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Hannover 2016 – wissenschaftliches Programm

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MO: Fachverband Molekülphysik

MO 18: The Modelling of Molecular Dynamics

MO 18.2: Vortrag

Donnerstag, 3. März 2016, 14:45–15:00, f142

Unraveling the Quantum State Mixing of Excitonic and Vibronic Excitations in the Dynamics of Molecular Aggregates — •Marco Schröter1, Tõnu Pullerits2, and Oliver Kühn11Institut für Physik, Universität Rostock, Albert-Einstein-Str. 23-24, 18059 Rostock, Germany — 2Chemical Physics, Lund University, Box 124, 22100 Lund, Sweden

One possible source of coherent oscillations observed in two-dimensional electronic spectroscopy experiments is the quantum state mixing (QSM) of electronic and vibronic excitations in molecular aggregates. In the present contribution the signatures of Coulomb coupling induced QSM between excitonic and vibronic excitations in the dynamics of a model aggregate are discussed. To this end numerically exact dissipative exciton dynamics calculations applying the hierarchy equations of motion (HEOM) method are performed. A Fourier analysis of the coherent oscillations in the population dynamics after an initial excitation of the highest exciton state is supplemented by exciton-vibronic structure calculations employing direct diagonalization [1]. This allows us to unravel the origin of the oscillations and to obtain insights on the general influence of QMS on the dynamics as a function of Coulomb and vibronic coupling strengths [2].

[1] M. Schröter et al., Physics Reports 567, 1 (2015)

[2] M. Schröter et al., Annalen der Physik 527, 536 (2015)

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