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 …

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 …

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.

This dissertation presents experimental and theoretical studies of transient degenerate four wave mixing (DFWM) in organic dyes. Chapter 1 is an introduction to DFWM. Chapter 2 describes DFWM experiments that were performed in the gain medium of a dye laser. Chapter 3 presents the theory of DFWM of short pulses in three level saturable media. Chapter 4 presents DFWM experiments of femtosecond pulses in the saturable absorber of a passively modelocked ring dye laser. Chapter 5 presents the theory of DFWM of ultrashort pulses in resonant media.

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.

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 …

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 …

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.

A theory is developed to explain the dependence of carrier transport in a thin semiconducting film on film thickness, magnetic field strength, and the dominant bulk scattering mechanism. This theory is based on the solution of the linearized Boltzmann equation in relaxation time form. The semiconductor is assumed to be bounded and nondegenerate with spherical energy surfaces and a scalar effective mass, It is also assumed to be flat banded with totally diffuse scattering at the surface. Classical Boltzmann statistics are used for equilibrium. The dependence of the relaxation time on the carrier energy is approximated by a power law equation. The principle improvement over similar theories is the treatment of the dependence of the relaxation time on carrier energy. The power law approximation for this dependence is valid for randomizing and elastic scattering mechanisms.

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 …

A resonant microwave cavity technique was employed to study the dielectric behavior of some polar and non-polar liquids near the phase transition temperatures at microwave frequencies of 7.2, 9.2 and 10.1 GHz. The Slater perturbation equations for a resonant microwave cavity are briefly discussed to show that the above technique can be used to determine both the real and imaginary parts of dielectric response. Abrupt changes in dielectric response were observed near the phase transition temperatures for the polar liquids studied in this investigation. The dielectric relaxation phenomenon in liquids has been treated as a chemical rate process and the abrupt change in the dielectric response of the liquids near phase transition temperatures is shown to be related to the dramatic changes in the free energy of activation of the molecules. Some values of the free energy of activation were deduced for the various compounds from data obtained in this investigation.