two different plants. The roots of corn (Zea mays) have been analyzed to study the enhancement of iron uptake by adding Fe (II) or Fe (III) of different concentrations to the germinating medium of the seeds. The Fe uptake enhancement effect produced by lacing the germinating medium with carbon nanotubes has also been investigated. The aim of this investigation is to ensure not only high crop yield but also Fe-rich food products especially from calcareous soil which covers 30% of world’s agricultural land. The result will help reduce iron deficiency anemia, which has been identified as the leading nutritional disorder especially in developing countries by the World Health Organization. For the second plant, Mexican marigold (Tagetes erecta), the effect of an arbuscular mycorrhizal fungi (Glomus intraradices) for the improvement of lead-phytoremediation of lead contaminated soil has been investigated. Phytoremediation provides an environmentally safe technique of removing toxic heavy metals (like lead), which can find their way into human food, from lands contaminated by human activities like mining or by natural disasters like earthquakes. The roots of Mexican marigold have been analyzed to study the role of arbuscular mycorrhizal fungi in enhancement of lead uptake from the contaminated rhizosphere.
Sputtering of Bi and Preferential Sputtering of an Inhomogeneous Alloy
Angular distributions and total yields of atoms sputtered from bismuth targets by normally incident 10 keV -50 keV Ne+ and Ar+ ions have been measured both experimentally and by computer simulation. Polycrystalline Bi targets were used for experimental measurements. The sputtered atoms were collected on high purity aluminum foils under ultra-high vacuum conditions, and were subsequently analyzed using Rutherford backscattering spectroscopy. The Monte-Carlo based SRIM code was employed to simulate angular distributions of sputtered Bi atoms and total sputtering yields of Bi to compare with experiment. The measured sputtering yields were found to increase with increasing projectile energy for normally incident 10 keV - 50 keV Ne+ and Ar+ ions. The shapes of the angular distributions of sputtered Bi atoms demonstrated good agreement between experiment and simulation in the present study. The measured and simulated angular distributions of sputtered Bi exhibited an over-cosine tendency. The measured value of the degree of this over-cosine nature was observed to increase with increasing incident Ne+ ion energy, but was not strongly dependent on incident Ar+ ion energy. The differential angular sputtering yield and partial sputtering yields due to Ar ion bombardment of an inhomogeneous liquid Bi:Ga alloy have been investigated, both experimentally and by computer simulation. Normally incident 25 keV and 50 keV beams of Ar+ were used to sputter a target of 99.8 at% Ga and 0.2 at% Bi held at 40° C in ultra-high vacuum (UHV), under which conditions the alloy is known to exhibit extreme Gibbsian surface segregation that produces essentially a monolayer of Bi atop the bulk liquid. Angular distributions of sputtered neutrals and partial sputtering yields obtained from the conversion of areal densities of Bi and Ga atoms on collector foils were determined. The Monte-Carlo based SRIM code was employed to simulate the experiment and obtain the angular distribution of sputtered components. The angular distribution of sputtered Ga atoms, originating from underneath the surface monolayer, was measured to be sharply peaked in angle about the surface normal direction compared to the Bi atoms originating from surface monolayer. The simulation study produced contradicting results, where the species originating from surface monolayer was strongly peaked around the surface normal compared to the species originating from beneath the surface monolayer.
Studies of Charged Particle Dynamics for Antihydrogen Synthesis
Synthesis and capture of antihydrogen in controlled laboratory conditions will enable precise studies of neutral antimatter. The work presented deals with some of the physics pertinent to manipulating charged antiparticles in order to create neutral antimatter, and may be applicable to other scenarios of plasma confinement and charged particle interaction. The topics covered include the electrostatic confinement of a reflecting ion beam and the transverse confinement of an ion beam in a purely electrostatic configuration; the charge sign effect on the Coulomb logarithm for a two component (e.g., antihydrogen) plasma in a Penning trap as well as the collisional scattering for binary Coulomb interactions that are cut off at a distance different than the Debye length; and the formation of magnetobound positronium and protonium.
Electrical Conduction Mechanisms in the Disordered Material System P-type Hydrogenated Amorphous Silicon
The electrical and optical properties of boron doped hydrogenated amorphous silicon thin films (a-Si) were investigated to determine the effect of boron and hydrogen incorporation on carrier transport. The a-Si thin films were grown by plasma enhanced chemical vapor deposition (PECVD) at various boron concentrations, hydrogen dilutions, and at differing growth temperatures. The temperature dependent conductivity generally follows the hopping conduction model. Above a critical temperature, the dominant conduction mechanism is Mott variable range hopping conductivity (M-VRH), where p = ¼, and the carrier hopping depends on energy. However, at lower temperatures, the coulomb interaction between charge carriers becomes important and Efros-Shklosvkii variable hopping (ES-VRH) conduction, where p=1/2, must be included to describe the total conductivity. To correlate changes in electrical conductivity to changes in the local crystalline order, the transverse optical (TO) and transverse acoustic (TA) modes of the Raman spectra were studied to relate changes in short- and mid-range order to the effects of growth temperature, boron, and hydrogen incorporation. With an increase of hydrogen and/or growth temperature, both short and mid-range order improve, whereas the addition of boron results in the degradation of short range order. It is seen that there is a direct correlation between the electrical conductivity and changes in the short and mid-range order resulting from the passivation of defects by hydrogen and the creation of trap states by boron. This work was done under the ARO grant W911NF-10-1-0410, William W. Clark Program Manager. The samples were provided by L-3 Communications.
