Mechanisms and applications of near-field and far-field enhancement using plasmonic nanoparticles




Harrison, Richard K., 1982-

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The resonant interaction of light with metal nanoparticles can result in extraordinary optical effects in both the near and far fields. Plasmonics, the study of this interaction, has the potential to enhance performance in a wide range of applications, including sensing, photovoltaics, photocatalysis, biomedical imaging, diagnostics, and treatment. However, the mechanisms of plasmonic enhancement often remain poorly understood, limiting the design and effectiveness of plasmonics for advanced applications. This dissertation focuses on evaluating the mechanisms of plasmonic enhancement and distinguishing between near and far field effects using simulations and experimental results. Thorough characterization of metal nanoparticle colloids shows that electromagnetic simulations can be used to accurately predict the optical response of nanoparticles only if the true shapes and size distributions are taken into account. By coupling these optical interaction calculations with heat transfer models, experimental limits for the maximum optical power before nanoparticle melting can be found. These limits are important for plasmonic multiphoton luminescence imaging applications. Subsequently, we demonstrate ultrafast laser plasmonic nanoablation of silicon substrates using gold nanorods to identify the near-field enhancement and mechanism of plasmon-assisted ablation. The experimentally observed shape of the ablation region and reduction of the ablation threshold are compared with simulations to show the importance of the enhanced electromagnetic fields in near-field nanoablation with plasmonic nanoparticles. The targeted use of plasmonic nanoparticles requires narrow size distribution colloids, because wide size distributions result in a blurring and weakening of the optical response. A new synthesis method is presented for the seeded-growth of nearly monodisperse metal nanoparticles ranging from 10 to 100 nm in diameter, both with and without dielectric shells of controlled thickness. This method is used to acquire fine control over the position and width of the plasmonic peak response. We also demonstrate self-assembled sub-monolayers of these particles with controllable concentrations, which is ideal for looking at plasmonic effects in surface and layered geometries.
Finally, we present results for the spatial distribution of absorption around plasmonic nanoparticles. We introduce field-based definitions for distinguishing near-field and far-field regions and develop a new set of equations to determine the point-by-point enhanced absorption in a medium around a plasmonic nanoparticle. This set of equations is used to study plasmon-enhanced optical absorption for thin-film photovoltaic cells. Plasmonic nanoparticle systems are identified using simulations and proof-of-concept experiments are used to demonstrate the potential of this approach.



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