Advances in Quantum Chemistry: Ratner Volume

0483916 - ÚOCHB 2018 RIV US eng M - Monography Chapter
Buchanan, E. A. - Havlas, Zdeněk - Michl, Josef
Singlet Fission: Optimization of Chromophore Dimer Geometry.
Advances in Quantum Chemistry: Ratner Volume. Cambridge: Academic Press, 2017 - (Sabin, J.; Brändas, E.), s. 175-227. Advances in Quantum Chemistry, 75. ISBN 978-0-12-812888-6
R&D Projects: GA ČR GA15-19143S
Institutional support: RVO:61388963
Keywords : photophysics * singlet fission * HOMO/LUMO model * Davydov splitting * biexciton
OECD category: Physical chemistry

After a brief review of electronic aspects of singlet fission, we describe a systematic simplification of the frontier orbital (HOMO/LUMO) model of singlet fission and Davydov splitting in a pair of rigid molecules. In both instances, the model includes electron configurations representing local singlet excitation on either chromophore, charge transfer in either direction, and triplet excitation in both chromophores (biexciton). The resulting equations are simple enough to permit complete searches for local extrema of the square of the electronic matrix element and to evaluate the effect of intermolecular interactions on the exoergicity of singlet fission and on the biexciton binding energy in the six-dimensional space of rigid dimer geometries. The procedure is illustrated on results for the six best geometries for dimers of ethylene and of an indigoid heterocycle with 24 carbon, nitrogen, and oxygen atoms.
Permanent Link: http://hdl.handle.net/11104/0279096