In this dissertation we use theoretical, computational, and experimental techniques to investigate the influence of structure and environment on the optical properties of nanoscale silver films. We have focused our study on two types of nanoscale films, those being smooth films with nanoscale thickness and chemically deposited nanostructured films. We examine the excitation of surface plasmon resonances in both types of films and study the sensitivity of these resonances to the film structure and the properties of the surrounding dielectric environment. Using smooth films we discuss the development of methods for measurement of fluid temperature and thermo-optic coefficients based on the sensitivity of surface plasmon excitations to film thickness and permittivity of the adjacent dielectric. We then examine the role of film microstructure in determining the photoluminescent properties of chemically deposited rough silver films. We develop a physical model to describe the chemical deposition process used to fabricate the films. We also develop a Monte Carlo algorithm to simulate the film deposition and test the model. We validate the model and simulations by comparing simulated and measured structural properties of the films across a wide range of film morphologies. We examine the dependence of the ensemble photoluminescence and surface enhanced Raman scattering on the film structure and excitation power. Our experimental and computational study of film growth and morphology allows us to understand how these light emission signals are influenced by the film microstructure. We also discuss how these signals and their sensitivity to the film microstructure and dielectric environment might be exploited for biochemical sensing applications.
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