Relaxation Time Measurements for Collision Processes in the Surface Layers of Conductors and Semiconductors Near 10 Ghz
This thesis represents one phase of a joint effort of research on the properties of liquids and solids. This work is concerned primarily with the microwave properties of solids. In this investigation the properties exhibited by conductor and semiconductor materials when they are subjected to electromagnetic radiation of microwave frequency are studied. The method utilized in this experiment is the perturbation of a resonant cavity produced by introduction of a cylindrically shaped sample into it.
Microwave Line Widths of the Asymmetric Top Formic Acid Molecule
This work consisted of an experimental investigation of the formic acid (HCOOH) molecule's rotational spectrum. Measurements of line widths were obtained for J = 5, 12, 13, 19, and 20 for a pressure range from 1 to 10 microns. A linear behavior between Av and p was observed as predicted by theory. The line width parameter Avp was observed to depend on the quantum number J. Hard sphere collision diameters b1 were calculated using the obtained AvP values. These deduced hard sphere values were found to be larger than the physical size of the molecule. This result was found to be in general agreement with other investigation in which long range forces (dipole-dipole) dominate.
Effects of Discharge Tube Geometry on Plasma Ion Oscillations
This study considers the effect, on plasma ion oscillations, of various lengths of discharge tubes as well as various cross sections of discharge tubes. Four different gases were used in generating the plasma. Gas pressure and discharge voltage and current were varied to obtain a large number of signals. A historical survey is given to familiarize the reader with the field. The experimental equipment and procedure used in obtaining data is given. An analysis of the data obtained is presented along with possible explanations for the observed phenomena. Suggestions for future study are made.
Automatic Frequency Control of Microwave Radiation Sources
Resonant cavity controlled klystron frequency stabilization circuits and quartz-crystal oscillator frequency stabilization circuits were investigated for reflex klystrons operating at frequencies in the X-band range. The crystal oscillator circuit employed achieved better than 2 parts in 10 in frequency stability. A test of the functional properties of the frequency standard was made using the Stark effect in molecules.
The Classical Limit of Quantum Mechanics
The Feynman path integral formulation of quantum mechanics is a path integral representation for a propagator or probability amplitude in going between two points in space-time. The wave function is expressed in terms of an integral equation from which the Schrodinger equation can be derived. On taking the limit h — 0, the method of stationary phase can be applied and Newton's second law of motion is obtained. Also, the condition the phase vanishes leads to the Hamilton - Jacobi equation. The secondary objective of this paper is to study ways of relating quantum mechanics and classical mechanics. The Ehrenfest theorem is applied to a particle in an electromagnetic field. Expressions are found which are the hermitian Lorentz force operator, the hermitian torque operator, and the hermitian power operator.
Synthesis Strategies and a Study of Properties of Narrow and Wide Band Gap Nanowires
Various techniques to synthesize nanowires and nanotubes as a function of growth temperature and time were investigated. These include growth of nanowires by a chemical vapor deposition (CVD) system using vapor-liquid-solid (VLS) growth mechanism and electro-chemical synthesis of nanowires and nanotubes. Narrow band gap InSb Eg = 0.17 eV at room temp) nanowires were successively synthesized. Using a phase diagram, the transition of the nanowire from metallic- semiconducting- semi-metallic phase was investigated. A thermodynamic model is developed to show that the occurrence of native defects in InSb nanowires influenced by the nanowire growth kinetics and thermodynamics of defect formation. Wide band gap ZnO (Eg = 3.34 eV) and In2O3 (3.7 eV) were also synthesized. ZnO nanowires and nanotubes were successfully doped with a transition metal Fe, making it a Dilute Magnetic Semiconductor of great technological relevance. Structural and electronic characterizations of nanowires were studied for different semiconducting, metallic and semi-metallic nanowires. Electron transport measurements were used to estimate intrinsic material parameters like carrier concentration and mobility. An efficient gas sensing device using a single In2O3 nanowire was studied and which showed sensitivity to reducing gas like NH3 and oxidizing gas like O2 gas at room temperature. The efficiency of the gas sensing device was found to be sensitive to the nature of contacts as well as the presence of surface states on the nanowire.
Effects of Quantum Coherence and Interference
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Quantum coherence and interference (QCI) is a phenomenon that takes place in all multi-level atomic systems interacting with multiple lasers. In this work QCI is used to create several interesting effects like lasing without inversion (LWI), controlling group velocity of light to extreme values, controlling the direction of propagation through non-linear phase matching condition and for controlling the correlations in field fluctuations. Controlling group velocity of light is very interesting because of many novel applications it can offer. One of the unsolved problems in this area is to achieve a slow and fast light which can be tuned continuously as a function of frequency. We describe a method for creation of tunable slow and fast light by controlling intensity of incident laser fields using QCI effects. Lasers are not new to the modern world but an extreme ultra-violet laser or a x-ray laser is definitely one of the most desirable technologies today. Using QCI, we describe a method to realize lasing at high frequencies by creating lasing without inversion. Role of QCI in creating correlations and anti-correlations, which are generated by vacuum fluctuations, in a three level lambda system coupled to two strong fields is discussed.
How Cooperative Systems Respond to External Forces
Cooperative interactions permeate through nature, bringing about emergent behavior and complexity. Using a simple cooperative model, I illustrate the mean field dynamics that occur at the critical point of a second order phase transition in the framework of Langevin equations. Through this formalism I discuss the response, both linear and nonlinear, to external forces. Emphasis is placed on how information is transferred from one individual to another in order to facilitate the collective response of the cooperative network to a localized perturbation. The results are relevant to a wide variety of systems, ranging from nematic liquid crystals, to flocks and swarms, social groups, and neural networks.
