2013
DOI: 10.1021/jz4011477
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Clustered Geometries Exploiting Quantum Coherence Effects for Efficient Energy Transfer in Light Harvesting

Abstract: Elucidating quantum coherence effects and geometrical factors for efficient energy transfer in photosynthesis has the potential to uncover non-classical design principles for advanced organic materials. We study energy transfer in a linear light-harvesting model to reveal that dimerized geometries with strong electronic coherences within donor and acceptor pairs exhibit significantly improved efficiency, which is in marked contrast to predictions of the classical Förster theory. We reveal that energy tuning du… Show more

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Cited by 45 publications
(72 citation statements)
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“…22,23 In this paper, NMR is utilized to simulate the quantum coherent dynamics in photosynthetic light harvesting. As a prototype, a tetramer including four chlorophylls, 13 as schematically illustrated in Fig. 1a, is employed in the NMR quantum simulation.…”
Section: Resultsmentioning
confidence: 99%
See 1 more Smart Citation
“…22,23 In this paper, NMR is utilized to simulate the quantum coherent dynamics in photosynthetic light harvesting. As a prototype, a tetramer including four chlorophylls, 13 as schematically illustrated in Fig. 1a, is employed in the NMR quantum simulation.…”
Section: Resultsmentioning
confidence: 99%
“…Because photosynthetic pigment-protein complexes are intrinsically open quantum systems, with system-bath couplings comparable to the intrasystem couplings, it is difficult to faithfully mimic the exact quantum dynamics of EET. Among the methods for describing EET, 1,[11][12][13] the hierarchical equation of motion (HEOM) yields a numerically exact solution at the cost of considerable computing time. 11,14 For the widely-studied Fenna-Matthews-Olson (FMO) complex, 5,6,11,13,15,16 a reliable result could be produced by 16,170 coupled differential equations at low temperatures, based on the HEOM 11,14 with 4 layers.…”
Section: Introductionmentioning
confidence: 99%
“…(1) cannot faithfully be employed to model population dynamics. Because the original Förster theory treats the intra-system couplings perturbatively, the theory should be generalized to describe the EET in a multichromophoric system when there are some clusters 48,49 .…”
Section: B Generalized Förster Theorymentioning
confidence: 99%
“…It was found that by combining the coherence of excitation transport and the thermal noise, the excitation may easily escape a local potential minima of the FMO and move to the reaction center. There were also works on studying the effects of the molecular geometric structure on the efficiency of energy transport [56]. Ref.…”
Section: Photosynthesismentioning
confidence: 99%