This work concerns the vacuum deposition of novel thin films that exhibit nonlinear optical effects due to their unusual microstructure. We discuss four different materials: 1) Tilted columns of aluminum-oxide 2) Gold particles in aluminum-oxide 3) Cadmium sulpho-selenide particles in aluminum-oxide 4) Silver particles in zinc-sulphide. We begin with a description of the vacuum system and some the techniques used to characterize the optical and structural properties of the films. This leads to our study of second-harmonic generation (SHG) in aluminum-oxide thin films deposited at an angle to the evaporant source. We show that SHG is very sensitive to the non-isotropic microstructure that results from such a deposition. and the behavior of the SHG signal with sample orientation provides insight to the symmetry properties of the microstructure. In a related study we show that AU/Al₂O₃ composite films produce a large SHG signal. We investigate the dependence of the strength of the SHG signal with fill-fraction of gold and show that it increases quadratically. in agreement with theory. The third material we discuss is cadmium sulpho-selenide doped aluminumoxide. We describe attempts at nucleating semiconductor crystallites in a variety of hosts through a process of co-deposition and subsequent annealing. We also deposit alternate layers of CdS-Se and Al₂O₃ with the semiconductor layer thin enough that interspersed crystallites form. This results in suspended. isolated crystallites similar to the doped-glass materials of interest to nonlinear optics. A waveguide of a CdS/Al₂O₃ "sandwich" demonstrates optical nonlinearity through a power-dependent prism coupling experiment, and the degree of nonlinearity is much greater than undoped glass, though less than doped glass. The final section of the dissertation is a theoretical description of nonlinear optical behavior in a novel composite material consisting of metal particles in a nonlinear dielectric host. We assume the enhanced field around the resonating particles drives the host locally nonlinear through either a Kerr-type or thermal nonlinearity. We calculate the change in optical properties of the medium due to this effect and show that for a system of silver in zinc-sulphide the nonlinearity can be significant.

Using laser pulses of duration comparable to semiconductor relaxation and dephasing times, the coherent phenomena common to two-level systems have been demonstrated in II-VI and III-V semiconductors. These light-matter interactions are characterized by electrons and holes in their initially excited states and/or a macroscopic polarization that persists after the excitation. A nonthermal carrier distribution was observed in bulk CdSe, demonstrating the extremely fast energy relaxation possible when carrier-LO-phonon scattering is included. Quantum-confined CdSe microcrystallites were then employed to limit the available decay avenues. The one and two-pair transitions were characterized, and using spectral hole-burning, energy relaxation was shown to be substantially slower than in bulk. Dipole dephasing remained very rapid. Persistent macroscopic polarization was demonstrated in semiconductors through pump and probe experiments conducted on time scales faster than the inverse linewidth of the exciton. In the first set of experiments, it was found that the exciton optical Stark shift deviates from that predicted by a steady-state theory. The shift is smaller than expected and lasts longer than the pump pulse. Both effects are explained by free evolution of the exciton's polarization. Transient exciton bleaching is observed and shown to be a result of adiabatic following. In a second study of coherent polarization, spectral oscillations at negative delay times were studied. Oscillations were measured in a wide variety of semiconductors, temporally preceding several different pump-probe phenomena. By comparison with a semiclassical theory, it was shown that spectral oscillations in the spectral region of the exciton are evidence of persistent exciton polarization. Oscillations in the band are due to four wave mixing of the pump and probe beams.

