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Two-dimensional spectroscopy of electronic couplings in photosynthesis

Author

Listed:
  • Tobias Brixner

    (University of California
    Lawrence Berkeley National Laboratory)

  • Jens Stenger

    (University of California
    Lawrence Berkeley National Laboratory)

  • Harsha M. Vaswani

    (University of California
    Lawrence Berkeley National Laboratory)

  • Minhaeng Cho

    (Korea University)

  • Robert E. Blankenship

    (Arizona State University)

  • Graham R. Fleming

    (University of California)

Abstract

Time-resolved optical spectroscopy is widely used to study vibrational and electronic dynamics by monitoring transient changes in excited state populations on a femtosecond timescale1. Yet the fundamental cause of electronic and vibrational dynamics—the coupling between the different energy levels involved—is usually inferred only indirectly. Two-dimensional femtosecond infrared spectroscopy based on the heterodyne detection of three-pulse photon echoes2,3,4,5,6,7 has recently allowed the direct mapping of vibrational couplings, yielding transient structural information. Here we extend the approach to the visible range3,8 and directly measure electronic couplings in a molecular complex, the Fenna–Matthews–Olson photosynthetic light-harvesting protein9,10. As in all photosynthetic systems, the conversion of light into chemical energy is driven by electronic couplings that ensure the efficient transport of energy from light-capturing antenna pigments to the reaction centre11. We monitor this process as a function of time and frequency and show that excitation energy does not simply cascade stepwise down the energy ladder. We find instead distinct energy transport pathways that depend sensitively on the detailed spatial properties of the delocalized excited-state wavefunctions of the whole pigment–protein complex.

Suggested Citation

  • Tobias Brixner & Jens Stenger & Harsha M. Vaswani & Minhaeng Cho & Robert E. Blankenship & Graham R. Fleming, 2005. "Two-dimensional spectroscopy of electronic couplings in photosynthesis," Nature, Nature, vol. 434(7033), pages 625-628, March.
  • Handle: RePEc:nat:nature:v:434:y:2005:i:7033:d:10.1038_nature03429
    DOI: 10.1038/nature03429
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    Cited by:

    1. Daniel Timmer & Moritz Gittinger & Thomas Quenzel & Sven Stephan & Yu Zhang & Marvin F. Schumacher & Arne Lützen & Martin Silies & Sergei Tretiak & Jin-Hui Zhong & Antonietta De Sio & Christoph Lienau, 2023. "Plasmon mediated coherent population oscillations in molecular aggregates," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Tobias Eul & Eva Prinz & Michael Hartelt & Benjamin Frisch & Martin Aeschlimann & Benjamin Stadtmüller, 2022. "Coherent response of the electronic system driven by non-interfering laser pulses," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    3. Arif Ullah & Pavlo O. Dral, 2022. "Predicting the future of excitation energy transfer in light-harvesting complex with artificial intelligence-based quantum dynamics," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    4. Ruidan Zhu & Wenjun Li & Zhanghe Zhen & Jiading Zou & Guohong Liao & Jiayu Wang & Zhuan Wang & Hailong Chen & Song Qin & Yuxiang Weng, 2024. "Quantum phase synchronization via exciton-vibrational energy dissipation sustains long-lived coherence in photosynthetic antennas," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    5. Magnus Röding & Siobhan J Bradley & Nathan H Williamson & Melissa R Dewi & Thomas Nann & Magnus Nydén, 2016. "The Power of Heterogeneity: Parameter Relationships from Distributions," PLOS ONE, Public Library of Science, vol. 11(5), pages 1-11, May.

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