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Updated: Aug 26, 2025

Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization
Published on: August 6, 2018
Third-order pump-probe spectroscopy applied to molecular dimers: characterization of relaxation dynamics and
Fabian Glaab1, Jasmin Süβ1, Volker Engel1
1Universität Würzburg, Institut für Physikalische und Theoretische Chemie, Emil-Fischer-Str. 42, 97074 Würzburg, Germany. volker.engel@uni-wuerzburg.de.
Abstract:
We investigate theoretically the excitonic dynamics in molecular dimers which is monitored by two time-delayed femtosecond laser pulses. A two-photon absorption leads to a wave packet dynamics in the manifold of second excited states. This opens up the channel for exciton-exciton annihilation (EEA) which involves non-radiative electronic transitions. It is shown that the time interval during which EEA takes place can be monitored by the detection of third-order signals which can be interpreted as originating from a pump-probe scheme. In the case of transient absorption, the spectra directly map intraband relaxation processes.
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