The use of second harmonic generation will be developed by Professor Corn to investigate the structure and dynamics of several important interfacial systems in this research project supported by the Analytical and Surface Chemistry Program. Studies of liquid-liquid interfaces will combine the SHG method with standard surface tension and electrochemical measurements to determine molecular adsorption and structure at the interface. Self assembled zirconium alkyl phosphonate layers will also be examined using SHG and vibrational spectroscopic methods, to determine molecular orientation within the interfacial layer. The molecular structural information obtained in these studies will be used to design and control the macroscopic properties of the interface. %%% This research project will combine state of the art non-linear optical methods such as second harmonic generation to probe the detailed molecular structure of several technologically important interfacial systems. Liquid-liquid interfaces, self-assembled zirconium alkly phosphonate monolayers, and electrochemical surfaces will be examined. The results of this research will provide the understanding essential to the rational design of interfacial systems.