Semiconductor based micro- and nano-structures grown in a systematic and controlled way using selective area growth are emerging as a promising route toward devices for integrated optical circuitry in optoelectronics and photonics field. This dissertation focuses on the experimental investigation of the nonlinear optical effects in selectively grown gallium nitride micro-pyramids that act as optical cavities, zinc oxide submicron rods and indium gallium nitride multiple quantum well core shell submicron tubes on the apex of GaN micro pyramids that act as optical antennae. Localized spatial excitation of these low dimensional semiconductor structures was optimized for nonlinear optical light (NLO) generation due to second harmonic generation (SHG) and multi-photon luminescence (MPL). The evolution of both processes are mapped along the symmetric axis of the individual structures for multiple fundamental input frequencies of light. Effects such as cavity formation of generated light, electron-hole plasma generation and coherent emission are observed. The efficiency and tunability of the frequency conversion that can be achieved in the individual structures of various geometries are estimated. By controlling the local excitation cross-section within the structures along with modulation of optical excitation intensity, the nonlinear optical process generated in these structures can be manipulated to generate coherent light in the UV-Blue region via SHG process or green emission via MPL process. The results show that these unique structures hold the potential to convert red input pulsed light into blue output pulsed light which is highly directional.
Among the well-known methods to form or modify the composition and physical properties of thin films, ion implantation has shown to be a very powerful technique. In particular, ion beam syntheses of binary iron silicide have been studied by several groups. Further, the interests in transition metal silicide systems are triggered by their potential use in advanced silicon based opto-electronic devices. In addition, ternary silicides have been by far less studied than their binary counterparts despite the fact that they have interesting magnetic and electronic properties. In this study, we investigate ion beam synthesis of Fe-Si binary structures and Fe-Co-Si ternary structures. This work involves fundamental investigation into development of a scalable synthesis process involving binary and ternary transitional metal silicide thin films and Nano-structures using low energy ion beams. Binary structures were synthesized by implanting Fe- at 50 keV energy. Since ion implantation is a dynamic process, Dynamic simulation techniques were used in these studies to determine saturation fluences for ion implantation. Also, static and dynamic simulation results were compared with experimental results. The outcome of simulations and experimental results indicate, dynamic simulation codes are more suitable than static version of the TRIM to simulate high fluence, low energy and, heavy ion implantation processes. Furthermore, binary Fe-Si phase distribution was determined at different implantation fluences and annealing temperatures. A higher fluence implantation at 2.16×1017 atoms/cm2 and annealing at 500 oC showed three different Fe-Si phase formations (β-FeSi2, FeSi and Fe3Si) in substrate. Further, annealing the samples at 800 oC for 60 minutes converted the Fe3Si phase into FeSi2 and FeSi phases. As an extension, a second set of Fe- ion implantations was carried with the same parameters while the substrate was placed under an external magnetic field. External magnetic fields stimulate the formation of magnetic phase centers in the ...
In this work, we study the use of a spatial light modulator (SLM) for local manipulation of phase in interfering laser beams to fabricate photonic crystal templates with embedded, engineered defects. A SLM displaying geometric phase patterns was used as a digitally programmable phase mask to fabricate 4-fold and 6-fold symmetric photonic crystal templates. Through pixel-by-pixel phase engineering, digital control of the phases of one or more of the interfering beams was demonstrated, thus allowing change in the interference pattern. The phases of the generated beams were programmed at specific locations, resulting in defect structures in the fabricated photonic lattices such as missing lattice line defects, and single-motif lattice defects in dual-motif lattice background. The diffraction efficiency from the phase pattern was used to locally modify the filling fraction in holographically fabricated structures, resulting in defects with a different fill fraction than the bulk lattice. Through two steps of phase engineering, a spatially variant lattice defect with a 90° bend in a periodic bulk lattice was fabricated. Finally, by reducing the relative phase shift of the defect line and utilizing the different diffraction efficiency between the defect line and the background phase pattern, desired and functional defect lattices can be registered into the background lattice through direct imaging of the designed phase patterns.