The Effects of Residual Gases on the Field Emission Properties of ZnO, GaN, ZnS Nanostructures, and the Effects of Light on the Resistivity of Graphene
In this dissertation, I present that at a vacuum of 3×10-7 Torr, residual O2, CO2, H2 and Ar exposure do not significantly degrade the field emission (FE) properties of ZnO nanorods, but N2 exposure significantly does. I propose that this could be due to the dissociation of N2 into atomic nitrogen species and the reaction of such species with ZnO. I also present the effects of O2, CO2, H2O, N2, H2, and Ar residual gas exposure on the FE properties of GaN and ZnS nanostructure. A brief review of growth of ZnO, GaN and ZnS is provided. In addition, Cs deposition on GaN nanostructures at ultra-high vacuum results in 30% decrease in turn-on voltage and 60% in work function. The improvement in FE properties could be due to a Cs-induced space-charge layer at the surface that reduces the barrier for FE and lowers the work function. I describe a new phenomenon, in which the resistivity of CVD-grown graphene increases to a higher saturated value under light exposure, and depends on the wavelength of the light—the shorter the wavelength, the higher the resistivity. First-principle calculations and theoretical analysis based on density functional theory show that (1) a water molecule close to a graphene defect is easier to be split than that of the case of no defect existing and (2) there are a series of meta-stable partially disassociated states for an interfacial water molecule. Calculated disassociation energies are from 2.5 eV to 4.6 eV, that match the experimental observation range of light wavelength from visible to 254 nm UV light under which the resistivity of CVD-grown graphene is increased.
Synthesis, Characterization, Structural, and Optical Properties of Zinc Oxide Nanostructures Embedded in Silicon Based Substrates
Structural and optical properties of ZnO nanostructures synthesized by low energy ion implantation technique were examined. ZnO molecular ions were implanted into Si/SiO2 substrates at room temperature and then furnace annealed under different temperatures and environments. In all as-implanted samples only Zn nanostructures with varying diameters distributed into the Si/SiO2 matrices were observed. No trace of ZnO was found. The distributions of Zn nanostructures in Si/SiO2 closely matched results from Stopping and Range of Ions in Matter (SRIM) simulations. During annealing at 750 oC, Zn diffused both toward and away from the surface of the substrate and combine with oxygen to form ZnO nanostructures. At higher annealing temperatures ZnO bonding started to break down and transfer to zinc silicate (Zn2SiO4), and at 900 oC the ZnO was completely converted into Zn2SiO4. The average sizes of Zn/ZnO nanostructures depended on the ion fluence. If the fluence increased the average sizes of nanostructures also increased and vice versa. For room temperature photoluminescence (RT-PL), band-edge emission in the ultraviolet (UV) region was observed from all samples annealed at 700 oC/750 oC and were slightly blue shifted as compare to bulk ZnO. Donor-bound exciton (D,X) and acceptor-bound exciton (A,X) transitions were observed in low temperature photoluminescence (PL). The lifetime of both donor-bound excitonic emission (D, X) and acceptor-bound excitonic emission (A, X) were found to be in the picosecond (ps) range.
An Electro- Magneto-static Field for Confinement of Charged Particle Beams and Plasmas
A system is presented that is capable of confining an ion beam or plasma within a region that is essentially free of applied fields. An Artificially Structured Boundary (ASB) produces a spatially periodic set of magnetic field cusps that provides charged particle confinement. Electrostatic plugging of the magnetic field cusps enhances confinement. An ASB that has a small spatial period, compared to the dimensions of a confined plasma, generates electro- magneto-static fields with a short range. An ASB-lined volume thus constructed creates an effectively field free region near its center. It is assumed that a non-neutral plasma confined within such a volume relaxes to a Maxwell-Boltzmann distribution. Space charge based confinement of a second species of charged particles is envisioned, where the second species is confined by the space charge of the first non-neutral plasma species. An electron plasma confined within an ASB-lined volume can potentially provide confinement of a positive ion beam or positive ion plasma. Experimental as well as computational results are presented in which a plasma or charged particle beam interact with the electro- magneto-static fields generated by an ASB. A theoretical model is analyzed and solved via self-consistent computational methods to determine the behavior and equilibrium conditions of a relaxed plasma. The equilibrium conditions of a relaxed two species plasma are also computed. In such a scenario, space charge based electrostatic confinement is predicted to occur where a second plasma species is confined by the space charge of the first plasma species. An experimental apparatus with cylindrical symmetry that has its interior surface lined with an ASB is presented. This system was developed by using a simulation of the electro- magneto-static fields present within the trap to guide mechanical design. The construction of the full experimental apparatus is discussed. Experimental results that show the characteristics of electron beam transmission through the experimental apparatus are presented. A description of the experimental hardware and software used for trapping a charged particle beam or plasma is also presented.
