Karsten,  Sven

Trajectory-based approaches to vibronic spectroscopy of molecular systems

Rostock : Universität , 2018

https://doi.org/10.18453/rosdok_id00002484

http://purl.uni-rostock.de/rosdok/id00002484

Abstract:

The goal of this thesis is to bridge the gap between the two standard theoretical approaches to vibronic spectroscopy via trajectory-based methods. As the starting point, a generalized time-correlation function is introduced and the ring-polymer molecular dynamics method is generalized to vibronic transitions, yielding an improvement over known classical approximations. Further, the vibronic spectrum is evaluated via the Matsubara dynamics. Employing an ad-hoc modification, the sign problem of the Matsubara method can be circumvented and the spectra of model systems are adequately simulated.

Dissertation Open Access