We present a time-dependent mixed quantum/semiclassical approach to calculating linear absorption spectra. Applying Variational Fixed Vibrational Basis/Gaussian Bath theory (FVB/GB) to the treatment of small molecules isolated in an extended cryogenic medium, an assumed time-scale separation between the few rapid, largely intramolecular modes of the guest and the several slower extended modes of the medium is utilized to partition a system from the surrounding bath. The system dynamics are handled with basis set methods, while the bath degrees of freedom are subject to a semiclasscial thawed Gaussian ansatz. The linear absorption spectrum for a realistic model system is calculated using FVB/GB results and then compared with a numerically exact calculation. Also contained in this dissertation are previously published theoretical works on Transient Absorption and Femtosecond Stimulated Raman Spectroscopy. Both encompass a rebuilding of the theory and elucidate the information content of the respective spectroscopic signals.
This dissertation includes previously published co-authored material.
| Identifer | oai:union.ndltd.org:uoregon.edu/oai:scholarsbank.uoregon.edu:1794/23124 |
| Date | 10 April 2018 |
| Creators | Kovac, Philip |
| Contributors | Cina, Jeffrey |
| Publisher | University of Oregon |
| Source Sets | University of Oregon |
| Language | en_US |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Rights | All Rights Reserved. |
Page generated in 0.0019 seconds