Novel Semi-Conductor Material Systems: Molecular Beam Epitaxial Growth and Characterization
Semi-conductor industry relies heavily on silicon (Si). However, Si is not a direct-band gap semi-conductor. Consequently, Si does not possess great versatility for multi-functional applications in comparison with the direct band-gap III-V semi-conductors such as GaAs. To bridge this gap, what is ideally required is a semi-conductor material system that is based on silicon, but has significantly greater versatility. While sparsely studied, the semi-conducting silicides material systems offer great potential. Thus, I focused on the growth and structural characterization of ruthenium silicide and osmium silicide material systems. I also characterized iron silicon germanide films using extended x-ray absorption fine structure (EXAFS) to reveal phase, semi-conducting behavior, and to calculate nearest neighbor distances. The choice of these silicides material systems was due to their theoretically predicted and/or experimentally reported direct band gaps. However, the challenge was the existence of more than one stable phase/stoichiometric ratio of these materials. In order to possess the greatest control over the growth process, molecular beam epitaxy (MBE) has been employed. Structural and film quality comparisons of as-grown versus annealed films of ruthenium silicide are presented. Structural characterization and film quality of MBE grown ruthenium silicide and osmium silicide films via in situ and ex situ techniques have been done using reflection high energy electron diffraction, scanning tunneling microscopy, atomic force microscopy, cross-sectional scanning electron microscopy, x-ray photoelectron spectroscopy, and micro Raman spectroscopy. This is the first attempt, to the best of our knowledge, to grow osmium silicide thin films on Si(100) via the template method and compare it with the regular MBE growth method. The pros and cons of using the MBE template method for osmium silicide growth are discussed, as well as the structural differences of the as-grown versus annealed films. Future perspectives include further studies on other semi-conducting silicides material systems in terms of growth optimization and characterization.
Field Dependence of Optical Properties in Quantum Well Heterostructures Within the Wentzel, Kramers, and Brillouin Approximation
This dissertation is a theoretical treatment of the electric field dependence of optical properties such as Quantum Confined Stark (QCS) shifts, Photoluminescence Quenching (PLQ), and Excitonic Mixing in quantum well heterostructures. The reduced spatial dimensionality in heterostructures greatly enhances these optical properties, more than in three dimensional semiconductors. Charge presence in the quantum well from doping causes the potential to bend and deviate from the ideal square well potential. A potential bending that varies as the square of distance measured from the heterostructure interfaces is derived self-consistently. This potential is used to solve the time-independent Schrodinger equation for bound state energies and wave functions within the framework of the Wentzel, Kramers, and Brillouin (WKB) approximation. The theoretical results obtained from the WKB approximation are limited to wide gap semiconductors with large split off bands such as gallium arsenide-gallium aluminum arsenide and indium gallium arsenide—indium phosphide. Quantum wells with finite confinement heights give rise to an energy dependent WKB phase. External electric and magnetic fields are incorporated into the theory for two different geometries. For electric fields applied perpendicular to the heterostructure multilayers, QCS shifts and PLQ are found to be in excellent agreement with the WKB calculations. Orthogonality between electrons and holes gives rise to interband mixing in the presence of an external electric field. On the contrary, intraband mixing between light and heavy holes is not sufficiently accounted for in the WKB approximation.
L-shell X-ray production cross sections of ₂₉Cu, ₃₂Ge, ₃₇Rb, ₃₈Sr, and ₃₉Y and M-shell X-ray production cross sections of ₇₉Au, ₈₂Pb, ₈₃Bi, ₉₀Th, and ₉₂U by 70-200 keV protons
L-shell x-ray production cross sections have been measured for thin targets of 29Cu, 32Ge, 37Rb, 38Sr, and 39Y. M-shell x-ray production cross sections have been measured for thin targets of 79Au, 82Pb, 83Bi, 90Th, and 92U. All targets were irradiated with a beam of H+ ions with energies in a range from 70 to 200 keV. Experimental cross sections are compared to other measurements at higher energies and to first Born (Plane Wave Born Approximation for direct ionization and Oppenheimer-Brinkman-Kramers-Nikolaev approximation for electron capture) and the ECPSSR (Energy loss, Coulomb deflection, Perturbed Stationary State calculations with Relativistic effects) theoretical cross sections.
Detection of the Resonant Vibration of the Cellular Membrane Using Femtosecond Laser Pulses
An optical detection technique is developed to detect and measure the resonant vibration of the cellular membrane. Biological membranes are active components of living cells and play a complex and dynamic role in life processes. They are believed to have oscillation modes of frequencies in the range of 1 to 1000 GHz. To measure such a high-frequency vibration, a linear laser cavity is designed to produce a train of femtosecond pulses of adjustable repetition rate. The method is then directly applied to liposomes, "artificial membrane", stained with a liphophilic potential sensitive dye. The spectral behavior of a selection of potential sensitive dyes in the membrane is also studied.
Microwave Spectra of ¹³C Isotopic Species of Methyl Cyanide in the Ground, v₈=1 and v₈=2 Vibrational States
The problem of the quadrupole interaction occurring in a vibrating-rotating C₃v symmetric top molecule has been studied in detail. The quadrupole interaction has been treated as another perturbation term to a general frequency expression accounting for the vibrating-rotating interaction of the molecule so that a complete frequency formula is obtained for both interactions, and from which hyperfine spectral components are predicted and measured. The hyperfine transitions in the ground, and v₈=1 and v₈=2 excited vibrational states of the ¹³C isotopes of methyl cyanide have been investigated in the frequency range 17-72 GHz, primarily in the low J transitions (0≤J≤3). The study of the ground state of isotope i3CH3i3CN, and the v₈=1, v₈=2 excited vibrational states for all the isotopes have been conducted here for the first time. A substantial perturbation has been discovered and discussed at the ΔJ=3→4 transitions within the Kl=1 sets in the v₈=1 mode for isotopes ¹³CH₃CN and CH₃¹³CN. A total of 716 hyperfine transitions have been assigned from measurements, only 7 of which have been measured previously. A total of 84 molecular constants have been reported; 70 of these constants are derived for the first time from microwave data.
