Enhanced quantum entanglement in the non-Markovian dynamics of biomolecular excitons

Thorwart, Michael; Eckel, J.; Reina, John H.; Nalbach, P.; Weiss, S.

doi:10.1016/j.cplett.2009.07.053

Cited by 192 publications

(220 citation statements)

References 29 publications

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“…Interesting conceptual studies on the possible constructive role of dephasing fluctuations on the efficiency of energy transfer in networks (18)(19)(20)(21)(22)(23) were initiated subsequently. However, critical questions were also formulated (24)(25)(26)(27)(28), which remained largely unresolved up to present.…”

Section: Significancementioning

confidence: 99%

Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer

Duan

Prokhorenko

Cogdell

et al. 2017

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

285

220

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During the first steps of photosynthesis, the energy of impinging solar photons is transformed into electronic excitation energy of the light-harvesting biomolecular complexes. The subsequent energy transfer to the reaction center is commonly rationalized in terms of excitons moving on a grid of biomolecular chromophores on typical timescales <100 fs. Today's understanding of the energy transfer includes the fact that the excitons are delocalized over a few neighboring sites, but the role of quantum coherence is considered as irrelevant for the transfer dynamics because it typically decays within a few tens of femtoseconds. This orthodox picture of incoherent energy transfer between clusters of a few pigments sharing delocalized excitons has been challenged by ultrafast optical spectroscopy experiments with the FennaMatthews-Olson protein, in which interference oscillatory signals up to 1.5 ps were reported and interpreted as direct evidence of exceptionally long-lived electronic quantum coherence. Here, we show that the optical 2D photon echo spectra of this complex at ambient temperature in aqueous solution do not provide evidence of any long-lived electronic quantum coherence, but confirm the orthodox view of rapidly decaying electronic quantum coherence on a timescale of 60 fs. Our results can be considered as generic and give no hint that electronic quantum coherence plays any biofunctional role in real photoactive biomolecular complexes. Because in this structurally well-defined protein the distances between bacteriochlorophylls are comparable to those of other light-harvesting complexes, we anticipate that this finding is general and directly applies to even larger photoactive biomolecular complexes.T he principle laws of physics undoubtedly also govern the principle mechanisms of biology. The animate world consists of macroscopic and dynamically slow structures with a huge number of degrees of freedom, such that the laws of statistical mechanics apply. Conversely, the fundamental theory of the microscopic building blocks is quantum mechanics. The physics and chemistry of large molecular complexes may be considered as a bridge between the molecular world and the formation of living matter. A fascinating question since the early days of quantum theory is on the borderline between the atomistic quantum world and the classical world of biology. Clearly, the conditions under which matter displays quantum features or biological functionality are contrarious. Quantum coherent features only become apparent when systems with a few degrees of freedom with a preserved quantum mechanical phase relation of a wave function are well shielded from environmental fluctuations that otherwise lead to rapid dephasing. This dephasing mechanism is very efficient at ambient temperatures, at which biological systems operate. Also, the function of biological macromolecular systems relies on their embedding in a "wet" and highly polar solvent environment, which is again hostile to any quantum coherence. Therefore, the common view ...

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Section: Significancementioning

confidence: 99%

Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer

Duan

Prokhorenko

Cogdell

et al. 2017

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

285

220

View full text Add to dashboard Cite

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“…Examples include the hierarchical equations of motion (HEOM), [41][42][43][44][45][46] density matrix renormalisation group (and related) techniques, 25,36,47,48 and those based on the path integral formalism. [49][50][51][52] All can converge to numerically exact results in specific circumstances. In contrast, despite their attraction in terms of simplicity, intuitive physical insight and efficiency, standard (e.g., Redfield) master equations are often invalid in regimes relevant to molecular complexes due to their limitation to weak system-environment couplings.…”

Section: Introductionmentioning

confidence: 99%

Energy transfer in structured and unstructured environments: Master equations beyond the Born-Markov approximations

Iles-Smith

Dijkstra

Lambert

et al. 2016

The Journal of Chemical Physics

128

164

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Criteria for the accuracy of small polaron quantum master equation in simulating excitation energy transfer dynamics J. Chem. Phys. 139, 224112 (2013) (2014)], we go beyond the commonly used Born-Markov approximations to incorporate system-environment correlations and the resultant non-Markovian dynamical effects. We obtain energy transfer dynamics for both underdamped and overdamped oscillator environments that are in perfect agreement with the numerical hierarchical equations of motion over a wide range of parameters. Furthermore, we show that the Zusman equations, which may be obtained in a semiclassical limit of the reaction coordinate model, are often incapable of describing the correct dynamical behaviour. This demonstrates the necessity of properly accounting for quantum correlations generated between the system and its environment when the Born-Markov approximations no longer hold. Finally, we apply the reaction coordinate formalism to the case of a structured environment comprising of both underdamped (i.e., sharply peaked) and overdamped (broad) components simultaneously. We find that though an enhancement of the dimer energy transfer rate can be obtained when compared to an unstructured environment, its magnitude is rather sensitive to both the dimer-peak resonance conditions and the relative strengths of the underdamped and overdamped contributions. C 2016 AIP Publishing LLC. [http://dx

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“…[10]) to the system, a fact which has interesting ramifications from the perspective of quantum information theory [11]. For example, non-Markovian processes have been shown to preserve entanglement [12] in many-body [13] and biomolecular [14] systems, and have been exploited in quantum key distribution [15], enhancing precision in quantum metrology [16], and implementing certain quantum information protocols [17,18]. Non-Markovianity also plays a detrimental role in quantum Darwinism, thus impeding the emergence of classical objectivity from a quantum world [19].…”

Section: Introductionmentioning

confidence: 99%

Characterizing non-Markovianity via quantum interferometric power

2015

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Non-Markovian evolution in open quantum systems is often characterized in terms of the backflow of information from environment to system and is thus an important facet in investigating the performance and robustness of quantum information protocols. In this work, we explore non-Markovianity through the breakdown of monotonicity of a metrological figure of merit, called the quantum interferometric power, which is based on the minimal quantum Fisher information obtained by local unitary evolution of one part of the system, and can be interpreted as a quantifier of quantum correlations beyond entanglement. We investigate our proposed non-Markovianity indicator in two relevant examples. First, we consider the action of a single-party dephasing channel on a maximally entangled two-qubit state, by applying the Jamiołkowski-Choi isomorphism. We observe that the proposed measure is consistent with established non-Markovianity quantifiers defined using other approaches based on dynamical divisibility, distinguishability, and breakdown of monotonicity for the quantum mutual information. Further, we consider the dynamics of two-qubit Werner states, under the action of a local, single-party amplitude damping channel, and observe that the nonmonotonic evolution of the quantum interferometric power is more robust than the corresponding one for entanglement in capturing the backflow of quantum information associated with the non-Markovian process. Implications for the role of non-Markovianity in quantum metrology and possible extensions to continuous variable systems are discussed.

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Enhanced quantum entanglement in the non-Markovian dynamics of biomolecular excitons

Cited by 192 publications

References 29 publications

Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer

Nature does not rely on long-lived electronic quantum coherence for photosynthetic energy transfer

Energy transfer in structured and unstructured environments: Master equations beyond the Born-Markov approximations

Characterizing non-Markovianity via quantum interferometric power

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