Quantum Coherent Energy Transfer over Varying Pathways in Single Light-Harvesting Complexes

Hildner, Richard; Brinks, Daan; Nieder, Jana B.; Cogdell, Richard J.; Hulst, Niek F. van

doi:10.1126/science.1235820

Cited by 303 publications

(479 citation statements)

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“…Thus, we predict the formation of SMOL in molecular systems fulfilling the above-indicated requirements. Potential candidates are J-aggregates 7 , bacteriorhodopsin, quantum dot hybrid systems 8 , photoactive proteins such as PS II and light harvesting complexes [23][24][25] arranged in an organized and oriented fashion of several layers thick.…”

Section: Discussionmentioning

confidence: 99%

“…The initial steps of photosynthesis involve the absorption of photons by pigment molecules located in a protein antenna matrix, which is followed by rapid and highly efficient funnelling of exciton energy to power the reaction centres in these specialized biological light-to-chemical energy converters. There is compelling experimental evidence that long-lived electronic quantum coherence and entanglement play an important part in energy transfer processes in such systems, even at physiological temperatures [23][24][25] .…”

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confidence: 99%

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Spatial modulation of light transmission through a single microcavity by coupling of photosynthetic complex excitations to surface plasmons

et al. 2015

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Molecule-plasmon interactions have been shown to have a definite role in light propagation through optical microcavities due to strong coupling between molecular excitations and surface plasmons. This coupling can lead to macroscopic extended coherent states exhibiting increment in temporal and spatial coherency and a large Rabi splitting. Here, we demonstrate spatial modulation of light transmission through a single microcavity patterned on a freestanding Au film, strongly coupled to one of the most efficient energy transfer photosynthetic proteins in nature, photosystem I. Here we observe a clear correlation between the appearance of spatial modulation of light and molecular photon absorption, accompanied by a 13-fold enhancement in light transmission and the emergence of a distinct electromagnetic standing wave pattern in the cavity. This study provides the path for engineering various types of bio-photonic devices based on the vast diversity of biological molecules in nature.

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Section: Discussionmentioning

confidence: 99%

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confidence: 99%

Spatial modulation of light transmission through a single microcavity by coupling of photosynthetic complex excitations to surface plasmons

et al. 2015

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“…(16). As the action of the Hessian on the gradient merely rescales the gradient, this equation states that the gradient is an eigenfunction of the Hessian along a straight control trajectory, with an associated eigenvalue ρ ′′ (s) ρ ′ (s) .…”

Section: 'Straight Shot' Eigen-relationmentioning

confidence: 99%

Exploring the complexity of quantum control optimization trajectories

Nanduri

Shir

Donovan

et al. 2015

Phys. Chem. Chem. Phys.

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The control of quantum system dynamics is generally performed by seeking a suitable applied field. The physical objective as a functional of the field forms the quantum control landscape, whose topology, under certain conditions, has been shown to contain no critical point suboptimal traps, thereby enabling effective searches for fields that give the global maximum of the objective. This paper addresses the structure of the landscape as a complement to topological critical point features. Recent work showed that landscape structure is highly favorable for optimization of state-to-state transition probabilities, in that gradient-based control trajectories to the global maximum value are nearly straight paths. The landscape structure is codified in the metric R ≥ 1.0, defined as the ratio of the length of the control trajectory to the Euclidean distance between the initial and optimal controls. A value of R = 1 would indicate an exactly straight trajectory to the optimal observable value. This paper extends the state-to-state transition probability results to the quantum ensemble and unitary transformation control landscapes. Again, nearly straight trajectories predominate, and we demonstrate that R can take values approaching 1.0 with high precision. However, the interplay of optimization trajectories with critical saddle submanifolds is found to influence landscape structure. A fundamental relationship necessary for perfectly straight gradient-based control trajectories is derived, wherein the gradient on the quantum control landscape must be an eigenfunction of the Hessian. This relation is an indicator of landscape structure and may provide a means to identify physical conditions when control trajectories can achieve perfect linearity. The collective favorable landscape topology 1 and structure provide a foundation to understand why optimal quantum control can be readily achieved.

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“…P hotochemical machines in nature are powered by sunlight to execute important biological functions such as photosynthesis for light energy conversion to chemical energy and photosensory function for signal transduction [1][2][3][4][5][6] . To reach high biological efficiency, the initial photoinduced dynamics are usually ultrafast to quickly funnel excitation energy into the functional coordinate(s) and avoid futile energy dissipation into the environment [2][3][4] .…”

mentioning

confidence: 99%

“…To reach high biological efficiency, the initial photoinduced dynamics are usually ultrafast to quickly funnel excitation energy into the functional coordinate(s) and avoid futile energy dissipation into the environment [2][3][4] . In addition to photosynthesis and photosignalling, blue light energy is used as a co-substrate for repairing DNA damage by photolyase with high quantum yield 7,8 .…”

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confidence: 99%

The molecular origin of high DNA-repair efficiency by photolyase

Tan

Liu

et al. 2015

Nat Commun

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The primary dynamics in photomachinery such as charge separation in photosynthesis and bond isomerization in sensory photoreceptor are typically ultrafast to accelerate functional dynamics and avoid energy dissipation. The same is also true for the DNA repair enzyme, photolyase. However, it is not known how the photoinduced step is optimized in photolyase to attain maximum efficiency. Here, we analyse the primary reaction steps of repair of ultraviolet-damaged DNA by photolyase using femtosecond spectroscopy. With systematic mutations of the amino acids involved in binding of the flavin cofactor and the cyclobutane pyrimidine dimer substrate, we report our direct deconvolution of the catalytic dynamics with three electron-transfer and two bond-breaking elementary steps and thus the fine tuning of the biological repair function for optimal efficiency. We found that the maximum repair efficiency is not enhanced by the ultrafast photoinduced process but achieved by the synergistic optimization of all steps in the complex repair reaction.

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Quantum Coherent Energy Transfer over Varying Pathways in Single Light-Harvesting Complexes

Cited by 303 publications

References 50 publications

Spatial modulation of light transmission through a single microcavity by coupling of photosynthetic complex excitations to surface plasmons

Spatial modulation of light transmission through a single microcavity by coupling of photosynthetic complex excitations to surface plasmons

Exploring the complexity of quantum control optimization trajectories

The molecular origin of high DNA-repair efficiency by photolyase

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