Quantum coherence as a witness of vibronically hot energy transfer in bacterial reaction center

Paleček, David; Edlund, Petra; Westenhoff, Sebastian; Zigmantas, Donatas

doi:10.1126/sciadv.1603141

Cited by 71 publications

(106 citation statements)

References 41 publications

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“…These resonances lead to inseparability of nuclear and electronic degrees of freedom (96,97), which some theoretical work has suggested may affect energy transfer (98). These resonances have also been reported in photosynthetic reaction centers (89,99,100). Yet, the character of a quantum state, which is initially strongly vibronic in nature, changes over time in a nontrivial way when the electronic and vibrational sectors are exposed to different dephasing and relaxation channels on very different time scales.…”

Section: Present Status Of Experiments: Revisiting Fmomentioning

confidence: 87%

“…In the presence of vibronic mixing of electronic and vibrational stateswhich seems to be the case in many photosynthetic complexescoherence signals are very much entangled, and an oscillation map analysis (Fig. 4) is indispensable (89). To outline a basic framework for the interpretation of QBs in 2D spectra and to provide readers with some basic tools to qualitatively assess 2D experiments on QBs, we schematically show their analysis in two relevant model systems in Fig.…”

Section: Studies Of Photosynthetic Excitonsmentioning

confidence: 99%

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Quantum biology revisited

et al. 2020

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Photosynthesis is a highly optimized process from which valuable lessons can be learned about the operating principles in nature. Its primary steps involve energy transport operating near theoretical quantum limits in efficiency. Recently, extensive research was motivated by the hypothesis that nature used quantum coherences to direct energy transfer. This body of work, a cornerstone for the field of quantum biology, rests on the interpretation of small-amplitude oscillations in two-dimensional electronic spectra of photosynthetic complexes. This Review discusses recent work reexamining these claims and demonstrates that interexciton coherences are too short lived to have any functional significance in photosynthetic energy transfer. Instead, the observed long-lived coherences originate from impulsively excited vibrations, generally observed in femtosecond spectroscopy. These efforts, collectively, lead to a more detailed understanding of the quantum aspects of dissipation. Nature, rather than trying to avoid dissipation, exploits it via engineering of exciton-bath interaction to create efficient energy flow.

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Section: Present Status Of Experiments: Revisiting Fmomentioning

confidence: 87%

Section: Studies Of Photosynthetic Excitonsmentioning

confidence: 99%

Quantum biology revisited

et al. 2020

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“…Obviously, since the detected oscillation signals originate from all the possible Liouville pathways including the excitonic and single-mode or multi-mode vibrationally coupled coherences, new methods either of apparatus or data analysis are called for clear distinguishing the electronic coherence from those of vibronic. It has been shown that the polarization modulated [67,68] 2DES can be an effective way toward this purpose as successfully demonstrated in a recent experiment, where the oscillation maps extracted from the doublecross polarized schemes (relative polarizations of π/4, −π/4, π/2, and 0 for laser pulses 1 to 4) strongly suppresses signals of intramolecular vibrational coherences produced by the Franck-Condon excitation of vibrational wave packets [69]. On the other hand, 2D singletime-domain exciton perturbation spectroscopy (2D-STEPS) and 2D time-resolved interexciton perturbation spectroscopy (2D-TRIPS) are the new approaches to extract information from 2DES spectra.…”

Section: Single-vibrational Mode Versus Multi-vibrational Mode Coumentioning

confidence: 92%

Detection of Electronic Coherence via Two-Dimensional Electronic Spectroscopy in Condensed Phase

Weng

2018

Chinese Journal of Chemical Physics

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Two dimensional Fourier transform electronic spectroscopy (2DES) in the visible region enables direct observation of complex dynamics of molecules including quantum coherence in the condensed phase. This review aims to provide a bridge between the principles and intuitive physical description of 2DES for tutorial purpose. Special emphasis is laid upon how 2DES circumvents the restrictions from both uncertainty principle and the wave-packet collapse during the coherent detection, leading to the successful detection of the coherence in terms of energy difference between the eigenstates showing as the quantum beats; then upon the possible mixing among the pure electronic transition, single-mode and multi-mode coupled vibronic transition leading to the observed beating phenomena. Finally, recent advances in experimentally distinguishing between the electronic coherence and the vibrational coherence are briefly discussed.

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“…sphaeroides RC. 46 On the basis of this mechanism, the 33 and 153 cm –1 oscillations can be assigned to excited-state vibronic coherence followed by a shift into the ground-state vibrational coherence. The assignment of the 235 cm –1 oscillations was not as definite as the 33 and 153 cm –1 ones.…”

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confidence: 98%

Vibronic Coherence in the Charge Separation Process of the Rhodobacter sphaeroides Reaction Center

Romero

Jones

et al. 2018

J. Phys. Chem. Lett.

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Two-dimensional electronic spectroscopy was applied to a variant of the reaction center (RC) of purple bacterium Rhodobacter sphaeroides lacking the primary acceptor ubiquinone in order to understand the ultrafast separation and transfer of charge between the bacteriochlorin cofactors. For the first time, characteristic 2D spectra were obtained for the participating excited and charge-transfer states, and the electron-transfer cascade (including two different channels, the P* and B* channels) was fully mapped. By analyzing quantum beats using 2D frequency maps, excited-state vibrational modes at 153 and 33 cm–1 were identified. We speculate that these modes couple to the charge separation (CS) process and collectively optimize the CS and are responsible for the superhigh efficiency.

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Quantum coherence as a witness of vibronically hot energy transfer in bacterial reaction center

Abstract: Observation of coherence shifts reveals hot energy transfer and excess energy dissipation mechanisms in photosynthesis.

Cited by 71 publications

References 41 publications

Quantum biology revisited

Quantum biology revisited

Detection of Electronic Coherence via Two-Dimensional Electronic Spectroscopy in Condensed Phase

Vibronic Coherence in the Charge Separation Process of the Rhodobacter sphaeroides Reaction Center

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