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Mapping of exciton-exciton annihilation in a molecular dimer via fifth-order femtosecond two-dimensional spectroscopy

Please always quote using this URN: urn:nbn:de:bvb:20-opus-178420
  • We present a theoretical study on exciton–exciton annihilation (EEA) in a molecular dimer. This process is monitored using a fifth-order coherent two-dimensional (2D) spectroscopy as was recently proposed by Dostál et al. [Nat. Commun. 9, 2466 (2018)]. Using an electronic three-level system for each monomer, we analyze the different paths which contribute to the 2D spectrum. The spectrum is determined by two entangled relaxation processes, namely, the EEA and the direct relaxation of higher lying excited states. It is shown that the change ofWe present a theoretical study on exciton–exciton annihilation (EEA) in a molecular dimer. This process is monitored using a fifth-order coherent two-dimensional (2D) spectroscopy as was recently proposed by Dostál et al. [Nat. Commun. 9, 2466 (2018)]. Using an electronic three-level system for each monomer, we analyze the different paths which contribute to the 2D spectrum. The spectrum is determined by two entangled relaxation processes, namely, the EEA and the direct relaxation of higher lying excited states. It is shown that the change of the spectrum as a function of a pulse delay can be linked directly to the presence of the EEA process.show moreshow less

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Author: Jasmin Süß, Johannes G. Wehner, Jakub Dostál, Volker Engel, Tobias Brixner
URN:urn:nbn:de:bvb:20-opus-178420
Document Type:Journal article
Faculties:Fakultät für Chemie und Pharmazie / Institut für Physikalische und Theoretische Chemie
Language:English
Parent Title (English):Journal of Physical Chemistry Letters
Year of Completion:2019
Volume:150
Issue:10
Pagenumber:104304
Source:Journal of Chemical Physics 150, 104304 (2019); https://doi.org/10.1063/1.5086151
URL:https://aip.scitation.org/doi/full/10.1063/1.5086151
DOI:https://doi.org/10.1063/1.5086151
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 54 Chemie / 541 Physikalische Chemie
GND Keyword:Exziton; Spektroskopie
Tag:2Dimensionale Spektroskopie; EEA
exciton; exciton-exciton
Release Date:2020/03/16
Embargo Date:2020/03/13
EU-Project number / Contract (GA) number:614623
OpenAIRE:OpenAIRE
Note:
This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in J. Süß et al., J. Chem. Phys. 150, 104304 (2019); https://doi.org/10.1063/1.5086151 and may be found at https://doi.org/10.1063/1.5086151.
Licence (German):License LogoDeutsches Urheberrecht