published_or_final_version / Statistics and Actuarial Science / Master / Master of Philosophy

Fluorinated norbornene monomers exhibit the requisite properties for inclusion in 157 nm photoresists, but traditional addition and radical polymerizations with these monomers have failed. Norbornanediols provide an alternate route to these materials via condensation polymerization, and methods have been developed for the efficient synthesis of the exo-2-syn-7- and endo-2-exo-3-dihydroxynorbornanes. Synthesis of the fluorinated analogues is complicated by steric and electronic effects; however, a high-yielding synthesis of endo-2-exo-3-dihydroxynorbornane bearing a 5-endo-[2,2-bis(trifluoromethyl)hydroxyethyl] substituent as well as its corresponding polymer are reported. As an alternative to 157 nm and other optical lithographies, Step and Flash Imprint Lithography, or S-FIL®, was introduced in 1999 by The University of Texas at Austin. It has proven to be a cost effective, high resolution alternative to traditional optical lithography. Often in the S-FIL process, residual resist may become imbedded within the template features resulting in device defects due to the imprint and repeat nature of S-FIL. The high silicon and cross-linking content of the resist formulations are extremely difficult, if not impossible to remove from quartz imprint mold without template degradation. Our approach to this problem was the synthesis of a family of thermally reversible, cross-linkable monomers that will facilitate resist removal while maintaining template integrity. Our monomers utilize classic Diels-Alder chemistry to provide thermal reversibility, while pendant acrylate functionalities facilitate cross-linking. Herein we report the synthesis of several Diels-Alder compounds, incorporate them into resist formulations, and test their efficacy for resist removal. In an effort to develop unique patternable materials, our laboratory is currently engaged in the design and development of photonic crystals comprised of organic elements with highly stable electro-optic activity. Fabrication of these devices requires polymers that can be patterned at high resolution, have large second order nonlinear optical (NLO) coefficients, and that are thermally stable after poling. Our route to these materials involves the synthesis of a prepolymer that can be spin coated, poled, and then fixed by a photochemical cross-linking reaction. We now describe an efficient synthetic route to a new class of biscross-linkable monomers and the characteristics of their corresponding nonlinear optical polymers. / text

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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.

Nonlinear phenomena originating from the distributed coupling process were observed when distributed couplers, such as prisms and gratings, were used to couple light into nonlinear ZnS thin film waveguides. The efficiency of the nonlinear distributed coupling process was found to depend on two independent parameters, the angle of the incident beam and the power of the incident beam. Depending on the detuning of the incident angle, from the optimum incident angle at low powers, either optical limiting, power-dependent switching, or power-dependent bistability of the coupling efficiency, and thereby of the in-coupled power, was observed. At zero detuning, a twenty-fold decrease of the coupling efficiency with increasing powers was measured. At a nonzero detuning of the incident angle, power-dependent switching at milliwatt powers was observed. At larger angular detunings, corresponding to the angular width. FWHM, of the coupling peak at low powers, power-dependent bistability was observed, and the width of the bistability loop was found to increase with increasing detunings. All-optical beam scanning via a nonlinear grating coupler was also demonstrated, utilizing a control-signal beam configuration, where the signal beam scanned through an angle of 0.5° when the power of the control beam was varied. The observed nonlinearity in ZnS was positive and of thermal origin. The power-induced change in the refractive index was found to be 0.01 and a relaxation time of 10 μsec was measured. Problems with the long-term stability of the nonlinear distributed coupling process were traced to the occurrence of desorption and adsorption of water vapor in the ZnS films.

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.