Nonlinear Absorption Initiated Laser-Induced Damage in [Gamma]-Irradiated Fused Silica, Fluorozirconate Glass and Cubic Zirconia
The contributions of nonlinear absorption processes to laser-induced damage of three selected groups of transparent dielectrics were investigated. The studied materials were irradiated and non-irradiated fused silica, doped and undoped fluorozirconate glass and cubic zirconia stabilized with yttria. The laser-induced damage thresholds, prebreakdown transmission, and nonlinear absorption processes were studied for several specimens of each group. Experimental measurements were performed at wavelengths of 1064 nm and 532 nm using nanosecond and picosecond Nd:YAG laser pulses. In the irradiated fused silica and fluorozirconate glasses, we found that there is a correlation between the damage thresholds at wavelength λ and the linear absorption of the studied specimens at λ/2. In other words, the laser-induced breakdown is related to the probability of all possible two-photon transitions. The results are found to be in excellent agreement with a proposed two-photon-initiated electron avalanche breakdown model. In this model, the initial "seed" electrons for the formation of an avalanche are produced by two-photon excitations of E' centers and metallic impurity levels which are located within the bandgaps of irradiated Si02 and fluorozirconate glasses, respectively. Once the initial electrons are liberated in the conduction band, a highly absorbing plasma is formed by avalanche impact ionization. The resultant heating causes optical damage. In cubic zirconia, we present direct experimental evidence that significant energy is deposited in the samples at wavelength 532 nm prior to electron avalanche formation. The mechanism is found to be due to formation of color centers (F+ or F° centers) by the two-photon absorption process. The presence of these centers was directly shown by transmission measurements. The two-photon absorption (2PA) process was independently investigated and 2PA coefficients obtained. The accumulated effects of the induced centers on the nonlinear absorption measurements were also considered and the 2PA coefficients were measured using short pulses where this effect is negligible. At room temperature, the color centers slowly diffuse out of the irradiated region. The density of these centers was monitored as a function of time. The initial distribution of the centers was assumed to have a Gaussian profile. For this model the diffusion equation was solved exactly and the diffusion constant obtained.
Coherent Resonant Interaction and Harmonic Generation in Atomic Vapors
This work examines the use of higher order multiphoton resonances in higher harmonic generation together with judicious exploitation of coherent interaction properties to achieve efficient harmonic generation. A detailed experimental study on third harmonic generation in two photon resonant coherent interaction and a theoretical study on four photon resonant coherent interaction have been conducted. Two photon resonant coheren propagation in lithium vapor (2S-4S and 2S-3D interaction) has been studied in detail as a function of phase and delay of the interacting pulse sequence. Under coherent lossless propagation of 90 phase shifted pulse pair, third harmonic generation is enhanced. A maximum energy conversion efficiency of 1% was measured experimentally. This experiment shows that phase correlated pulse sequence can be used to control multiphoton coherent resonant effects. A larger two photon resonant enhancement does not result in more efficient harmonic generation, in agreement with the theoretical prediction. An accurate (to at least 0.5 A°) measurement of intensity dependent Stark shift has been done with the newly developed "interferometric wavemeter." Stark shifts as big as several pulse bandwidths (of picosecond pulses) result in a poor tuning of multiphoton resonance and become a limiting factor of resonant harmonic generation. A complete theory has been developed for harmonic generation in a four photon resonant coherent interaction. A numerical application of the theory to the Hg atom successfully interprets the experimental observations in terms of the phase dependent stimulated Raman scattering. With the intensity required for four photon resonant transition, the calculation predicts a dramatic Stark shift effect which completely destroys the resonance condition. This model provides a basis for the development of future schemes for efficient higher order coherent upconversion.
Two Photon Resonant Picosecond Pulse Propagation in Lithium Vapor
The work of this dissertation has been to prove that the coherence of multiphoton excitation can be studied by an appropriately phased and time delayed sequence of pulses. An application of this fundamental study of coherence has been made for the enhancement of third harmonic generation. The coherent recovery of the energy lost to the two photon absorption process enalled a larger propagation distance for the fundamental than in an interaction which is incoherent or coherent, but not using a 90 degree phase shifted pulse pair. Phase matching over this longer propagation distance gave an enhancement of third harmonic generation.
Dispersion of the Nonlinear Refractive Index of CS₂ in the Spectral Range of 9-11 μm
The nonlinear refractive index (n2) of room temperature liquid CS2 in the wavelength range of 9 to 11 micrometers is measured. A line tunable hybrid C02 TEA laser and amplifier system is used for the experiments. In these measurements the well known photoacoustic method is utilized to observe the onset of whole beam self-focusing. The photoacoustic signal in a CS2 cell, much longer than the confocal parameter, is monitored. The departure of the acoustic signal from linear growth marks the critical power for the onset of nonlinearity. It is experimentally verified that the phenomenon is power dependent as expected from self-focusing theory. The value of n2 is then calculated from the theoretical model of self focusing. Measurements of the on-axis irradiance transmitted through the nonlinear material as well as the measurements of beam distortion are used to verify the validity of the photoacoustic method. In all the measurements the on-axis intensity was smaller than the calculated threshold intensity for stimulated Brillouin scattering. The back reflection was monitored to make sure that stimulated Brillouin scattering was not playing a role in the phenomenon.
