Ploetz, Per-Arno and Niehaus, Thomas and Kuehn, Oliver (2014) A new efficient method for calculation of Frenkel exciton parameters in molecular aggregates. JOURNAL OF CHEMICAL PHYSICS, 140 (17): 174101. ISSN 0021-9606, 1089-7690
Full text not available from this repository. (Request a copy)Abstract
The Frenkel exciton Hamiltonian is at the heart of many simulations of excitation energy transfer in molecular aggregates. It separates the aggregate into Coulomb-coupled monomers. Here it is shown that the respective parameters, i.e., monomeric excitation energies and Coulomb couplings between transition densities can be efficiently calculated using time-dependent tight-binding-based density functional theory (TD-DFTB). Specifically, Coulomb couplings are expressed in terms of self-consistently determined Mulliken transition charges. The approach is applied to two dimer systems. First, formaldehyde oxime for which a detailed comparison with standard DFT using the B3LYP and the PBE functionals as well as with SCS-CC2 is provided. Second, the Coulomb coupling is explored in dependence on the intermolecular coordinates for a perylene bisimide dimer. This provides structural evidence for the previously observed biphasic aggregation behavior of this dye. (C) 2014 AIP Publishing LLC.
| Item Type: | Article |
|---|---|
| Uncontrolled Keywords: | DENSITY-FUNCTIONAL-THEORY; EXCITATION-ENERGY TRANSFER; PERYLENE BISIMIDE DYE; TIGHT-BINDING METHOD; STATE PROPERTIES; COMPLEX MATERIALS; RESPONSE THEORY; APPROXIMATION; SIMULATIONS; POTENTIALS; |
| Subjects: | 500 Science > 530 Physics |
| Divisions: | Physics > Institute of Theroretical Physics > Alumni or Retired Professors > Group Thomas Niehaus |
| Depositing User: | Dr. Gernot Deinzer |
| Date Deposited: | 08 Nov 2019 14:42 |
| Last Modified: | 08 Nov 2019 14:42 |
| URI: | https://pred.uni-regensburg.de/id/eprint/10189 |
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