Exciton dissociation at donor-acceptor heterojunctions: Dynamics using the collective effective mode representation of the spin-boson model
- Laboratoire de Chimie Physique, Bât 349, Université Paris-Sud, UMR 8000, F-91405 Orsay (France)
- Institut für Physikalische und Theoretische Chemie, Goethe Universität Frankfurt, Max-von-Laue-Str. 7, D-60438 Frankfurt am Main (Germany)
- Laboratoire Collisions, Agrégats, Réactivité, UMR 5589, IRSAMC, Université Paul Sabatier, F-31062 Toulouse (France)
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.
- OSTI ID:
- 22255231
- Journal Information:
- Journal of Chemical Physics, Vol. 140, Issue 4; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
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