Predicting and verifying the tunable optical properties of metal nanostructures is central to designing materials optimized for specific applications. Chemically- deposited nanostructures have been well-studied near the percolation threshold, but at lower surface coverages they exhibit sample-to-sample variations in the optical response. We identify how these variations are driven by the high variability in the particle size distribution in a particular surface coverage range. We then explore film- coupled nanoparticle systems consisting of a silver nanoparticle, thin dielectric spacer layer, and flat silver film, to enable tuning toward the blue and green parts of the spectrum. We use the boundary element method to visualize charge distributions of various resonances. We fabricate samples using thermal evaporation and spin coating methods, and use polarized reflectance spectroscopy to measure their optical response at an ensemble level. We achieve a 532nm resonance for 80nm silver nanoparticles on 13nm PMMA spacers and 100nm silver thin films. The resulting design is a candidate for enhancing fluorescence in a new spectral range. This dissertation includes previously unpublished co-authored material.

This thesis will explore the ultrafast modulation and optical tunability of plasmonic filters in the terahertz (THz) spectral region. First, the principles and functional design of THz metasurfaces are explored through plasmonic surface lattice resonance interactions and lumped-element circuit models. We will then describe the methodology of generating and detecting THz radiation through the nonlinear processes of optical rectification and electrooptic sampling, respectively. Next, the implementation of a THz time-domain spectroscopy technique is discussed in the context of pump-probe measurements and time-domain resonance analysis. We then show how THz probed materials can be characterized in terms of a temporal and spectral analysis. We will demonstrate how this time-domain technique can allow us to characterize the interaction of plasmonic resonators with optically active substrates and 2D nanomaterials. A completely tunable THz plasmonic notch resonance is modulated utilizing a static and dynamic method of optical tunability in silicon. Active tunability is also demonstrated in a graphene-based plasmonic resonator through the hot carrier multiplication effect. The significance of this work lies in the application of designing controllable devices for future THz communication technologies.