Exciton transfer dynamics and quantumness of energy transfer in the Fenna-Matthews-Olson complex

Nalbach, P.; Braun, Daniel; Thorwart, Michael

doi:10.1103/physreve.84.041926

Cited by 144 publications

(193 citation statements)

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“…However, previous calculations of 2d-echo spectra of seven-site FMO complex have been often performed with a single-peak Drude-Lorentz spectral density [18,19], and did not yield long-lasting cross-peak oscillations. The situation is different in the population dynamics, which has been analyzed for different spectral densities [26] and yields no significant differences in the duration of population beatings for different spectral density.…”

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“…Realistic models of the exciton dynamics in the FMO complex have to include higher order phonon processes as well as the finite time scale of the reorganization process [17]. This requires to go beyond approximative rate equations [23] and non-perturbative techniques [24][25][26][27][28][29][30] are necessary to study the dissipative transfer dynamics.One key parameter determining the duration of coherent oscillations is the spectral density, which encodes the the mode-dependent exciton-bath coupling. The spectral density has important implications for the two contributions to the decoherence rate γ which is the sum of the relaxation rate γ r and the pure-dephasing rate γ d ([33], ch.…”

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Long-Lived Electronic Coherence in Dissipative Exciton Dynamics of Light-Harvesting Complexes

Kreisbeck

Kramer

2012

J. Phys. Chem. Lett.

236

320

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The observed prevalence of oscillatory signals in the spectroscopy of biological light-harvesting complexes at ambient temperatures has led to a search for mechanisms supporting coherent transport through larger molecules in noisy environments. We demonstrate a generic mechanism supporting long-lasting electronic coherence up to 0.3 ps at a temperature of 277 K. The mechanism relies on two properties of the spectral density: (i) a large dissipative coupling to a continuum of higherfrequency vibrations required for efficient transport and (ii) a small slope of the spectral density at zero frequency.PACS numbers: 03.65. Yz, 78.47.nj, 05.60.Gg Long-lasting oscillatory signals in optically excited light-harvesting complexes (LHCs) point towards the prevalence of a coherent electronic dynamics in molecular networks at physiological temperatures [2][3][4][5]. The experiments probe the electronic dynamics using twodimensional (2d) echo-spectroscopy for a series of delaytimes between the excitation pulse and the probe pulse. The 2d spectroscopy makes studies of the dynamics of dissipative systems possible and has found further applications in mesoscopic systems such as molecular nanotubes [6] and semiconductor devices [7]. Due to its known crystallographic structure and relative simplicity, the Fenna-Matthews-Olson (FMO) complex serves as the prototype system for studying the choreography of the energy transfer from the antenna to the reaction center of a light harvesting complex [8]. In 2d spectra long-lasting beatings are observed, ranging from 1.2 ps at T = 150 K to 0.3 ps at T = 277 K [9]. The interplay of coherent dynamics, which leads to a delocalization of an initial excitation arriving at the FMO network from the antenna, and the coupling to a vibronic environment with slow and fast fluctuations, has lead to studies of environmentally assisted transport in LHCs [10,11].An important open question is whether coherence plays a key-role in the functioning of light-harvesting complexes [8]. The theoretical understanding of the experiments is in its early stages and atomistic simulations based on molecular dynamics have not reached agreement [12,13]. A calculation of 2d echo-spectra based on the molecular dynamics simulation [14] does not show clear coherent oscillations at T = 277 K. One key ingredient for efficient transfer dynamics is the strong coupling to vibronic modes, which induces energy dissipation [10,11,15]. For the FMO complex the thermalization occurs within picoseconds and was observed by Brixner et al. by the decay of diagonal-peak amplitudes to lower energies [16]. It has been proposed that the inclusion of the finite time scale of the reorganization process gives rise to long-lasting coherence in LHCs [17]. While a sluggish bath relaxation leads to prolonged population beatings in the FMO network, calculations of 2d echo-spectra show oscillations of the exciton cross-peaks for only about 1/6th of the experimentally recorded time at T = 150 K [18]. For an even longer bath-relaxation cross-peak osci...

