The objectives are to better understand the electronic structure and behavior of organic molecules and their aggregates that are prototype to health related systems. The work includes the development of unique spectroscopic methods to bring out hitherto unknown structural features. Methods being developed include very high resolution spectroscopy of crystals using lasers and with magnetic and electric fields. The research uses and develops laser techniques for the study of complex systems: In particular novel experiments are proposed using dye lasers and picosecond lasers to explore dynamical properties of excited states in aggregates and non-radiative relaxation pathways in metalloporphyrins. The research also seeks to develop the theory and experimental aspects of resonance light scattering and use coherent resonant quasi-Raman processes to learn details of the structures of prototype organic molecules, and hemeproteins. A major new direction of the research involves direct studies of the chemical dynamics of diatom (O2, CO, NO) interactions with heme in prototype systems as well as hemeproteins. These experiments involve picosecond timescale spectroscopic and kinetic studies having unprecendented precision. Experiments are planned to measure vibrational relaxation times and vibrational energy transfer dynamics in aggregated systems such as isotopically mixed molecular crystals. The vibrational relaxation dynamics of simple diatomic and triatomic ions in aqueous solution will be explored, and used to generate theoretical models for energy transfer. Experiments related to the basis of coherent light generation in molecular four-level systems are planned in order the resonant CARS and CSRS processes can be properly understood, and applied to interesting spectroscopic questions. Metalloporphyrins in paraffins at low temperature will be studied using resonant CARS and CSRS. An experimental approach to picosecond transient Raman spectroscopy is planned, focused initially on FeTPP:C1 and HbX dissociation.
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