Ultrafast Multi-Dimentional Infrared Vibrational Echo Spectroscopy of Molecular Dynamics on Surfaces and in Bulk Systems.

摘要

During the current grant period we have made substantial progress. We have been applying ultrafast 2D IR vibrational echo spectroscopy to important problems of molecular dynamics; we have been using a variety of techniques to study room temperature ionic liquids (RTILs); and we have advanced the early stages of investigation of interfacial and surface phenomena using ultrafast IR spectroscopy. We made a major theoretical advance in how to analyze ultrafast 2D IR vibrational echo spectral diffusion data. We further developed and applied 2D IR Vibrational Echo Chemical Exchange Spectroscopy, which we pioneered during the last AFOSR grant period. We have also been studying RTILs using optical heterodyne detected optical Kerr Effect measurements, time resolved fluorescence spectroscopy, and initial experiments directed to using 2D IR vibrational echo spectroscopy. Of particular importance we have realized a main new thrust of the work, that is, we have performed the first investigations of the dynamics of a heterogeneous catalyst using ultrafast infrared vibration echo spectroscopy of a submonolayer of molecules. Ultrafast two-dimensional infrared vibrational echo spectroscopy has proven broadly useful for studying molecular dynamics in solutions.