Simulations of pump-probe exitations of electronic wave packets for a large qusi-rigid molecular system by means of an extension to the time-dependent configuration interaction singles method
- In this paper, we report simulations of laser-driven many-electron dynamics by means of the time-dependent configuration interaction singles (TD-CIS) approach. Photoionization is included by a heuristic model within calculations employing standard Gaussian basis sets. Benzo[g]-N-methyl-quinolinium-7-hydroxylate (BMQ7H) serves as a test system to generate predefined wave packets, i.e. a superposition between the ground and fifth excited state, in a large molecule. For this molecule, these two states have a very similar geometry, which enables us to use the fixed nuclei approximation. Furthermore, this geometric stability would also prevent a dephasing of the electron wave packet due to nuclear dynamics in an experimental realization of our simulations. We also simulate the possible detection of such a wave packet by ultra short probe laser pulses, i.e. pump-probe spectra.
Author details: | Stefan KlinkuschGND, Tillmann KlamrothORCiDGND |
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DOI: | https://doi.org/10.1142/S0219633613500053 |
ISSN: | 0219-6336 |
Title of parent work (English): | Journal of theoretical and computational chemistry |
Publisher: | World Scientific |
Place of publishing: | Singapore |
Publication type: | Article |
Language: | English |
Year of first publication: | 2013 |
Publication year: | 2013 |
Release date: | 2017/03/26 |
Tag: | Electron dynamics; pump-probe; time-dependent configuration interaction |
Volume: | 12 |
Issue: | 3 |
Number of pages: | 17 |
Funding institution: | Deutsche Forschungsgemeinschaft [Sonderforschungsbereich 658] |
Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
Peer review: | Referiert |