Files
Document type
ArticleVersion
Published versionPublication date
Publication license
Please use this identifier to cite or link to this item: https://hdl.handle.net/2445/219447
A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds
Journal Title
Director/Tutor
Additional contribution
Journal ISSN
Volume Title
Abstract
Perylenediimide molecules constitute a family of chromophores that undergo singlet fission, a process in which an excited singlet state converts into lower energy triplets on two neighboring molecules, potentially increasing the efficiency of organic solar cells. Here, the nonorthogonal configuration interaction method is applied to study the effect of the different crystal packing of various perylenediimide derivatives on the relative energies of the singlet and triplet states, the intermolecular electronic couplings, and the relative rates for singlet fission. The analysis of the wave functions and electronic couplings reveals that charge transfer states play an important role in the singlet fission mechanism. Dimer conformations where the PDI molecules are at large displacements along the long axis and short on the short axis are posed as the most favorable for singlet fission. The role of the substituent at the imide group has been inspected concluding that, although it has no effect in the energies, for some conformations it significantly influences the electronic couplings, and therefore, replacing this substituent with hydrogen may introduce artifacts in the computational modeling of the PDI molecules.
Related resource
Subject
Subject (English)
Citation
Citation
SOUSA ROMERO, Carmen, et al. A Non-orthogonal Configuration Interaction approach to Singlet Fission in Perylenediimide compounds. Journal of Physical Chemistry A. 2023. Vol. 127, num. 9944-9958. ISSN 1089-5639. [consulted: 16 of October of 2026]. Available at: https://hdl.handle.net/2445/219447