Anomalous Behavior in the Rotational Spectra of the v₈=2 and the v₈=3 Vibrations for the ¹³C and ¹⁵N Tagged Isotopes of the CH₃CN Molecule in the Frequency Range 17-95 GHz
The rotational microwave spectra of the three isotopes (^13CH_3^12C^15N, ^12CH_3^13C^15N, and ^13CH_3^13C^15N) of the methyl cyanide molecule in the v_8=3, v_8=2, v_7=1 and v_4=1 vibrational energy levels for the rotational components 1£J£5 (for a range of frequency 17-95 GHz.) were experimentally and theoretically examined. Rotational components in each vibration were measured to determine the mutual interactions in each vibration between any of the vibrational levels investigated. The method of isotopic substitution was employed for internal tuning of each vibrational level by single and double substitution of ^13C in the two sites of the molecule. It was found that relative frequencies within each vibration with respect to another vibration were shifted in a systematic way. The results given in this work were interpreted on the basis of these energy shifts. Large departure between experimentally measured and theoretically predicted frequency for the quantum sets (J, K=±l, ϑ=±1), Kϑ-l in the v_8=3 vibrational states for the ^13c and ^15N tagged isotopes of CH_3CN showed anomalous behavior which was explained as being due to Fermi resonance. Accidently strong resonances (ASR) were introduced to account for some departures which were not explained by Fermi resonance.
Carbon K-Shell X-Ray and Auger-Electron Cross Sections and Fluorescence Yields for Selected Molecular Gases by 0.6 To 2 .0 MeV Proton Impact
Absolute K-shell x-ray cross sections and Auger-electron cross sections are measured for carbon for 0.6 to 2.0 MeV proton incident on CH₄, n-C₄H₁₀ (n-Butane), i-C₄H₁₀ (isobutane), C₆H₆ (Benzene), C₂H₂ (Acetylene), CO and CO₂. Carbon K-shell fluorescence yields are calculated from the measurements of x-ray and Auger-electron cross sections. X-ray cross sections are measured using a variable geometry end window proportional counter. An alternate method is described for the measurement of the transmission of the proportional counter window. Auger electrons are detected by using a constant transmission energy Π/4 parallel pi ate electrostatic analyzer. Absolute carbon K-shell x-ray cross sections for CH₄ are compared to the known results of Khan et al. (1965). Auger-electron cross sections for proton impact on CH₄ are compared to the known experimental values of RΦdbro et al. (1979), and to the theoretical predictions of the first Born and ECPSSR. The data is in good agreement with both the first Born and ECPSSR, and within our experimental uncertainties with the measurements of RΦdbro et al. The x-ray cross sections, Auger-electron cross sections and fluorescence yields are plotted as a function of the Pauling charge, and show significant variations. These changes in the x-ray cross sections are compared to a model based on the number of electrons present in the 2s and 2p sub shells of these carbon based molecules. The changes in the Auger-electron cross sections are compared to the calculations of Matthews and Hopkins. The variation in the fluorescence yield is explained on the basis of the multiconfiguration Dirac-Fock model.
Linear and Nonlinear Optical Techniques to Characterize Narrow Gap Semicondutors: (Hg /Cd)Te and InSb
Several methods have been developed and used to characterize the narrow gap semiconductors Hg^_xCdxTe (HgCdTe) (0.20<x<0.32) and InSb both in the presence of CO2 laser radiation and in the dark. The results have allowed the determination of certain band parameters including the fundamental energy bandgap Eg which is directly related to x, the mole fraction of Cd. In the dark, characterization of several different samples of HgCdTe and InSb were carried out by analyzing the temperature dependence of the Hall coefficient and the magnetic field positions of the magnetophonon extrema from which their x-values were determined. The quality of the magnetophonon spectra is also shown to be related to the inhomogeneity Ax of the HgCdTe samples. One-photon magneto-absorption (OPMA) spectra have been obtained for x ~ 0.2 samples of p-HgCdTe thin films and n-HgCdTe bulk samples. Analysis of the OPMA transition energies allows the x-value to be determined to within « ±0.001. A method is also discussed which can be used to estimate the sample inhomogeneity Ax. Nonlinear optical properties of semiconductors are not only scientifically interesting to study, but are also proving to be technologically important as various nonlinear optical devices are being developed. One of the most valuable nonlinear optical characterization method uses twophoton absorption (TPA). Two techniques using TPA processes were developed and used to measure the cut-off wavelength of several different samples of HgCdTe (x ~ 0.3) from which x-values were determined to within «± 0.0005. Intensity and temperature dependent measurements on impurity and TPA processes have also been carried out and the results are compared with rate equations describing the photo-excited carrier dynamics. These results have yielded important information about the optical and material properties of HgCdTe such as the detection of impurity and trapping levels, TPA coefficients, carrier lifetimes, and recombination mechanisms. TPA and impurity absorption studies were also carried out on n— and p—InSb in order to obtain information about impurity levels, carrier lifetimes, and recombination mechanisms.
Optical Nonlinearities in Semiconductors for Limiting
I have conducted detailed experimental and theoretical studies of the nonlinear optical properties of semiconductor materials useful for optical limiting. I have constructed optical limiters utilizing two-photon absorption along with photogenerated carrier defocusing as well as the bound electronic nonlinearity using the semiconducting material ZnSe. I have optimized the focusing geometry to achieve a large dynamic range while maintaining a low limiting energy for the device. The ZnSe monolithic optical limiter has achieved a limiting energy as low as 13 nJ (corresponding to 300W peak power) and a dynamic range as large as 105 at 532 nm using psec pulses. Theoretical analysis showed that the ZnSe device has a broad-band response covering the wavelength range from 550 nm to 800 nm. Moreover, I found that existing theoretical models (e.g. the Auston model and the band-resonant model using Boltzmann statistics) adequately describe the photo-generated carriers refractive nonlinearity in ZnSe. Material nonlinear optical parameters, such as the two-photon absorption coefficient β_2=5.5cm/GW, the refraction per unit carrier density σ_n=-0.8∗10^-21cm^3 and the bound electronic refraction n_2=-4∗10^-11esu, have been measured via time-integrated beam distortion experiments in the near field. A numerical code has been written to simulate the beam distortion in order to extract the previously mentioned material parameters. In addition, I have performed time-resolved distortion measurements that provide an intuitive picture of the carrier generation process via two-photon absorption. I also characterized the optical nonlinearities in a ZnSe Fabry-Perot thin film structure (an interference filter). I concluded that the nonlinear absorption alone in the thin film is insufficient to build an effective optical limiter, as it did not show a net change in refraction using psec pulses. An innovative numerical program was developed to simulate the nonlinear beam propagation inside the Fabry-Perot structure. For comparison, pump-probe experiments were performed using both thin film and bulk ZnSe. The results showed relatively long carrier lifetimes (>300 psec) in both samples. A numerical code was written to fit the pump-probe experimental results. The fitting yielded that carrier lifetimes (recombination through traps), radiative decay rate, two-photon absorption coefficient as well as the free carrier absorption coefficient for ZnSe bulk material.
