Dynamical Spectroscopy of Prototypes in Condensed Phase Chemistry

Download or read book Dynamical Spectroscopy of Prototypes in Condensed Phase Chemistry written by and published by . This book was released on 2001 with total page 0 pages. Available in PDF, EPUB and Kindle. Book excerpt: Significant accomplishments were made under the program of dynamical spectroscopy, aimed at elucidating details of chemical dynamics in condensed media. In fact, there now is a well-defined field of multi-dimensional spectroscopy, entirely aimed at the essence of what we had proposed. In the same natural vain of evolution, we developed the rather powerful technique of Time and Frequency Resolved Coherent Anti Stokes Raman Scattering (TFRCARS), as a tool that goes beyond the interrogation of interactions and molecular dynamics in condensed media. This four-wave mixing scheme, with transform limited detection of evolving coherences, can be regarded as a complete experiment in the creation, manipulation, and interrogation of quantum coherences. As such, it foreshadows useful quantum control, be it for chemical or computational purposes. A significant part of our present effort is aimed at devising and implementing control with shaped pulses to demonstrate computational algorithms in the laboratory. The original inspiration for developing TFRCARS was our aim to manipulate molecular wavepackets in regions where direct pumping could not be achieved, due to the inaccessible Franck-Condon factors. The target of those studies was the detailed dissection of non-adiabatic dynamics in the condensed phase prototype of solvated molecular iodine. While significant progress has been made toward this end, both direct experimentation and theoretical understanding of this process remain somewhat illusive. Highlights of advances made in theory and experiment are given based on some 20 published works that have appeared during this funding period, as a result of partial or total support by the grant.