The vacuum ultraviolet molecular hydrogen laser is evaluated as a selective ion source for analytical mass spectrometry of easily-ionized compounds. The types of compounds ionized below the photon energy of 7.8 eV include polynuclear aromatic hydrocarbons, and many amines and nitrogen-containing heterocycles. The latter two categories encompass a large number of pharmaceuticals and drugs of abuse. H₂ laser photoionization produces parent molecular ions only, for all compounds studied thus far. Selectivity of the threshold photoionization process is very high, as compounds within as little as 0.2 eV above the threshold are completely rejected. The ability of the technique to discriminate against interfering matrix components is demonstrated for both simple synthetic and complex "real world" mixtures. Easily interpreted spectra are obtained from simple extracts of spiked coffee, beer, soy sauce, urine and blood serum. The most important interference is shown to be electron impact ionization arising from acceleration of stray electrons in the ion source. Most of this ionization is caused by low-energy secondaries generated when stray primaries are collected by the ion source electrodes. The primaries are produced mainly by interaction of scattered laser radiation with metal surfaces. This interference can be controlled through proper instrumental design.

This dissertation is an experimental study of a novel type of interferometry based on the generation of Second Harmonic (SH) light. In this work interferometers are described in which an interference pattern arises when two SH waves are superimposed. These waves come from doubling the fundamental frequency of a laser by means of non-linear crystals. Three interferometers are described that have different applications according to their sensitivity to detect wavefront distortions. One interferometer has low sensitivity and is useful in the contouring of refractive objects that produce large wavefront distortions of the order of hundreds of visible wavelengths. The other two interferometers have high sensitivity and one of them is capable of detecting wavefront distortions as small as 1/20 of wavelength. Special emphasis is placed on development of the first interferometer which is a real-time, common-path, self-referencing interferometer that yields interferograms in the visible. The interferometer is based on the fact that a SH wavefront generated under PM conditions is a faithful replica of the laser wavefront. The two interfering SH wavefronts are produced one before and the other after the object under study, and by virtue of its chromatism, they are very slightly different. Consequently, very low density fringes are produced upon their superposition. In this application, noncritically phase matched crystals perform best, and we have found that Y-cut LiNbO₃ crystals configured for surface acousto-optic applications are very convenient. The conversion efficiencies are very low (of the order of 10⁻⁵) consequently optical damage to the LiNbO₃ due to the SH is no problem. The crystals are phase matched by controlling their temperature and are used with a repetitively pulsed Nd:Yag laser operating at 1.06 μm. The chief limitations of this interferometer come from practical considerations in imaging objects with high spatial frequencies that reduce the contrast of the interferograms. The high sensitivity interferometers make use of the changes of phase and amplitude induced in the SH wavefront by the phase mismatch of angle tuned crystals to provide information. The interferometers are directly sensitive to small wavefront tilts and do not require additional reference wavefronts.

The culmination of a comprehensive experimental study of a number of nonlinear optical materials and their device applications. The optical phenomenology surrounding the interaction of laser radiation with these materials is emphasized. In addition to using interferometric techniques for their investigation and application, the overall theme of the research is the incorporation of interferometric descriptions of these interactions. Interference is commonly regarded to be the domain of linear optics; this work invalidates that notion. Nonlinear optics (NLO) is presented as simply a natural extension of linear optics. After a complete introduction to the general theory and relevant concepts required in the field of NLO, the first half of this manuscript presents a number of studies concerned with second-order nonlinear crystals for laser frequency conversion. The second half of this dissertation presents research on the nonlinear optical properties of semiconductors and semiconductor microstructures for optical-bistability-related applications. Optical bistability and related phenomena made possible using these materials in a nonlinear Fabry-Perot interferometer are stressed.

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