This project, supported in the Analytical and Surface Chemistry Program, targets the development of nanostructured gold surfaces which will be applied to fundamental studies of interfacial electrochemistry, spectroscopy, and microscopy. During the tenure of this thirty-three month standard grant, Professor Michael Natan and his students at Penn State University will fabricate tailored gold surfaces by self-assembling nanometer sized gold particles onto substrates covered with organic or inorganic thin films. These gold surfaces will then be used for probing the direct voltammetry of redox enzymes, for the optimization of metal roughness for surface enhanced Raman spectroscopy (SERS), for studies of electron transfer through organic films, for SERS spectroscopy of proteins, for the development of near-field SERS microscopy, and for the controlled electrochemical release of molecules from a single nanoelectrode. Microstructured metal surfaces offer unique properties which can be advantageously exploited in a broad range of electrochemical, spectroscopic, and microscopic applications. Using molecular self- assembly protocols, Professor Michael Natan and his students at Penn State University are pioneering techniques for tailoring microstructured gold surfaces for use in these applications. The successful pursuit of the goals of this project should give rise to significant progress in electrochemical and optical sensors, and could afford new techniques in near-field optical microscopy.