Ultrafast Spectroscopy and Other Applications of Lasers in Chemistry

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Robin Hochstrasser of the University of Pennsylvania is supported by the Experimental Physical Chemistry Program to continue his studies on ultrafast dynamics in liquids. Femtosecond (fs) laser spectroscopic techniques will be brought to bear on two central themes: solvent control of chemical reactions and the relaxation of molecular excitations. Specific techniques to be developed include fs transient infrared spectroscopy at low frequencies; terahertz spectroscopy to probe low frequency motions in molecular pump-probe experiments; and fs time-resolved X-ray scattering on liquid samples. Focus is on solvent-assisted uni- and bimolecular reaction dynamics and electronic and vibrational relaxation. Quantum chemical calculations of the potential energy surfaces and classical molecular dynamics simulations will also be carried out. The study of the transformation of energetically excited molecules in condensed phases from one molecular isomeric configuration to another will significantly expand our knowledge of how a complex molecule undergoes internal rearrangements and how these are mediated by a surrounding solvent.