Multidimensional Femtosecond Studies of Chemical Reaction Dynamics

University Of Colorado At Boulder, Boulder CO

Investigators

Abstract

In this award funded by the Experimental Physical Chemistry Program of the Division of Chemistry, Professor David Jonas of University of Colorado will use two-dimensional spectroscopy to study the role of the phase of an optical excitation pulse on the dynamical control of molecular systems. In particular, three broad areas will be examined. First, an approach for removing propagation distortions in femtosecond 2D spectra of strongly absorbing samples will be tested. Two-dimensional spectroscopy will then be used to probe the speed of electronic motion from one orbital to another via conical intersections, which are an important mechanism that facilitates bonding changes during chemical reactions. Finally, shaped femtosecond pulses will be used to determine whether phase control of weak laser fields can modify the outcome of light-driven reactions in condensed phases without changing the intensity spectrum of the light. Two-dimensional Fourier transform infrared and optical spectroscopy is a relatively new technique that has the potential of becoming an important analytical tool for the measurement of new molecular properties. Just as in 2D-NMR, analogous 2D optical and infrared Fourier transform spectra show characteristic spectra in two-dimensional patterns that reveal adjacent bonds and their relative geometry. In particular, these studies will help establish the theory behind the types of multidimensional electronic spectroscopies currently being applied to a range of scientific problems. Graduate students and postdoctoral research associates who participate in this research acquire new knowledge and skills in preparation for advanced studies or entrance into the scientific/technological job market.