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

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.

Authors:
;  [1];  [2];  [3];  [1]
  1. Laboratoire de Chimie Physique, Bât 349, Université Paris-Sud, UMR 8000, F-91405 Orsay (France)
  2. Institut für Physikalische und Theoretische Chemie, Goethe Universität Frankfurt, Max-von-Laue-Str. 7, D-60438 Frankfurt am Main (Germany)
  3. Laboratoire Collisions, Agrégats, Réactivité, UMR 5589, IRSAMC, Université Paul Sabatier, F-31062 Toulouse (France)
Publication Date:
OSTI Identifier:
22255231
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 140; Journal Issue: 4; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; BOSONS; DENSITY MATRIX; DISSOCIATION; EFFICIENCY; ELECTRON TRANSFER; ENERGY GAP; FULLERENES; HETEROJUNCTIONS; SPECTRAL DENSITY; SPIN; TIME DEPENDENCE

Citation Formats

Chenel, Aurélie, Mangaud, Etienne, Laboratoire Collisions, Agrégats, Réactivité, UMR 5589, IRSAMC, Université Paul Sabatier, F-31062 Toulouse, Burghardt, Irene, Meier, Christoph, Desouter-Lecomte, Michèle, and Département de Chimie, Université de Liège, Sart Tilman, B6, B-4000 Liège. Exciton dissociation at donor-acceptor heterojunctions: Dynamics using the collective effective mode representation of the spin-boson model. United States: N. p., 2014. Web. doi:10.1063/1.4861853.
Chenel, Aurélie, Mangaud, Etienne, Laboratoire Collisions, Agrégats, Réactivité, UMR 5589, IRSAMC, Université Paul Sabatier, F-31062 Toulouse, Burghardt, Irene, Meier, Christoph, Desouter-Lecomte, Michèle, & Département de Chimie, Université de Liège, Sart Tilman, B6, B-4000 Liège. Exciton dissociation at donor-acceptor heterojunctions: Dynamics using the collective effective mode representation of the spin-boson model. United States. https://doi.org/10.1063/1.4861853
Chenel, Aurélie, Mangaud, Etienne, Laboratoire Collisions, Agrégats, Réactivité, UMR 5589, IRSAMC, Université Paul Sabatier, F-31062 Toulouse, Burghardt, Irene, Meier, Christoph, Desouter-Lecomte, Michèle, and Département de Chimie, Université de Liège, Sart Tilman, B6, B-4000 Liège. 2014. "Exciton dissociation at donor-acceptor heterojunctions: Dynamics using the collective effective mode representation of the spin-boson model". United States. https://doi.org/10.1063/1.4861853.
@article{osti_22255231,
title = {Exciton dissociation at donor-acceptor heterojunctions: Dynamics using the collective effective mode representation of the spin-boson model},
author = {Chenel, Aurélie and Mangaud, Etienne and Laboratoire Collisions, Agrégats, Réactivité, UMR 5589, IRSAMC, Université Paul Sabatier, F-31062 Toulouse and Burghardt, Irene and Meier, Christoph and Desouter-Lecomte, Michèle and Département de Chimie, Université de Liège, Sart Tilman, B6, B-4000 Liège},
abstractNote = {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.},
doi = {10.1063/1.4861853},
url = {https://www.osti.gov/biblio/22255231}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 4,
volume = 140,
place = {United States},
year = {Tue Jan 28 00:00:00 EST 2014},
month = {Tue Jan 28 00:00:00 EST 2014}
}