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Long-Lived Electronic Coherence in Dissipative Exciton Dynamics of Light-Harvesting Complexes

Kreisbeck

Kramer

2012

J. Phys. Chem. Lett.

236

320

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“…Recent femtosecond experiments in photosynthetic complexes have revived the interest in the same issues. Oscillatory temporal features in 2D spectra have been initially attributed to electronic coherence but growing evidence indicates that this could be due as well to strongly coupled vibronic motions (37)(38)(39)(40). The simplest approach to energy transfer is based on the Redfield equations that treat the system/bath coupling perturbatively to second order.…”

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Photosynthetic reaction center as a quantum heat engine

Dorfman

Voronine

Mukamel

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

283

339

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Two seemingly unrelated effects attributed to quantum coherence have been reported recently in natural and artificial light-harvesting systems. First, an enhanced solar cell efficiency was predicted and second, population oscillations were measured in photosynthetic antennae excited by sequences of coherent ultrashort laser pulses. Because both systems operate as quantum heat engines (QHEs) that convert the solar photon energy to useful work (electric currents or chemical energy, respectively), the question arises whether coherence could also enhance the photosynthetic yield. Here, we show that both effects arise from the same population-coherence coupling term which is induced by noise, does not require coherent light, and will therefore work for incoherent excitation under natural conditions of solar excitation. Charge separation in light-harvesting complexes occurs in a pair of tightly coupled chlorophylls (the special pair) at the heart of photosynthetic reaction centers of both plants and bacteria. We show the analogy between the energy level schemes of the special pair and of the laser/photocell QHEs, and that both population oscillations and enhanced yield have a common origin and are expected to coexist for typical parameters. We predict an enhanced yield of 27% in a QHE motivated by the reaction center. This suggests nature-mimicking architectures for artificial solar energy devices.photosynthesis | quantum biology | population oscillations | quantum coherence A ccording to the laws of quantum thermodynamics, quantum heat engines (QHEs) convert hot thermal radiation into low-entropy useful work (1, 2). The ultimate efficiency of such QHEs is usually governed by a detailed balance between absorption and emission of the hot pump radiation (3). The laser is an example of a QHE, which can use incoherent pump (heat) radiation to produce highly coherent (low-entropy) light ( Fig. 1 A and B). Moreover, it was demonstrated both theoretically and experimentally that noise-induced quantum coherence (4) can break detailed balance and yield lasers without population inversion (5) and/or with enhanced efficiency (Fig. 1C).Recently it has been shown that quantum coherence can, in principle, enhance the efficiency of a solar cell or a photodetector (6-10). This photocell QHE (Fig. 1D) can be described by the same model as the laser QHE (Fig. 1E) and obeys similar detailed balance physics. To use the broad solar spectrum and eliminate phonon loss, we separate solar flux into narrow frequency intervals and direct it onto a cell array where each of the cells has been prepared to have its band gap equal to that photon energy (7). In particular, Shockley and Queisser (11) invoked detailed balance to show that the open-circuit voltage of a photocell is related to the energy input of a "hot" monochromatic thermal light by the Carnot factor. However, just as in the case of the laser, we can, in principle, break detailed balance by inducing coherence (Fig. 1F), which can enhance the photocell efficiency (9, 10).Other recent p...

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“…A number of microscopic models have been developed and their studies highlight the possibility of quantum coherence playing an important role in, for example, the energy and charge transfer process in mesoscopic bio-chemical systems [1][2][3][4][5][6][7] or artificial photosynthetic complexes [8,9]. At the same time first experimental studies have shown that quantum coherence can play a significant role in photosynthetic light-harvesting complexes [10][11][12] and in chromophoric energy transport [13].…”

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confidence: 99%

Noise-enhanced quantum transport on a closed loop using quantum walks

Chandrashekar

Busch

2014

Quantum Inf Process

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We study the effect of noise on the transport of a quantum state from a closed loop of n−sites with one of the sites as a sink. Using a discrete-time quantum walk dynamics, we demonstrate that the transport efficiency can be enhanced with noise when the number of sites in the loop is small and reduced when the number of sites in the loop grows. By using the concept of measurement induced disturbance we identify the regimes in which genuine quantum effects are responsible for the enhanced transport.

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Exciton transfer dynamics and quantumness of energy transfer in the Fenna-Matthews-Olson complex

Cited by 144 publications

References 43 publications

Long-Lived Electronic Coherence in Dissipative Exciton Dynamics of Light-Harvesting Complexes

Long-Lived Electronic Coherence in Dissipative Exciton Dynamics of Light-Harvesting Complexes

Photosynthetic reaction center as a quantum heat engine

Noise-enhanced quantum transport on a closed loop using quantum walks

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