We investigate the conditions under which electron irradiation of single-walled carbon nanotube (SWCNT) bundles with 2 keV electrons produces an increase in the Raman D peak. We find that an increase in the D peak does not occur when SWCNTs are preheated in situ at 600 C for 1 h in ultrahigh vacuum (UHV) before irradiation is performed. Exposing SWCNTs to air or other gases after preheating in UHV and before irradiation results in an increase in the D peak. Small diameter SWCNTs that are not preheated or preheated and exposed to air show a significant increase in the D and G bands after irradiation. X-ray photoelectron spectroscopy shows no chemical shifts in the C1s peak of SWCNTs that have been irradiated versus SWCNTs that have not been irradiated, suggesting that the increase in the D peak is not due to chemisorption of adsorbates on the nanotubes.
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 ...
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.
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 ...
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.
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.
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 ...
We perform high precision measurements of an isotope shift between the two stable isotopes of helium. We use laser excitation of the 2^3 S_1-2^3 P_0 transition at 1083 nm in a metastable beam of 3He and 4He atoms. A newly developed tunable laser frequency selector along with our previous electro-optic frequency modulation technique provides extremely reliable, adaptable, and precise frequency and intensity control. The intensity control contributes negligibly to overall experimental uncertainty by stabilizing the intensity of the required sideband and eliminating the unwanted frequencies generated during the modulation of 1083 nm laser carrier frequency. The selection technique uses a MEMS based fiber switch and several temperature stabilized narrow band (~3 GHz) fiber gratings. A fiber based optical circulator and an inline fiber amplifier provide the desired isolation and the net gain for the selected frequency. Also rapid (~2 sec.) alternating measurements of the 2^3 S_1-2^3 P_0 interval for both species of helium is achieved with a custom fiber laser for simultaneous optical pumping. A servo-controlled retro-reflected laser beam eliminates residual Doppler effects during the isotope shift measurement. An improved detection design and software control makes negligible subtle potential biases in the data collection. With these advances, combined with new internal and external consistency checks, we are able to obtain results consistent with the best previous measurements, but with substantially improved precision. Our measurement of the 2^3 S_1-2^3 P_0 isotope shift between 3He and 4He is 31 097 535.2 (5) kHz. The most recent theoretic calculation combined with this measurement yields a new determination for nuclear size differences between 3He and 4He: ∆r_c=0.292 6 (1)_exp (8)_th (52)_exp fm, with a precision of less than a part in 〖10〗^4 coming from the experimental uncertainty (first parenthesis), and a part in 〖10〗^3 coming from theory. This value is consistent with electron scattering ...
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.
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.
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).
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 ...
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.
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.
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.
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.
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 ...
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.
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.
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.
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.
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.
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.
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 Hartree-Fock-Bogoliubov theory of homogeneous boson systems at finite temperatures is rederived using, a free energy variational principle. It is shown that a t-matrix naturally emerges in the theory. Phenomenological modifications are made (1) to remove the energy gap at zero momentum, and (2) to eliminate the Hartree-Fock-like terms, which dress the kinetic energy of the particle. A numerical calculation of the energy spectrum is made over a temperature range of 0.00 to 3.14 K using the Morse dipole-dipole-2 potential and the Frost-Musulin potential. The energy spectrum of the elementary excitations is calculated self-consistently. It has a phonon behavior at low momentum and a roton behavior at higher momentum, so it is in qualitative agreement with the observed energy spectrum of liquid He II. However, the temperature dependence of the spectrum is incorrectly given. At the observed density of 0.0219 atoms A-3, the depletion of the zero-momentum state at zero temperature is 40.5% for the Morse dipole-dipole-2potential, and 43.2% for the Frost- Musulin potential. The depletion increases gradually until at 3.14 K the zero momentum density becomes zero discontinuously, which indicates a transition to the ideal Bose gas.
The frequency shifts and Q changes of a resonant microwave cavity were utilized as a basis for determining microwave properties of solids and liquids. The method employed consisted of varying the depth of penetration of a cylindrical sample of the material into a cavity operating in the TM0 1 0 Mode. The liquid samples were contained in a thin-walled quartz tube. The perturbation of the cavity was achieved by advancing the sample into the cavity along the symmetry axis by employing a micrometer drive appropriately calibrated for depth of penetration of the sample. A differentiation method was used to obtain the half-power points of the cavity resonance profile at each depth of penetration. The perturbation techniques for resonant cavities were used to reduce the experimental data obtained to physical parameters for the samples. The probing frequency employed was near 9 gHz.
