Resonance Raman and Time Dependent Theory Studies of Ground and Excited State Mixed Valence.

다국어 초록 (Multilingual Abstract)

The work covered in this thesis focuses on application and development of mixed valence theory, which is described in chapter 1. Mixed Valence molecules have two or more equivalent charge bearing units which interact with each other through a bridge. The interaction provides an interesting problem of curved crossed potentials, which show different behavior depending on the strength of interaction. The second chapter provides an example of a simple molecule with a strong interaction between the charge bearing units, which is the simplest mixed valence scenario. In the final chapter a mixed valence system whose interaction is tunable by solvent is observed. This system was tuned to a very weak interaction such that the curve crossed potential dominates the spectral signal observed. The mixed valence theory formalism is also extended from only two charge bearing units to allow for three charge bearing units. The specific details of the mixed valence theory can be understood by the employment of time-dependent theory of molecular spectroscopy. In addition to its use in understanding the trends of mixed valence theory it can also be used to understand how the normal coordinates are affected by photoexcitation by calculating the resonance Raman and electronic spectra observed for each molecule.