Nordlander, Peter J.2009-06-042009-06-042000Wolfgang, John A.. "Hot electron dynamics and impurity scattering on gold nanoshell surfaces." (2000) Diss., Rice University. <a href="https://hdl.handle.net/1911/18045">https://hdl.handle.net/1911/18045</a>.https://hdl.handle.net/1911/18045Recent ultrafast pump-probe experiments studying the relaxation rate of an optically excited hot electron distribution on Au/Au2S gold nanoshells indicate that this relaxation rate can be modified by the chemical environment surrounding the shell. This work will begin a theoretical investigation of the effect of chemical adsorbates---solvents and impurities---upon nanoshell hot electron dynamics. The effects of water, polyvinyl alcohol (PVA), sulfur, p-aminobenzoic acid, p-mercaptobenzoic acid and propylamine adsorbates are examined for their electronic interaction with a noble metal surface. p-Aminobenzoic acid is found to have a very large dipole moment when adsorbed to the metal surface, in contrast to p-mercaptobenzoic acid, propylamine and water. This correlates well to the experimentally observed results where nanoshells dispersed in an aqueous soulution with p-aminobenzoic acid display a faster relaxation rate compared to nanoshells dispersed in a pure water, aqueous propylamine or aqueous p-mercaptobenzoic acid environments. This thesis will also introduce a non-equilibrium Green's function approach, based on the formalism developed by Baym and Kadanoff, to model the dynamics of a hot electron distribution. The model will be discussed in terms of a simple potential scattering mechanism, which may in later work be expanded to include more complex electron-electron and electron-phonon interactions. Lastly acoustic oscillation modes are calculated for solid gold spheres and gold-silicon nanoshells. These modes describe an effect of electron-phonon coupling between the hot electron distribution and the nanoshell lattice, whereby the electronic energy is converted into mechanical energy.71 p.application/pdfengCopyright is held by the author, unless otherwise indicated. Permission to reuse, publish, or reproduce the work beyond the bounds of fair use or other exemptions to copyright law must be obtained from the copyright holder.Condensed matter physicsThesisTHESIS PHYS. 2001 WOLFGANG