The K-shell x-ray and ionization cross sections are measured for protons on Ag, Cd, Sn, Sb, Te, Ba, and La over the ion energy range of 0.6 to 2.0 MeV. The data are compared to the predictions of the PWBA, the PWBA with corrections for binding energy and/or Coulomb deflection, the BEA, and the constrained BEA predictions. In general, the non-relativistic PWBA with binding energy correction gives the best overall agreement with the measurements of proton-induced x-ray processes for the K-shell of the elements studied in this work. The data further suggest the need for relativistic PWBA treatment of the interactions in the K-shell for the range of binding energies represented by the elements investigated in this work.
The gauge-invariant formulation of quantum mechanics is compared to the conventional approach for the case of a one-dimensional charged harmonic oscillator in an electromagnetic field in the electric dipole approximation. The probability of finding the oscillator in the ground state or excited states as a function of time is calculated, and the two approaches give different results. On the basis of gauge invariance, the gauge-invariant formulation of quantum mechanics gives the correct probability, while the conventional approach is incorrect for this problem. Therefore, expansion coefficients or a wave function cannot always be interpreted as probability amplitudes. For a physical interpretation as probability amplitudes the expansion coefficients must be gauge invariant.
The problem with which this investigation is concerned is that of demonstrating the applicability of a particular theory and technique to two materials of different band structure, InSb and HgSe, and in doing so, determining the deformation potentials of these materials. The theory used in this investigation predicts an inversion-asymmetry splitting and an anisotropy of the Fermi surface under uniaxial stress. No previous studies have ever verified the existence of an anisotropy of the Fermi surface of semiconductors under stress. In this work evidence will be given which demonstrates this anisotropy. Although the inversion-asymmetry splitting parameter has been determined for some materials, no value has ever been reported for InSb. The methods presented in this paper allow a value of the splitting parameter to be determined for InSb.
This thesis relates a technique for increasing the optical strength of NaCl and KCl single-crystal samples. The 1.06-μm pulsed laser damage thresholds were increased by factors as large as 4.6 for a bulk NaCl single-crystal sample. The bulk laser damage breakdown threshold (LDBT) of the crystal was measured prior to and after heat treatment at 800*C using a Nd:YAG laser operating at 1.06 μm. Bulk and surface LDBTs were also studied on samples annealed at 400° C. These samples showed differences in damage morphology on both cleaved and polished surfaces, and the cleaved surfaces had improved damage thresholds. However, neither the polished surfaces nor the bulk showed improved threshold at the lower annealing temperature.
The Bogoliubov theory of excitations in superfluid helium is used to study collective modes at zero temperature. A repulsive delta function shell potential is used in the quasiparticle excitation energy spectrum to fit the observed elementary excitation spectrum, except in the plateau region. The linearized equation of motion method is used to obtain the secular equation for a collective mode consisting of a linear combination of one and two free quasiparticles of zero total momentum. It is shown that in this case for high-lying collective modes, vertices involving three quasiparticles cancel, and only vertices involving four quasiparticles are important. A decomposition into various angular momentum states is then made. Bound roton pairs in the angular momentum D-state observed in light-scattering experiments exist only for an attractive coupling between helium atoms in this oversimplified model. Thus, the interaction between particles can be reinterpreted as a phenomenological attractive coupling between quasiparticles, in order to explain the Raman scattering from bound roton pairs in superfluid helium.
Characteristic L-shell x rays of the five rare earths Pr, Sm, Eu, Gd, and Dy were studied in this work. The x rays were produced by ionization from 0.3 to 2.0 MeV protons from the 2.0 MV Van de Graaff at North Texas State University. Total L-shell ionization and x-ray production cross sections were measured for Sm and compared to the BEA, CBEA and PWBA theories. Total L-shell ionization cross sections were measured for Pr, Eu, Gd, and Dy and compared to the BEA, CBEA, and PWBA. The CBEA and PWBA fit the samarium data well for both ionization and x-ray production cross sections. The BEA was generally 40 per cent lower than the data. The CBEA and the PWBA also fit the ionization cross section data for Pr, Eu, Gd and Dy, while the BEA was generally 40 per cent lower than the data.
