Rostock 2019 – wissenschaftliches Programm
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MO: Fachverband Molekülphysik
MO 18: Posters 2: Time Resolved Spectroscopy
MO 18.5: Poster
Mittwoch, 13. März 2019, 16:15–18:15, S Foyer LLM
Mapping of exciton-exciton annihilation in a molecular dimer via fifth-order femtosecond two-dimensional spectroscopy — •Jasmin Süß1, Johannes Wehner1, Jakub Dostál2,3, Tobias Brixner2,3, and Volker Engel1 — 1Institut für Physikalische und Theoretische Chemie, Emil-Fischer-Str. 42, 97074 Würzburg, Germany — 2Institut für Physikalische und Theoretische Chemie, Am Hubland, 97074 Würzburg, Germany — 3Center for Nanosystems Chemistry (CNC), Theodor-Boveri-Weg, 97074 Würzburg, Germany
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 two-dimensional 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.