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Efficiency of energy transfer in a light-harvesting system under quantum coherence

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 Added by Chiu Fan Lee
 Publication date 2008
  fields Physics
and research's language is English




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We investigate the role of quantum coherence in the efficiency of excitation transfer in a ring-hub arrangement of interacting two-level systems, mimicking a light-harvesting antenna connected to a reaction center as it is found in natural photosynthetic systems. By using a quantum jump approach, we demonstrate that in the presence of quantum coherent energy transfer and energetic disorder, the efficiency of excitation transfer from the antenna to the reaction center depends intimately on the quantum superposition properties of the initial state. In particular, we find that efficiency is sensitive to symmetric and asymmetric superposition of states in the basis of localized excitations, indicating that initial state properties can be used as a efficiency control parameter at low temperatures.



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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 Forster theory. We reveal that energy tuning due to coherent delocalization of photoexcitations is mainly responsible for the efficiency optimization. This coherence-assisted energy-tuning mechanism also explains the energetics and chlorophyll arrangements in the widely-studied Fenna-Matthews-Olson complex. We argue that a clustered network with rapid energy relaxation among donors and resonant energy transfer from donor to acceptor states provides a basic formula for constructing efficient light-harvesting systems, and the general principles revealed here can be generalized to larger systems and benefit future innovation of efficient molecular light-harvesting materials.
Several recent studies of energy transfer in photosynthetic light harvesting complexes have revealed a subtle interplay between coherent and decoherent dynamic contributions to the overall transfer efficiency in these open quantum systems. In this work we systematically investigate the impact of temporal and spatial correlations in environmental fluctuations on excitation transport in the Fenna-Matthews-Olson photosynthetic complex. We demonstrate that the exact nature of the correlations can have a large impact on the efficiency of light harvesting. In particular, we find that (i) spatial correlations can enhance coherences in the site basis while at the same time slowing transport, and (ii) the overall efficiency of transport is optimized at a finite temporal correlation that produces maximum overlap between the environmental power spectrum and the excitonic energy differences, which in turn results in enhanced driving of transitions between excitonic states.
The non-equilibrium stationary coherences that form in donor-acceptor systems are investigated to determine their relationship to the efficiency of energy transfer to a neighboring reaction center. It is found that the effects of asymmetry in the dimer are generally detrimental to the transfer of energy. Four types of systems are examined, arising from combinations of localized trapping, delocalized (Forster) trapping, eigenstate dephasing and site basis dephasing. In the cases of site basis dephasing the interplay between the energy gap of the excited dimer states and the environment is shown to give rise to a turnover effect in the efficiency under weak dimer coupling conditions. Furthermore, the nature of the coherences and associated flux are interpreted in terms of pathway interference effects. In addition, regardless of the cases considered, the ratio of the real part and the imaginary part of the coherences in the energy-eigenbasis tends to a constant value in the steady state limit.
Quantum coherence is one of the most striking features of quantum mechanics rooted in the superposition principle. Recently it has been demonstrated that it is possible to harvest the quantum coherence from a coherent scalar field. In order to explore a new method of detecting axion dark matter, we quantify a coherent measure of a detector and show that the detector can harvest the quantum coherence from the axion dark matter.
We propose a scheme to simulate the exciton energy transfer (EET) of photosynthetic complexes in a quantum superconducting circuit system. Our system is composed of two pairs of superconducting charge qubits coupled to two separated high-Q superconducting transmission line resonators (TLRs) connected by a capacitance. When the frequencies of the qubits are largely detuned with those of the TLRs, we simulate the process of the EET from the first qubit to the fourth qubit. By tuning the couplings between the qubits and the TLRs, and the coupling between the two TLRs, we can modify the effective coupling strengths between the qubits and thus demonstrate the geometric effects on the EET. It is shown that a moderate clustered geometry supports optimal EET by using exciton delocalization and energy matching condition. And the population loss during the EET has been trapped in the two TLRs.
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