We investigate the quantum dynamics of energy and charge transfer in a wheel-shaped artificial photosynthetic antenna-reaction center complex. This complex consists of six light-harvesting chromophores and an electron-acceptor fullerene. To describe quantum effects on a femtosecond time scale, we derive the set of exact non-Markovian equations for the Heisenberg operators of this photosynthetic complex in contact with a Gaussian heat bath. With these equations we can analyze the regime of strong system-bath interactions, where reorganization energies are of the order of the intersite exciton couplings. We show that the energy of the initially excited antenna chromophores is efficiently funneled to the porphyrin-fullerene reaction center, where a charge-separated state is set up in a few picoseconds, with a quantum yield of the order of 95%. In the single-exciton regime, with one antenna chromophore being initially excited, we observe quantum beatings of energy between two resonant antenna chromophores with a decoherence time of ∼100 fs. We also analyze the double-exciton regime, when two porphyrin molecules involved in the reaction center are initially excited. In this regime we obtain pronounced quantum oscillations of the charge on the fullerene molecule with a decoherence time of about 20 fs (at liquid nitrogen temperatures). These results show a way to directly detect quantum effects in artificial photosynthetic systems.
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28 June 2011
Research Article|
June 23 2011
Quantum effects in energy and charge transfer in an artificial photosynthetic complex
Pulak Kumar Ghosh;
Pulak Kumar Ghosh
a)
1
Advanced Science Institute
, RIKEN, Wako, Saitama 351-0198, Japan
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Anatoly Yu. Smirnov;
Anatoly Yu. Smirnov
1
Advanced Science Institute
, RIKEN, Wako, Saitama 351-0198, Japan
2Physics Department,
The University of Michigan
, Ann Arbor, Michigan 41109-1040, USA
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Franco Nori
Franco Nori
1
Advanced Science Institute
, RIKEN, Wako, Saitama 351-0198, Japan
2Physics Department,
The University of Michigan
, Ann Arbor, Michigan 41109-1040, USA
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a)
Author to whom correspondence should be addressed. Electronic mail: [email protected].
J. Chem. Phys. 134, 244103 (2011)
Article history
Received:
January 27 2011
Accepted:
May 25 2011
Citation
Pulak Kumar Ghosh, Anatoly Yu. Smirnov, Franco Nori; Quantum effects in energy and charge transfer in an artificial photosynthetic complex. J. Chem. Phys. 28 June 2011; 134 (24): 244103. https://doi.org/10.1063/1.3600341
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