Coordinated Studies of the Reaction Dynamics for Isolated and Solvated Molecules

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In this project, funded by the Experimental Physical Chemistry Program of the Chemistry Division, Prof. Brooks Pate of the University of Virginia will investigate the reaction dynamics of isolated molecules and the way that solvation changes this intrinsic behavior. A new experimental design for ultrafast vibrational spectroscopy will be developed. By combining state-of-the-art experimental techniques for gas and solution phase molecular spectroscopy, this work bridges two of the major fields of physical chemistry: intramolecular dynamics and solution chemistry. A major part of the project is to examine how the solvent affects intramolecular vibrational coherence imparted to the system by a laser pulse. These experiments will test the ability to manipulate the vibrational motion and structure of isolated molecules through infrared (IR) pulse sequences. With experiments conducted in solution it will be possible to determine whether the coherence required for quantum manipulation is preserved. A second goal of the project is the development of a new spectrometer for measuring reaction kinetics using dynamical rotational spectroscopy (DRS).The instrumental development parts of this project will broadly impact several areas of science and technology, such as applications in the field of combustion kinetics, new approaches to measuring the kinetics of molecular geometry change, and new tools to study the ability to manipulate molecular properties through control of the quantum dynamics. This work has potential applications in the fields of biophysical chemistry and nanoscience. Students who participate in this research will gain valuable experience in the design, construction and testing of new measurement equipment. The students will also receive strong training in the fundamental concepts of both time-domain and frequency-domain spectroscopy that will allow them to appreciate the relative strengths of these complementary techniques.