Direct observation of exciton–exciton interactions
Please always quote using this URN: urn:nbn:de:bvb:20-opus-226271
- Natural light harvesting as well as optoelectronic and photovoltaic devices depend on efficient transport of energy following photoexcitation. Using common spectroscopic methods, however, it is challenging to discriminate one-exciton dynamics from multi-exciton interactions that arise when more than one excitation is present in the system. Here we introduce a coherent two-dimensional spectroscopic method that provides a signal only in case that the presence of one exciton influences the behavior of another one. Exemplarily, we monitor excitonNatural light harvesting as well as optoelectronic and photovoltaic devices depend on efficient transport of energy following photoexcitation. Using common spectroscopic methods, however, it is challenging to discriminate one-exciton dynamics from multi-exciton interactions that arise when more than one excitation is present in the system. Here we introduce a coherent two-dimensional spectroscopic method that provides a signal only in case that the presence of one exciton influences the behavior of another one. Exemplarily, we monitor exciton diffusion by annihilation in a perylene bisimide-based J-aggregate. We determine quantitatively the exciton diffusion constant from exciton–exciton-interaction 2D spectra and reconstruct the annihilation-free dynamics for large pump powers. The latter enables for ultrafast spectroscopy at much higher intensities than conventionally possible and thus improves signal-to-noise ratios for multichromophore systems; the former recovers spatio–temporal dynamics for a broad range of phenomena in which exciton interactions are present.…
Author: | Jakub Dostál, Franziska Fennel, Federico Koch, Stefanie Herbst, Frank Würthner, Tobias Brixner |
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URN: | urn:nbn:de:bvb:20-opus-226271 |
Document Type: | Journal article |
Faculties: | Fakultät für Chemie und Pharmazie / Institut für Organische Chemie |
Fakultät für Chemie und Pharmazie / Institut für Physikalische und Theoretische Chemie | |
Language: | English |
Parent Title (English): | Nature Communications |
Year of Completion: | 2018 |
Volume: | 9 |
Article Number: | 2466 |
Source: | Nature Communications (2018) 9:2466. https://doi.org/10.1038/s41467-018-04884-4 |
DOI: | https://doi.org/10.1038/s41467-018-04884-4 |
Dewey Decimal Classification: | 5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften |
Tag: | energy transfer; optical spectroscopy; self-assembly |
Release Date: | 2024/06/14 |
Licence (German): | CC BY: Creative-Commons-Lizenz: Namensnennung 4.0 International |