Multidimensional Femtosecond Studies of Chemical Reaction Dynamics in Condensed Phases

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The Experimental Physical Chemistry Program of the Chemistry Division funds this project. Experimental and theoretical studies will be undertaken to develop techniques for two-dimensional (2D) Fourier transform optical and infrared spectroscopies in analogy to the well-established 2D Fourier transform nuclear magnetic resonance (NMR) methods. To this end work will focus on four broad areas: 1) theoretical studies will be undertaken of pulse propagation and signal generation in a sample to enable quantitative experiments on optically dense samples; 2) experiments will be done to attempt a demonstration of optical analogs of the "intramolecular" and "intermolecular" double quantum coherence found in magnetic resonance; 3) 2D vibrational correlation spectra will be measured for a series of molecules with identical oscillators in various geometries; and 4) the electronic dynamics in the degenerate states of a few molecules will be probed by 2D spectroscopy and polarization dependent pump-probe experiments using femtosecond pulses from a high stability visible optical amplifier.2D Fourier transform infrared and optical spectroscopy is a relatively new t that has the potential of becoming an important analytical tool. Just as in 2D-NMR, analogous 2D-optical and infrared Fourier transform spectra may show characteristic vibrational frequencies in two-dimensional patterns that reveal adjacent bonds and their relative geometry. A long-term goal of this work is to develop of new 2D optical spectrometers for the measurement of new molecular properties. Graduate and undergraduate students as well as postdoctoral research associates will participate in this research. They will acquire new knowledge and skills in preparation for advance studies or entrance into the scientific/technological job market.