Beschreibung angeregter Molekülzustände in komplex strukturierter Umgebung durch einen effizienten, individuell selektierenden MRCI-Algorithmus gekoppelt an ein molekularmechanisches Kraftfeld

Atomistic theoretical descriptions of thermal chemical recations in complex environments are well achieved by combined quantum and molecular mechanical (QM/MM) methods. The goal of this work is to extend such techniques to enable the description of photochemical reactions and to carry out case studies subsequently. In order to tackle the enormous computational demand due to the involvement of excited electronic states, we (i) largely speed up the individually selecting multi-refernce configuration interaction (IS/MRCI) scheme by Tavan and Schulten (1980) by a new grahical algorithm and (ii) take use of recently developed semimempirical valence shell models (Thiel 1997) which are well suited for excited electronic states. The efficiency and accuracy of the resulting IS/MRCI-algorithm is demonstrated by its application to the first electronic excited states of butadiene. The new QM/MM method is used to calculate absorption energies along a molecular dynamics trajectory of a small Schiff base in isotonic solution.

Level thesis:degree_level

thesis.doctoral

Grantor dc:publisher

Ludwig-Maximilians-Universität

Year

2003

Author dc:creator

• Strodel, Paul

Repository record source_url

https://edoc.ub.uni-muenchen.de/2067/

OAI identifier oai:identifier

oai:edoc.ub.uni-muenchen.de:2067