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Please use this identifier to cite or link to this item: http://hdl.handle.net/1807/16725

Title: Elastic Scattering Phenomena in Molecularly-linked Gold Nanoparticle Films
Authors: Dunford, Jeffrey Loren
Advisor: Dhirani, Al-Amin
Department: Chemistry
Keywords: electronic scattering
self-assembled nanoparticle film
quasilocalized hopping
weak localization
reflectionless tunneling
Issue Date: 19-Jan-2009
Abstract: We have investigated the conductance, g, of 1,4-butanedithiol linked Au nanoparticle films as a function of temperature, T, bias potential, V, and applied magnetic field, B. An interesting temperature dependence is observed for non-metallic films with thicknesses just below a critical film thickness: g ~ exp [-(T_0/T)^(1/2)] for 20 K < T < 300 K. We show that this temperature dependence is incompatible with an Efros-Shklovskii "variable range hopping" model, since "hopping distances" are too large to be consistent with tunneling processes, and tend to scale with size of super-clusters of molecularly-linked nanoparticles. We propose a "quasilocalized hopping" model based on competition between single-electron charging of super-clusters and electron backscattering within super-clusters to explain the observed temperature dependence. Various electron scattering time scales are extracted from magnetoconductance data using a modified "weak localization" model. Elastic scattering time scales are comparable to those required for an electron to traverse a nanoparticle, while inelastic and spin-orbit scattering time scales are consistent with those found in studies of conventionally-prepared granular Au films. At interfaces between metallic 1,4-butanedithiol-linked Au nanoparticle films and conventional superconductors, we find that g consistently exhibits peaks, as well as oscillations, that depend simultaneously on both V and B. Such peaks and correlated conductance oscillations are predicted by an enhanced Andreev reflection process due to disorder-driven elastic scattering and electron-hole interference in the nanoparticle film. While oscillations have been predicted by a so-called "reflectionless tunneling" model, they have not been observed at other normal-superconductor interfaces. We speculate that oscillations are observable in this system due to synthetically controlled uniformity of elastic scattering length (i.e., nanoparticle diameter) and a reduced number of current-carrying pathways, especially near the interface. Contrary to predictions of existing "reflectionless tunneling" models, we find that the periods of oscillation in B decrease as T increases. This suggests that the area of interfering pathways increases with T. We propose that this increasing area can be attributed to magnetic field penetration into the superconductor. Conductance data agrees remarkably well with known temperature dependence of penetration depth predicted by BCS theory. Our study shows that this additional region of flux must be considered in experimental and theoretical studies of "reflectionless tunneling", and underscores the utility of molecularly-linked nano\-particle films as a platform for studying charge transport.
URI: http://hdl.handle.net/1807/16725
Appears in Collections:Doctoral
Department of Chemistry - Doctoral theses

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