The problem with which this investigation is concerned is that of making experimental measurements of proton-induced K-shell x-ray production cross sections and to study the dependence of these cross sections upon the energy of the incident proton. The measurements were made by detection of the characteristic x-rays emitted as a consequence of the ionization of the K-shell of the atom. The method for relating this characteristic x-ray emission to the x-ray production cross section is discussed in this work.
A source-modulation microwave spectrograph was utilized to measure line width parameters for several spectral lines in the pure rotational spectrum of formaldehyde (H₂CO). The spectrograph featured high-gain ac amplification and phase-sensitive detection, and was capable of measuring microwave lines having absorption coefficients as small as 10⁻⁷ cm⁻¹ with a frequency resolution on the order of 30 kHz. Center frequencies of the measured lines varied from 4,830 MHz to 72,838 MHz; hence, most of the observations were made on transitions between K-doublets in the rotational spectrum. Corrections were applied to the measured line width parameters to account for Doppler broadening and, where possible, for deviations due to magnetic hyperfine structure in some of the K-doubled lines. Low modulation voltages and low microwave power levels were used to minimize modulation and saturation broadenings; other extraneous broadenings were found to be insignificant. The primary broadening mechanism at low gas pressure is pressure broadening, and a review of this topic is included. Line width parameters for the several observed transitions were determined by graphing half-widths versus pressure for each spectral line, and performing a linear least-squares fit to the data points. Repeatability measurements indicated the accuracy of the line width parameters to be better than ±10 percent. The reasons for this repeatability spread are discussed, Broadening of each line was measured for self- and foreign-gas broadening by atomic helium and diatomic hydrogen. Effective collision diameters were calculated for each broadening interaction, based on the observed rates of broadening.
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.
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 ...
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.
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.
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.
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.
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 ...
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.
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.
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.
L- and M-shell x-ray production cross sections have been measured for thin solid targets of neodymium, gadolinium, holmium, ytterbium, gold, and lead by 25 MeV 12/6C^q+ (q=4,5,6) and by 32 MeV 16/8O^q+ (q=5,7,8). The cross sections were determined from measurements made with thin targets (< 2.5 μg/cm2). For projectiles with one or two K-shell vacancies, the target x-ray production cross sections were found to be enhanced over those for projectiles without a K-shell vacancy. The sum of direct ionization to the continuum (DI) plus electron capture (EC) to the L, M, N... shells and EC to the K-shell of the projectile have been extracted from the data. The results are compared to the predictions of first Born theories, i.e., plane wave Born approximation for DI and Oppenheimer-Brinkman-Kramers formula of Nikolaev for EC and to the ECPSSR approach that accounts for Energy loss and Coulomb deflection of the projectile as well as for Relativistic and Perturbed Stationary States of inner shell electrons.
A pair of nonidentical two-level atoms, separated by a fixed distance R, interact through photon exchange. The system is described by a state vector which is assumed to be a superposition of four "essential states": (1) the first atom is excited, the second one is in the ground state, and no photon is present, (2) the first atom is in its ground state, the second one is excited, and no photon is present, (3) both atoms are in their ground states and a photon is present, and (4) both atoms are excited and a photon is also present. The system is initially in state (1). The probabilities of each atom being excited are calculated for both the minimally-coupled interaction and the multipolar interaction in the electric dipole approximation. For the minimally-coupled interaction Hamiltonian, the second atom has a probability of being instantaneously excited, so the interaction is not retarded. For the multipolar interaction Hamiltonian, the second atom is not excited before the retardation time, which agrees with special relativity. For the minimally-coupled interaction the nonphysical result occurs because the unperturbed Hamiltonian is not the energy operator in the Coulomb gauge. For the multipolar Hamiltonian in the electric dipole approximation the unperturbed Hamiltonian is the energy operator. An active view of unitary transformations in nonrelativistic quantum electrodynamics is used to derive transformation laws for the potentials of the electromagnetic field and the static Coulomb potential. For a specific choice of unitary transformation the transformation laws for the potentials are used in the minimally-coupled second-quantized Hamiltonian to obtain the multipolar Hamiltonian, which is expressed in terms of the quantized electric and magnetic fields.
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.
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