The goal of this thesis is to engineer the interaction between surface plasmons and semiconductor nanocrystals for nanophotonic applications. Plasmonic metals support surface plasmon polaritons, hybrid photon and electron waves that propagate along a metal-dielectric interface. Unlike photons, surface plasmons can be confined in sub-diffraction geometries. This has two important consequences: 1) optical devices can be designed at the nanoscale, and 2) the high density of electromagnetic fields allows study of enhanced light-matter interactions. Surface plasmons have been exploited to demonstrate components of optoelectronic circuits, optical antennas, surface enhanced spectroscopy, enhanced fluorescence from fluorophores, and nanolasers. Despite the advances, surface plasmon losses limit their propagation lengths to tens of micrometers in the visible wavelengths, hindering many applications. Recently, the template-stripping approach was shown to fabricate metal films that exhibit larger grains and smoother surface, reducing the grain boundary and roughness scattering. To further improve the plasmonic properties, we investigate the importance of deposition conditions in the template-stripping approach. We provide insight and recipes to enhance the plasmonic performance of the most commonly used metals in the ultraviolet, visible, and near-infrared. We also explore the potential of low temperatures to improve the performance of metal films, where the electron-electron and electron-phonon scattering should be reduced. This sets a limit on the minimum loss metals can exhibit. Using this knowledge, we study the optical properties of quantum-confined semiconductor nanocrystals near metal structures. Semiconductor nanocrystals have many attractive characteristics that make them suitable for solid-state lighting and solar cells among others. Specifically, CdSe nanocrystals have been heavily studied for their large absorption and emission cross-sections, size dependent emission wavelengths, photostability, and high quantum yields. Here, we focus on studying the emission from CdSe nanocrystals near plasmonic structures in the weak and strong coupling regimes. In the weak coupling regime, plasmonic structures can be used to selectively modify the radiative rates at the desired wavelengths. We tailor plasmonic structures to enhance and tune the emission from the surface states of CdSe nanocrystals throughout the visible. Due to their size, a significant fraction of atoms are on the surface; however, electron-hole recombination via surface states is typically dark. We further use electrochemistry to probe the energy levels of the surface states. In the strong coupling regime, the energy levels of the surface plasmons and nanocrystals hybridize to form polariton states. In this regime, we demonstrate polariton emission from CdSe/CdSZnS core/shell/shell nanocrystals on silver hole arrays. Emission from these polariton states should be coherent and has implications for thresholdless lasing. While the above studies focus on the change in nanocrystal behavior near metals, these nanocrystals can also be used to improve plasmonic performance. We study the potential of thin layers of CdSe nanocrystals to amplify surface plasmons and enhance their propagation lengths. When the nanocrystals are excited using an external pump, propagating surface plasmons can stimulate emission from these nanocrystals and amplify. If more surface plasmons are generated than lost, then surface-plasmon signals can propagate over extremely long distances and even amplified. We calculate the gain provided and discuss the importance of key parameters such as the absorption and emission cross section, spacer layer thickness, nanocrystal lifetime, and temperature. Finally, we systematically study the emission properties and exciton decay in Ag-doped CdSe nanocrystals, which were recently shown to exhibit enhanced photoluminescence. Overall, this thesis aims to improve plasmonic performance with and without the presence of a gain medium, and advances the understanding of optical behavior of CdSe nanocrystals near metal structures in the weak and strong coupling regimes.
University of Minnesota Ph.D. dissertation. August 2015. Major: Chemical Engineering. Advisors: David Norris, Eray Aydil. 1 computer file (PDF); xi, 189 pages.
Coupling of Surface Plasmons and Semiconductor Nanocrystals for Nanophotonics Applications.
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