Surface plasmons, due to their extreme sensitivity to changes in refractive indexoccurring at a metal/dielectric interface and their ability to significantly enhanceelectromagnetic fields near a metal, offer exciting opportunities for real-time, fully labelfree forms of chemical/biological detection and field-enhanced applications includingsurface enhanced Raman scattering (SERS), and photovoltaics. Novel classes ofplasmonic crystals fabricated with precisely controlled arrays of subwavelength metalnanostructures provide a promising platform for the sensing and imaging of surfacebinding events with micrometer spatial resolution over large areas. Soft lithography, onefamily of unconventional nanofabrication methods, provides a robust, cost-effective routefor generating highly uniform, functional nanostructures over large areas with molecularscale resolution. This dissertation describes the development and utility of several classesof functional, nanostructured plasmonic materials with predictable optical properties. Anovel, low-cost optical sensor with atomic scale sensitivity at visible wavelength rangewas developed by tuning the optical response of a plasmonic crystal to visiblewavelengths through optimization of the distribution and thickness of the thin metal film.Sensing and imaging of various surface binding events were studied to demonstrate theirutility for label-free detection. Finite-Difference Time-Domain (FDTD) calculations werecarried out to model the optical response of the system and gain insight into the physicsof the system. New classes of plasmonic crystals were developed using new materials andfabrication methods, in concert with rational design of the device form factor guided byboth experiment and computational electrodynamics simulations.
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