Nanofabricated Surfaces: Atomic Force Microscopy and Surface-Enhanced Laser Spectroscopy at Ultrahigh Vacuum and Electrochemical Interfaces

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This research project involves a systematic study of the microscopic mechanisms of surface enhanced laser spectroscopies, including surface enhanced Raman, hyper-Raman, second harmonic generation, and sum frequency generation spectroscopy. Several methods of nanostructure preparation, combined with scanning probe microscopic characterization of these structured surfaces, will be used to probe the electromagnetic and chemical mechanisms of surface enhanced laser spectroscopies. This work, supported by the Analytical and Surface Chemistry Program, will directly test present models of the surface enhancement mechanism by fashioning surfaces which match the structures modeled in leading theoretical descriptions of the effect. Contributions to the understanding of the surface enhanced spectroscopy, as well as to the development and characterization of nanostructured surfaces should result from this work. Impact well beyond the use of this method for studies of roughened surfaces is expected. Further development of the analytical methods of surface enhanced laser spectroscopy relies on the development of a quantitative, predictive explanation of the enhancement process. This research program will develop the theoretical underpinning for this technique by a careful set of experiments which rationally prepare surface structures which can be accurately theoretically modeled. The insights gained from the comparison of measurements on modelable surfaces should allow development of a quantitative theory. It is expected that useful methods for the fabrication of materials with nanostructured surfaces will also result.