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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

Exploring time-dependent approaches towards the calculation of dynamics and spectroscopic signals: A mixed quantum/semiclassical wave packet method and the theory of transient absorption and femtosecond stimulated Raman scattering

Kovac, Philip 10 April 2018 (has links)
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.

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