A Comprehensive Model for the Rotational Spectra of Propyne CH₃CCH in the Ground and V₁₀=1,2,3,4,5 Vibrational States
The energy states of C₃ᵥ symmetric top polyatomic molecules were studied. Both classical and quantum mechanical methods have been used to introduce the energy states of polyatomic molecules. Also, it is shown that the vibration-rotation spectra of polyatomic molecules in the ground and excited vibrational states can be predicted by group theory. A comprehensive model for predicting rotational frequency components in various v₁₀ vibrational levels of propyne was developed by using perturbation theory and those results were compared with other formulas for C₃ᵥ symmetric top molecules. The v₁₀=1,2,3 and ground rotational spectra of propyne in the frequency range 17-70 GHz have been reassigned by using the derived comprehensive model. The v₁₀=3 and v₁₀=4 rotational spectra of propyne have been investigated in the 70 GHz, and 17 to 52 GHz regions, respectively, and these spectral components assigned using the comprehensive model. Molecular constants for these vibrationally excited states have been determined from more than 100 observed rotational transitions. From these experimentally observed components and a model based upon first principles for C₃ᵥ symmetry molecules, rotational constants have been expressed in a form which enables one to predict rotational components for vibrational levels for propyne up to v₁₀=5. This comprehensive model also appears to be useful in predicting rotational components in more highly excited vibrational levels but data were not available for comparison with the theory. Several techniques of assignment of rotational spectra for each excited vibrational state are discussed. To get good agreement between theory and experiment, an additional term 0.762(J+1) needed to be added to Kℓ=1 states in v₁₀=3. No satisfactory theoretical explanation of this term has been found. Experimentally measured frequencies for rotational components for J→(J+1)=+1 (0≤J≤3) in each vibration v₁₀=n (0≤n≤4) are presented and compared with those calculated using the results of basic perturbation theory. The v₉=2 rotational spectrum of the propyne molecule was introduced in Appendix A to compare the rotational spectra of the same molecule in different vibrational levels v₉ and v₁₀.
K-, L-, and M-Shell X-Ray Production Cross Sections for Beryllium, Aluminum and Argon Ions Incident Upon Selected Elements
Incident 0.5 to 2.5 MeV charged particle beams were used to ionize the inner-shells of selected targets and study their subsequent emission of characteristic x-rays. ⁹Be⁺ ions were used to examine K-shell x-ray production from thin F, Na, Al, Si, P, Cl, and K targets, L-shell x-ray production from thin Cu, An, Ge, Br, Zr and Ag targets, and M-shell x-ray production from thin Pr, Nd, Eu, Dy, Ho, Hf, W, Au, Pb and Bi targets. L-shell x-ray production cross sections were also measured for ²⁷Al⁺ ions incident upon Ni, Cu, Zn, As, Zr, and Pd targets. M-shell x-ray production cross sections were measure for ²⁷Al⁺ and ⁴⁰Ar⁺ ions incident upon Pr, Nd, Gd, Dy, Lu, Hf, Au, Pb, Bi, and U targets. These measurements were performed using the 2.5 MV Van de Graaff accelerator at North Texas State University. The x-rays were detected with a Si(Li) detector whose efficiency was determined by fitting a theoretical photon absorption curve to experimentally measure values. The x-ray yields were normalized to the simultaneously measured Rutherford backscattered (RBS) yields which resulted in an x-ray production cross section per incident ion. The RBS spectrum was obtained using a standard surface barrier detector calibrated for to account for the "pulse height defect." The experimental results are compared to the predictions of both the first Born and ECPSSR theories; each of which is composed of two parts, the direct ionization (DI) of the target electron to the continuum and the capture (EC) of the target electron to the projectile. The first Born describes DI by the Plane-Wave-Born-Approximation (PWBA) and EC by the Oppenheimer-Brinkman-Kramers treatment of Nikolaev (OBKN). ECPSSR expands upon the first Born by using perturbed (PSS) and relativistic (R) target electron wave functions in addition to considering the energy loss (E) of the projectile in the target and its deviation from straight line trajectory (Coulomb deflection (C)). The measurements presented show that the first Born theories overestimate the measured results rather significantly for all experiments using the ⁹Be beams to examine the inner shell x-rays, while the ECPSSR predictions fir the measured data much better. For incident ²⁷Al and ⁴⁰Ar ions, the measured results are not predicted by the theories. The first Born generally over-predicts the data for low target atomic numbers while under-predicting at high atomic numbers. The ECPSSR theory greatly under-predicts the results (factors of 10³ to 10²⁰). Reasons for this behavior are discussed as well as suggestions for future experiments.
