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Register a new userClustered Geometries Exploiting Quantum Coherence Effects for Efficient Energy Transfer in Light Harvesting
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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.
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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.
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.
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.
Energy relaxation in light-harvesting complexes has been extensively studied by various ultrafast spectroscopic techniques, the fastest processes being in the sub-100 fs range. At the same time much slower dynamics have been observed in individual complexes by single-molecule fluorescence spectroscopy (SMS). In this work we employ a pump-probe type SMS technique to observe the ultrafast energy relaxation in single light-harvesting complexes LH2 of purple bacteria. After excitation at 800 nm, the measured relaxation time distribution of multiple complexes has a peak at 95 fs and is asymmetric, with a tail at slower relaxation times. When tuning the excitation wavelength, the distribution changes in both its shape and position. The observed behaviour agrees with what is to be expected from the LH2 excited states structure. As we show by a Redfield theory calculation of the relaxation times, the distribution shape corresponds to the expected effect of Gaussian disorder of the pigment transition energies. By repeatedly measuring few individual complexes for minutes, we find that complexes sample the relaxation time distribution on a timescale of seconds. Furthermore, by comparing the distribution from three long-lived complexes with the whole ensemble, we demonstrate that the ensemble can be considered ergodic. Our findings thus agree with the commonly used notion of an ensemble of identical LH2 complexes experiencing slow random fluctuations.
Photosynthetic organisms harvest light energy, utilizing the absorption and energy transfer properties of protein-bound chromophores. Controlling the harvesting efficiency is critical for the optimal function of the photosynthetic apparatus. Here, we show that cyanobacterial light-harvesting antenna may be able to regulate the flow of energy in order to switch reversibly from efficient energy conversion to photo-protective quenching via a structural change. We isolated cyanobacterial light harvesting proteins, phycocyanin and allophycocyanin, and measured their optical properties in solution and in an aggregated-desiccated state. The results indicate that energy band structures are changed, generating a switch between two modes of operation: exciton transfer and quenching; achieved without dedicated carotenoid quenchers. This flexibility can contribute greatly to the large dynamic range of cyanobacterial light harvesting systems.
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