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Updated: Apr 17, 2026

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
Exciton dissociation at donor-acceptor heterojunctions: dynamics using the collective effective mode representation
Aurélie Chenel1, Etienne Mangaud1, Irene Burghardt2
1Laboratoire de Chimie Physique, Bât 349, Université Paris-Sud, UMR 8000, F-91405 Orsay, France.
Abstract:
Following the recent quantum dynamics investigation of the charge transfer at an oligothiophene-fullerene heterojunction by the multi-configuration time dependent Hartree method [H. Tamura, R. Martinazzo, M. Ruckenbauer and I. Burghardt, J. Chem. Phys. 137, 22A540 (2012)], we revisit the transfer process by a perturbative non-Markovian master equation treated by the time local auxiliary density matrix approach. We compare the efficiency of the spin-boson model calibrated by quantum chemistry with the effective mode representation. A collective mode is extracted from the spin-boson spectral density. It is weakly coupled to a residual bath of vibrational modes, allowing second-order dynamics. The electron transfer is analyzed for a sampling of inter-fragment distances showing the fine interplay of the electronic coupling and energy gap on the relaxation. The electronic coherence, expected to play a role in the process, is preserved during about 200 fs.
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