The Rotational Spectra of Propyne in the Ground, V₁₀=1, V₁₀=2, and V₉=1 Vibrational States
The problem of a vibrating-rotating polyatomic molecule is treated, with emphasis given to the case of molecules with C_3v symmetry. It is shown that several of the gross features of the rotational spectra of polyatomic molecules in excited vibrational states can be predicted by group theoretical considerations. Expressions for the rotational transition frequencies of molecules of C_3v symmetry in the ground vibrational state, singly excited degenerate vibrational states, and doubly excited degenerate vibrational states are given. The derivation of these expressions by fourth order perturbation theory as given by Amat, Nielsen, and Tarrago is discussed. The ground and V_10=1 rotational spectra of propyne have been investigated in the 17 to 70 GHz, and 17 to 53 GHz regions, respectively, and compared with predictions based on higher frequency measurements. The V_9=1 and V_10=2 rotational spectra of propyne have been investigated and assigned for the first time. A perturbation of the V_9=1 rotational spectra for K=-l has been discovered and discussed.
Nonlinear Absorption Techniques and Measurements in Semiconductors
We have conducted a detailed experimental and theoretical study of nonlinear absorption in semiconductors. Experimental measurements were made on a variety of materials at wavelengths of 1.06 and 0.53 microns using a picosecond Nd:YAG laser. Both two- and three-photon processes were investigated. Values of nonlinear absorption coefficients extracted from these measurements show excellent agreement with recent theory and scaling rules. Our theoretical investigation has been carried out for two-, three-,and n-photon absorption, for both continuous and pulsed sources. Expressions are obtained for the transmission of the sample in terms of the incident irradiance for each case. The physical interpretation of these results is discussed. We have also considered the effects of the photogenerated carriers on the measurements. Equations are developed that include linear absorption by these carriers. We have observed severe distortions on the transmitted beam, caused by changes in the refractive index of the material, due to the presence of these carriers. We present a model that accurately describes these effects in terms of the photogenerated carrier density. We have developed several novel techniques for monitoring nonlinear absorption. In particular, we have adapted the photoacoustic technique to the measurement of nonlinear absorption in semiconductors. We have also developed a technique employing irradiance modulation to greatly enhance the sensitivity to nonlinear processes and simultaneously discriminate against linear background signals. A related technique has been used to observe coherent mixing effects in semiconductors with cw, modelocked dye lasers.
Cooperation-induced Criticality in Neural Networks
The human brain is considered to be the most complex and powerful information-processing device in the known universe. The fundamental concepts behind the physics of complex systems motivate scientists to investigate the human brain as a collective property emerging from the interaction of thousand agents. In this dissertation, I investigate the emergence of cooperation-induced properties in a system of interacting units. I demonstrate that the neural network of my research generates a series of properties such as avalanche distribution in size and duration coinciding with the experimental results on neural networks both in vivo and in vitro. Focusing attention on temporal complexity and fractal index of the system, I discuss how to define an order parameter and phase transition. Criticality is assumed to correspond to the emergence of temporal complexity, interpreted as a manifestation of non-Poisson renewal dynamics. In addition, I study the transmission of information between two networks to confirm the criticality and discuss how the network topology changes over time in the light of Hebbian learning.
Electron Density and Collision Frequency Studies Using a Resonant Microwave Cavity as a Probe
Electron densities and collision frequencies were obtained on a number of gases in a dc discharge at low pressures (0.70-2mm of Hg). These measurements were performed by microwave probing of a filament of the dc discharge placed coaxially in a resonant cavity operating in a TM₀₁₀ mode. The equipment and techniques for making the microwave measurements employing the resonant cavity are described. One of the main features of this investigation is the technique of differentiating the resonance signal of the loaded cavity in order to make accurate measurements of the resonant frequency and half-power point frequencies.
Magnetomorphic Oscillations in Zinc
In making this study it is important to search for ways to enhance and, if possible, make detection of MMO signals simpler in order that this technique for obtaining FS measurements may be extended to other materials. This attempt to improve measurement techniques has resulted in a significant discovery: the eddy-current techniques described in detail in a later section which should allow MMO to be observed and sensitively measured in many additional solids. The second major thrust of the study has been to use the newly discovered eddy-current technique in obtaining the first indisputable observation of MMO in zinc.
Quantum-Confined CdS Nanoparticles on DNA Templates
As electronic devices became smaller, interest in quantum-confined semiconductor nanostructures increased. Self-assembled mesoscale semiconductor structures of II-VI nanocrystals are an especially exciting subject because of their controllable band gap and unique photophysical properties. Several preparative methods to synthesize and control the sizes of the individual nanocrystallites and the electronic and optical properties have been intensively studied. Fabrication of patterned nanostructures composed of quantum-confined nanoparticles is the next step toward practical applications. We have developed an innovative method to fabricate diverse nanostructures which relies on the size and a shape of a chosen deoxyribonucleic acid (DNA) template.
Structural and Photoelectron Emission Properties of Chemical Vapor Deposition Grown Diamond Films
The effects of methane (CH4), diborone (B2H6) and nitrogen (N2) concentrations on the structure and photoelectron emission properties of chemical vapor deposition (CVD) polycrystalline diamond films were studied. The diamond films were grown on single-crystal Si substrates using the hot-tungsten filament CVD technique. Raman spectroscopy and x-ray photoelectron spectroscopy (XPS) were used to characterize the different forms of carbon in the films, and the fraction of sp3 carbon to sp3 plus sp2 carbon at the surface of the films, respectively. Scanning electron microscopy (SEM) was used to characterize the surface morphology of the films. The photoelectron emission properties were determined by measuring the energy distributions of photoemitted electrons using ultraviolet photoelectron spectroscopy (UPS), and by measuring the photoelectric current as a function of incident photon energy.