The purpose of this thesis is to make a broadband antireflection coating configuration known as a quarter-wave stack consisting of one layer of titania and of one layer of silica nanoparticles. We utilize much that is already known about silica nanoparticle deposition. The first objective of this thesis is deposition and characterization of titania nanoparticle films deposited on glass microscope slides by a technique known as Ionic Self-Assembled Multilayers or ISAM deposition. This technique takes advantage of the electrostatic attraction between oppositely charged materials and ideally results in a uniform nanoparticle film whose thickness and optical properties can be tightly controlled. Deposition of a quarter-wave stack based on ISAM deposition of silica and titania nanoparticles is significantly simpler and less expensive than alternative deposition methods. Initial attempts to deposit titania films were unsuccessful because of excess diffuse scattering due to inhomogeneities in the film. In order to reduce diffuse scattering, two approaches were considered. The first approach was to improve the deposition process itself by experimenting with different values of deposition parameters such as solution pH and solution molarity. The other approach focused on removing the large nanoparticle aggregates from the colloidal solutions of titania nanoparticles that were suspected to be responsible for rough film surfaces resulting in diffuse scattering. This approach was successful. In addition, evidence suggested that surface roughness contributed more to diffuse scattering than the bulk of the films. After minimizing diffuse scattering from titania nanoparticle films, we used known results from research on silica nanoparticle films to deposit quarter-wave stacks consisting of one layer of titania nanoparticles with high refractive index and one layer of silica nanoparticles with low refractive index. This contrast in refractive indices is a desirable characteristic of quarter-wave stacks. The thicknesses and refractive indices of the two layers in the quarter-wave stacks were measured by ellipsometry and compared to the nominal thicknesses of these layers. Finally, the reflectance was derived from a model of the quarter-wave stack and was compared to the measured reflectance. It was found that construction of a quarter-wave stack by ISAM is possible but that it will be necessary to acquire data from more experiments. / Ph. D.

This thesis presents the characterization of the optical and mechanical properties of silica nanoparticle films fabricated by ionic self-assembly, also known as layer-by-layer (LbL) deposition. Utilizing electrostatic attraction of oppositely-charged materials permits uniform and rapid growth of the constituents onto planar and curved surfaces. In this work, silica nanoparticles are adsorbed onto glass and polycarbonate substrates, as well as micron-scale glass fibers, with the purpose of improving the optical quality of the respective media. Several methods are presented to improve the adhesion and cohesion of silica nanoparticle films on glass substrates. In the first method, the substrate and nanoparticle surfaces are coated with materials containing sulfonate end groups. Next, a photo-reactive polycation known as diazo-resin (DAR) is used in ISAM deposition with the modified silica nanoparticles. Subsequent exposure to UV converts the ionic bonds between the DAR and sulfonate groups into covalent ones. The second method to improve the mechanical strength is to heat the ISAM silica nanoparticle film at a high enough temperature (500 °C) to remove the polymer and partially fuse the nanoparticles. This technique is known as calcination and is shown to significantly improve the mechanical robustness of the film without compromising the optical properties. The final method involves the deposition of precursor and capping polymer layers around bulk silica nanoparticle films with both bilayer and quadlayer designs. The addition of these polymer layers improves the surface contact between adjacent nanoparticles but reduces the film porosity and consequently the optical transparency. Currently the calcination technique is the only one that significantly improves the film adhesion and cohesion, but suggestions are offered to potentially improve the performance of films made by the other two methods. An alternative way to functionalize polycarbonate substrates for silica nanoparticle ISAM deposition is also presented. The molecular structure of polycarbonate at the surface can be modified by exposing it to deep UV (λ = 185, 254 nm). By doing so, the surface becomes populated with carboxylate species, and thus permits ISAM deposition of poly(allylamine hydrochloride) (PAH) and silica nanoparticles. A variety of spectroscopic methods show that the molecular structure is changed by this procedure, and SEM shows that UV treatment improves the uniformity of ISAM films on polycarbonate. Finally, PAH/silica nanoparticle ISAM films are deposited onto glass fibers. The fibers are used for mechanical reinforcement of polymer composite optical media. The role of the nanoparticle film on the fibers is to reduce light scattering at the interfaces of materials with different thermo-optic coefficients, in other words, transmittance losses associated with changes in temperature. Fiber bundles coated with silica nanoparticles suffer from unacceptable levels of aggregation, and hence do not currently improve the transmittance over the temperature spectrum. Some evidence is presented, however, to suggest that the transparency can be improved if fiber aggregation during ISAM deposition can be avoided. / Ph. D.