Materials in the form of thin films that have been deposited from the vapor phase are significantly different from similar bulk materials, both optically and mechanically, because of their columnar structure and consequent porosity. Their porosity have been verified in different ways. The effects of the pores on optical and mechanical performance and, in particular, the influence of water adsorption, have also been demonstrated. Three techniques used for investigating optical instabilities in thin films are given. They all involve sharp resonances. The resonances are associated either with surface plasmons, metal-dielectric narrowband filters, or all dielectric narrowband filters. These resonances are very sensitive functions of layer properties and hence can be used to detect and measure changes in the layers, particularly those that are induced by adsorption of moisture. Moisture adsorption in thin films is a complex process that occurs unevenly in patches. Using resonance techniques, the adsorption isotherms of change in refractive index, of growth rate in patch size, and of peak wavelength shift, which are all important in characterizing the porosity of films, have been measured. Some effects that locally increase film porosity and create central pores that permit water to penetrate into multilayer structures have been investigated. Based on these results, some suggestions for preventing water adsorption in films are then made. Moisture penetration into thin film structures is the major source of optical coating instability and it is therefore very important that the mechanisms of penetration by understood. Some deductions of the mechanisms are made from the experimental results.

Nonlinear optical properties of passive and active semiconductors are investigated experimentally and theoretically. Improvement of switching cycle time in optical nonlinear etalons to 40 ps is demonstrated, and strained-layer InGaAs/GaAs quantum well material is used in an asymmetric etalon to greatly improve switching power and contrast. Coherent energy transfer (CET) induced by injection of an external light field is demonstrated in a GaAs quantum well vertical-cavity surface-emitting laser (VCSEL). The evolution of CET induced asymmetric gain with increasing injected power is investigated experimentally and theoretically, and it is found that the CET induced effective gain peak and dip are detuned proportionally with injected power as in homogeneously broadened media and in contrast to other multi-wave effects in GaAs which are detuned proportionally with the light field. Transfer of gain modification between orthogonally polarized modes of the VCSEL and cascading of gain modification within a mode is observed and investigated. The approach of a laser to an injection locked state through increased injected power is investigated experimentally and theoretically, showing new emission frequencies produced which evolve to chaos-like behavior before reaching the phase locked state. CET induced gain modification is used to demonstrate low-power high-contrast switching between polarization modes of the VCSEL with differential gain of 3,510. Switching speed and switching bistability is observed and investigated. Injection induced modification of VCSEL transverse modes is studied experimentally and theoretically. Field defects in the resulting field are observed, and their locations are dependent on the frequency of the injected field, in contrast to the temporally evolving defects normally observed. The rich behavior of nonlinear properties, especially in gain media provide interesting results and valuable applications.

We consider in this work the contribution of anisotropic microstructure to polarization effects in thin films. The microstructure is pictured by a simple model as composed of identical columns with elliptical cross section elongated in a direction perpendicular to that of the vapor incidence. The asymmetry in columnar structure that results from oblique deposition is identified as the common source for the significant dichroism and birefringence observed in metal and dielectric films, respectively. A four-dimensional theory for multilayer systems is presented that starts from first principles, unifies previous treatments for particular cases of film anisotropy, and properly handles the most general case of elliptically polarized mode propagation. In this framework and from a set of polarimetric measurements, a simple method is devised, with explicit consideration of the anisotropic microstructure, for the determination of the physical thickness and principal refractive indices of a single dielectric film. A sequence of transmittance measurements is performed with a zirconium oxide film deposited at 65° and, substrate role and instrumental errors considered, good agreement is obtained between theory and experiment. Spectrophotometer data for a narrowband filter with 21 layers deposited at 30° is shown to confirm theoretical predictions of peak positions with Angstrom resolution. A hypothetical metal film is discussed that reproduces the essential features observed in the optical behavior of an aluminum film deposited at 85°. Potential applications and suggestions for future work are included.

