CAREER: Surface-Enhanced Nonlinear Spectroscopy: Mapping Electronic Excited States, Probing Surface Adsorbate Structure, and Ultrasensitive Detection

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This CAREER award by the Chemical Measurement and Imaging (CMI) program supports Professor Jon Camden at the University of Tennessee Knoxville to develop surface nonlinear spectroscopy as a analytical method for probing the two-photon properties of molecules, surface adsorbate structure, and ultrasensitive detection. A method for measuring absolute SEHRS enhancement factors is presented and subsequently utilized to elucidate the respective roles of chemical and electromagnetic enhancements in SEHRS. The wavelength dependent nature of the molecule-plasmon coupling and of resonance enhanced hyper-Raman will provide information on the complex interplay of molecular excited states important in two-photon processes. Detailed comparisons between experiment and theory are pursued, which will benchmark new electronic structure methods for the calculation of nonlinear molecular properties. The studies will demonstrate SEHRS to be a powerful, routinely applicable, and ultrasensitive analytical tool. Further, this work will provide the basis for future studies of surface-enhanced nonlinear spectroscopy. In addition to the scientific objectives of this proposal, the PI seeks to increase the number of high-school students pursuing Science, Technology, Engineering, and Mathematics (STEM) majors in college. The PI will collaborate to provide curricular enrichment to local public high-schools through the creation of ASPIRE teams (Aspiring Scientists Participating in Research and Education). ASPIRE teams will deliver hands-on laboratory experiments to local high school classrooms once a month during the regular school year, for a total of six activities. The activities are aligned to meet the requirements of Tennessee State curriculum and introduce students to the properties of nanoscale materials. Regular assessments are used to refine the activities and gauge their impact.