Potential-driven reversible regulation of hierarchical dynamics of nano-entities and functionalization of electrified interfaces

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1. In situ characterization methods being indispensable as basic techniques in this research were developed for the measurements of adsorption state, molecular orientation, micro-environment and molecular assembling structure as well as their potential dependent dynamics on electrode surfaces: (1) Electroreflectance methods were sophisticated, for example, to elucidate the adsorption orientation of macromolecules and to track the potential step transients of the surface processes, (2) An 1R reflection instrument was constructed, and (3) The fluorescence spectral analysis and moving imaging microscopic observation were developed.2. The title research targets at electrified interfaces included liquid alkane thin films, surface assemblies of amphiphiles, viologen adsorption layers, a fluorescent dendrimer, and surface-modified Au nanoparticles. Representative achievements are listed below.(1) Alkane molecules were found to be potential-responsible on a Au(III) electrode. The dynamics extended to far distances from the electrode surface to the bulk of the aqueous solution.(2) Systematic understandings of potential-driven assembling structural changes of pyridyl and imidazolyl terminated amphiphiles on a Au(III) electrode surface were established.(3) Two-dimensional faradaic phase transition behavior of various viologen molecules on a HOPG electrode was described in terms of interplay of multiple modes of intermolecular interactions.(4) An anomalous effect of dendrimer adsorption upon redox reaction was found. Potential dependent reshape of dendrimer also was analyzed.(5) Potential-driven dynamics of Au nanoparticles were elucidated, together with adsorption-desorption and charging-discharging processes as well as anion effects.3. These results would be quite useful for design of dynamics and interfacial functionalization in the near future.