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Plasmonic core-multi-shell nanomaterials for improving energy efficiency and sensingDutta, Amartya 22 January 2021 (has links)
In recent times, plasmonics has been a hallmark in improving optoelectronic device performance as well as in improving sensing. Confining light in dimensions below the diffraction limit and subsequently converting the incident photons into localized charge-density oscillations called localized surface plasmons, optical enhancements of the local fields by many orders of magnitude is possible. This dissertation explores the use of such surface plasmon resonances in core multishell nanostructures and demonstrates the values of such structures in energy harvesting and sensing. Additionally, it also shows the use of emerging plasmonic materials like metal nitrides (TiN, ZrN) instead of traditional plasmonic materials (Au, Ag) in the nanostructure designs.
Utilizing the localized surface plasmon resonance (LSPR) in metallic components of core multishell nanowires, calculations of the local density of states as a measure of emission were made using a Green’s function method, while the absorption and scattering were simulated using the Mie formalism. Combining both the absorption and the emission, the quantum efficiency of white LEDs was calculated and the optimal material/dimensions for maximal performance was determined for different phosphor components in a white LED. Additionally, the use of ZrN as a plasmonic cloak for noise cancellation in Si photodetectors is shown and the performance is compared with an Au cloak. Using the developed methodology, it is proved that ZrN cloaks can outperform Au cloaks in a certain region of the visible spectrum, showing the benefit of using such plasmonic systems in place of traditional materials. The fabrication of the different components of the core multishell nanowires is also presented, and in particular, fabrication of ultra-thin (sub-10 nm) plasmonic TiN is achieved.
Utilizing plasmon hybridization, a tunable double resonance feature is observed in Au/SiO2/Au core shell shell (CSS) nanoparticles, which have been then demonstrated to improve the photocatalytic performance in hematite. In particular, the double resonance peak allows absorption of light beyond the band gap of hematite and subsequent conversion into photocurrent through hot electron injection. Comparison has been made with Au nanoparticles, and it has been shown that the CSS nanoparticles outperform Au nanoparticles significantly. These CSS nanoparticles have also been used for bioimaging, in particular for Raman spectroscopy, with strong results at high densities of the nanoparticles. Utilizing stronger scattering SiO2/Au Nanoshells, it has been possible to work towards single particle imaging of molecules and demonstration of this phenomenon has been shown here through the use of coherent Raman scattering spectroscopy.
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