The spectral behavior of a cotton canopy with four different soil types inserted underneath, respectively, was examined at various levels of vegetation density. Measured composite spectra, representing mixtures of vegetation with different soil backgrounds were compared with existing measures of greenness, including the NIR-Red band ratios, the perpendicular vegetation index and the green vegetation index. Observed spectral patterns involving constant vegetation amounts with different soil backgrounds could not be explained nor predicted by either the ratio or the orthogonal greenness measures. All greenness measures were found to be strongly dependent on soil brightness. Furthermore, soil-induced greenness changes became greater with increasing amounts of vegetation up to 60% green cover. Three versions of factor analysis were subsequently utilized to determine if soil background influences could be filtered from canopy spectral data sets. In R-mode factor analysis, canopy spectra were decomposed into orthogonal features called brightness and greenness. The greenness feature, however, was found to be dependent, not only on vegetation density, but on soil background spectral properties. Of most concern were soil brightness influences which resulted in lowered greenness values with wet or dark soil backgrounds and identical vegetation conditions. The Q-mode version of factor analysis decomposed canopy spectra into additive, soil and vegetation, reflectance components. Although soil spectral response was found to contribute and mix into the derived greenness measure, significant improvements in vegetation discrimination occurred, especially at low vegetation densities. Finally, the T-mode version of factor analysis successfully separated the spectral influences of soil background from the larger response due to vegetation canopy development. Canopy spectra were decomposed into soil-dependent and soil-independent canopy components. The soil-dependent component was found to resemble the spectral response of green vegetation due to the scattering and transmittance properties of the overlying vegetation canopy. Results showed how the soil-dependent signal mixed into various measures of greenness and hampered vegetation discrimination. The filtering of soil background response from spectral data sets significantly improved greenness indices and vegetation analyses.

The incentive for conducting Degenerate Four Wave Mixing (DFWM) within guided wave devices is two-fold: (1) By coupling the optical beams into guided wave devices, the optical power densities can be increased orders of magnitude due to the tight confinement of the beams. Such an increase in power density means a concomitant increase in conversion efficiency of the signal beam. (2) The potential signal processing applications of DFWM (logic gates, switching, correlation/convolution), particularly for ultra-fast serial processing, would be better exploited, and adjoined to existing integrated circuit technology, by such an integrated optic/guided wave approach. In this dissertation we describe experiments and present data confirming the presence of DFWM within a planar glass thin film with carbon disulphide as the nonlinear cover medium. Optical pulses from a Q-switched, frequency doubled Nd:YAG laser are coupled into the glass film. The nonlinear polarization required to produce the desired conjugate signal is generated within the CS₂ by the evanescent tails of the guided input beams as they probe the nonlinear cover medium. The signals measured agree well with theory, but because they were so small in magnitude, signal-to noise ratios were small due to stray background radiation scattering from beamsplitters and other associated optics. Additionally, recent studies (Jain & Lind, 1983) indicate nonlinear responses in semiconductor (CdS/Se) doped glasses, commercially available as color glass filters, that are orders of magnitude higher than corresponding nonlinearities within CS₂, in addition to possessing subnanosecond response times. We have performed experiments upon such glasses in an effort to fabricate nonlinear optical waveguides within them via ion-exchange techniques. We have successfully fabricated single mode planar guides, but they are currently too lossy to allow demonstration of any guided wave nonlinearities. Also, we describe experiments in which we have measured (bulk) DFWM grating lifetimes with greater precision than previously reported. Results indicate a fast (20 to 50 pico-seconds, depending on the particular glass) electronic response, superimposed upon, but clearly distinguishable from, a slower (10's of nanoseconds) thermal response.

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We established measurement and analysis techniques necessary to investigate the optical properties of some transition metal compounds: specifically the carbides and nitrides of Ti, Zr, and Hf. Two distinct techniques determined the optical constants of these films: a Nestell-Christy method to invert measurements of thickness, reflection, and transmission and a Kramers-Kronig analysis of reflection. The compositions of the samples were evaluated by X-ray diffraction, Auger spectroscopy, scanning electron microprobe analysis, and nuclear analysis. We found it possible to correlate these materials' optical and electronic properties and relate these to compositional changes. The ability to engineer a specific optical response of materials is discussed. Additions of carbon and nitrogen change the optical properties in a specific manner; the roles of these elements as electron donors and their effect on the location and population of the d electron bands with respect to the Fermi level are postulated.