Exciton dissociation at donor-acceptor heterojunctions: dynamics using the collective effective mode representation of the spin-boson model

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 pr...

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Bibliographic Details
Published in:The Journal of chemical physics 2014-01, Vol.140 (4), p.044104-044104
Main Authors: Chenel, Aurélie, Mangaud, Etienne, Burghardt, Irene, Meier, Christoph, Desouter-Lecomte, Michèle
Format: Article
Language:English
Subjects:
ATOMIC AND MOLECULAR PHYSICS
BOSONS
Chemistry
Chimie
DENSITY MATRIX
DISSOCIATION
EFFICIENCY
ELECTRON TRANSFER
ENERGY GAP
FULLERENES
HETEROJUNCTIONS
Physical, chemical, mathematical & earth Sciences
Physics
Physique, chimie, mathématiques & sciences de la terre
SPECTRAL DENSITY
SPIN
TIME DEPENDENCE
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Summary: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.
ISSN:0021-9606
1089-7690
1089-7690
DOI:10.1063/1.4861853