(De)localization dynamics of molecular excitons
- Molecular excitons play a central role in processes of solar energy conversion, both natural and artificial. It is therefore no wonder that numerous experimental and theoretical investigations in the last decade, employing state-of-the-art spectroscopic techniques and computational methods, have been driven by the common aim to unravel exciton dynamics in multichromophoric systems. Theoretically, exciton (de)localization and transfer dynamics are most often modelled using either mixed quantum-classical approaches (e.g., trajectory surface hopping) or fully quantum mechanical treatments (either using model diabatic Hamiltonians or direct dynamics). Yet, the terms such as "exciton localization" or "exciton transfer" may bear different meanings in different works depending on the method in use (quantum-classical vs. fully quantum). Here, we relate different views on exciton (de)localization. For this purpose, we perform molecular surface hopping simulations on several tetracene dimers differing by a magnitude of exciton coupling andMolecular excitons play a central role in processes of solar energy conversion, both natural and artificial. It is therefore no wonder that numerous experimental and theoretical investigations in the last decade, employing state-of-the-art spectroscopic techniques and computational methods, have been driven by the common aim to unravel exciton dynamics in multichromophoric systems. Theoretically, exciton (de)localization and transfer dynamics are most often modelled using either mixed quantum-classical approaches (e.g., trajectory surface hopping) or fully quantum mechanical treatments (either using model diabatic Hamiltonians or direct dynamics). Yet, the terms such as "exciton localization" or "exciton transfer" may bear different meanings in different works depending on the method in use (quantum-classical vs. fully quantum). Here, we relate different views on exciton (de)localization. For this purpose, we perform molecular surface hopping simulations on several tetracene dimers differing by a magnitude of exciton coupling and carry out quantum dynamical as well as surface hopping calculations on a relevant model system. The molecular surface hopping simulations are done using efficient long-range corrected time-dependent density functional tight binding electronic structure method, allowing us to gain insight into different regimes of exciton dynamics in the studied systems.…
Verfasserangaben: | Evgenii TitovORCiDGND, Tristan Kopp, Joscha HocheORCiDGND, Alexander HumeniukGND, Roland MitrićORCiDGND |
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DOI: | https://doi.org/10.1039/d2cp00586g |
ISSN: | 1463-9076 |
ISSN: | 1463-9084 |
Pubmed ID: | https://pubmed.ncbi.nlm.nih.gov/35506999 |
Titel des übergeordneten Werks (Englisch): | Physical chemistry, chemical physics : PCCP ; a journal of European chemical societies |
Untertitel (Englisch): | comparison of mixed quantum-classical and fully quantum treatments |
Verlag: | Royal Society of Chemistry |
Verlagsort: | Cambridge |
Publikationstyp: | Wissenschaftlicher Artikel |
Sprache: | Englisch |
Datum der Erstveröffentlichung: | 22.04.2022 |
Erscheinungsjahr: | 2022 |
Datum der Freischaltung: | 08.12.2023 |
Band: | 24 |
Ausgabe: | 20 |
Seitenanzahl: | 14 |
Erste Seite: | 12136 |
Letzte Seite: | 12148 |
Fördernde Institution: | European Research Council (ERC) through Consolidator Grant DYNAMO; [646737]; Deutsche Forschungsgemeinschaft (DFG) [454020933] |
Organisationseinheiten: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
DDC-Klassifikation: | 5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften |
Peer Review: | Referiert |
Publikationsweg: | Open Access / Hybrid Open-Access |