Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 134, Issue 24, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.3600341
Keywords
charge exchange; fullerenes; molecule-photon collisions; organic compounds; photosynthesis; reaction kinetics theory
Funding
- National Science Foundation [0726909]
- JSPS-RFBR [09-02-92114]
- MEXT
- Funding Program for Innovative Research and Development on Science and Technology (FIRST)
- Direct For Computer & Info Scie & Enginr [0726909] Funding Source: National Science Foundation
- Division of Computing and Communication Foundations [0726909] Funding Source: National Science Foundation
- Grants-in-Aid for Scientific Research [21102002, 22224007] Funding Source: KAKEN
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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 similar to 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. (C) 2011 American Institute of Physics. [doi: 10.1063/1.3600341]
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