Publication

Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex

Thyrhaug, E., Tempelaar, R., Alcocer, M. J. P., Zidek, K., Bina, D., Knoester, J., Jansen, T. L. C. & Zigmantas, D., Jul-2018, In : Nature Chemistry. 10, 7, p. 780-786 7 p.

Research output: Contribution to journalArticleAcademicpeer-review

APA

Thyrhaug, E., Tempelaar, R., Alcocer, M. J. P., Zidek, K., Bina, D., Knoester, J., ... Zigmantas, D. (2018). Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex. Nature Chemistry, 10(7), 780-786. https://doi.org/10.1038/s41557-018-0060-5

Author

Thyrhaug, Erling ; Tempelaar, Roel ; Alcocer, Marcelo J. P. ; Zidek, Karel ; Bina, David ; Knoester, Jasper ; Jansen, Thomas L. C. ; Zigmantas, Donatas. / Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex. In: Nature Chemistry. 2018 ; Vol. 10, No. 7. pp. 780-786.

Harvard

Thyrhaug, E, Tempelaar, R, Alcocer, MJP, Zidek, K, Bina, D, Knoester, J, Jansen, TLC & Zigmantas, D 2018, 'Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex', Nature Chemistry, vol. 10, no. 7, pp. 780-786. https://doi.org/10.1038/s41557-018-0060-5

Standard

Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex. / Thyrhaug, Erling; Tempelaar, Roel; Alcocer, Marcelo J. P.; Zidek, Karel; Bina, David; Knoester, Jasper; Jansen, Thomas L. C.; Zigmantas, Donatas.

In: Nature Chemistry, Vol. 10, No. 7, 07.2018, p. 780-786.

Research output: Contribution to journalArticleAcademicpeer-review

Vancouver

Thyrhaug E, Tempelaar R, Alcocer MJP, Zidek K, Bina D, Knoester J et al. Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex. Nature Chemistry. 2018 Jul;10(7):780-786. https://doi.org/10.1038/s41557-018-0060-5


BibTeX

@article{53e9f47f3f3944089a82665391c40890,
title = "Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex",
abstract = "The idea that excitonic (electronic) coherences are of fundamental importance to natural photosynthesis gained popularity when slowly dephasing quantum beats (QBs) were observed in the two-dimensional electronic spectra of the Fenna-Matthews-Olson (FMO) complex at 77 K. These were assigned to superpositions of excitonic states, a controversial interpretation, as the strong chromophore-environment interactions in the complex suggest fast dephasing. Although it has been pointed out that vibrational motion produces similar spectral signatures, a concrete assignment of these oscillatory signals to distinct physical processes is still lacking. Here we revisit the coherence dynamics of the FMO complex using polarization-controlled two-dimensional electronic spectroscopy, supported by theoretical modelling. We show that the long-lived QBs are exclusively vibrational in origin, whereas the dephasing of the electronic coherences is completed within 240 fs even at 77 K. We further find that specific vibrational coherences are produced via vibronically coupled excited states. The presence of such states suggests that vibronic coupling is relevant for photosynthetic energy transfer.",
keywords = "GREEN SULFUR BACTERIA, LIGHT-HARVESTING COMPLEX, 2-DIMENSIONAL ELECTRONIC SPECTROSCOPY, PHOTOSYNTHETIC ENERGY-TRANSFER, FMO ANTENNA PROTEIN, QUANTUM COHERENCE, CHLOROBIUM-TEPIDUM, BACTERIOCHLOROPHYLL PROTEIN, HERZBERG-TELLER, IR-SPECTROSCOPY",
author = "Erling Thyrhaug and Roel Tempelaar and Alcocer, {Marcelo J. P.} and Karel Zidek and David Bina and Jasper Knoester and Jansen, {Thomas L. C.} and Donatas Zigmantas",
year = "2018",
month = "7",
doi = "10.1038/s41557-018-0060-5",
language = "English",
volume = "10",
pages = "780--786",
journal = "Nature Chemistry",
issn = "1755-4330",
publisher = "Nature Publishing Group",
number = "7",

}

RIS

TY - JOUR

T1 - Identification and characterization of diverse coherences in the Fenna-Matthews-Olson complex

AU - Thyrhaug, Erling

AU - Tempelaar, Roel

AU - Alcocer, Marcelo J. P.

AU - Zidek, Karel

AU - Bina, David

AU - Knoester, Jasper

AU - Jansen, Thomas L. C.

AU - Zigmantas, Donatas

PY - 2018/7

Y1 - 2018/7

N2 - The idea that excitonic (electronic) coherences are of fundamental importance to natural photosynthesis gained popularity when slowly dephasing quantum beats (QBs) were observed in the two-dimensional electronic spectra of the Fenna-Matthews-Olson (FMO) complex at 77 K. These were assigned to superpositions of excitonic states, a controversial interpretation, as the strong chromophore-environment interactions in the complex suggest fast dephasing. Although it has been pointed out that vibrational motion produces similar spectral signatures, a concrete assignment of these oscillatory signals to distinct physical processes is still lacking. Here we revisit the coherence dynamics of the FMO complex using polarization-controlled two-dimensional electronic spectroscopy, supported by theoretical modelling. We show that the long-lived QBs are exclusively vibrational in origin, whereas the dephasing of the electronic coherences is completed within 240 fs even at 77 K. We further find that specific vibrational coherences are produced via vibronically coupled excited states. The presence of such states suggests that vibronic coupling is relevant for photosynthetic energy transfer.

AB - The idea that excitonic (electronic) coherences are of fundamental importance to natural photosynthesis gained popularity when slowly dephasing quantum beats (QBs) were observed in the two-dimensional electronic spectra of the Fenna-Matthews-Olson (FMO) complex at 77 K. These were assigned to superpositions of excitonic states, a controversial interpretation, as the strong chromophore-environment interactions in the complex suggest fast dephasing. Although it has been pointed out that vibrational motion produces similar spectral signatures, a concrete assignment of these oscillatory signals to distinct physical processes is still lacking. Here we revisit the coherence dynamics of the FMO complex using polarization-controlled two-dimensional electronic spectroscopy, supported by theoretical modelling. We show that the long-lived QBs are exclusively vibrational in origin, whereas the dephasing of the electronic coherences is completed within 240 fs even at 77 K. We further find that specific vibrational coherences are produced via vibronically coupled excited states. The presence of such states suggests that vibronic coupling is relevant for photosynthetic energy transfer.

KW - GREEN SULFUR BACTERIA

KW - LIGHT-HARVESTING COMPLEX

KW - 2-DIMENSIONAL ELECTRONIC SPECTROSCOPY

KW - PHOTOSYNTHETIC ENERGY-TRANSFER

KW - FMO ANTENNA PROTEIN

KW - QUANTUM COHERENCE

KW - CHLOROBIUM-TEPIDUM

KW - BACTERIOCHLOROPHYLL PROTEIN

KW - HERZBERG-TELLER

KW - IR-SPECTROSCOPY

U2 - 10.1038/s41557-018-0060-5

DO - 10.1038/s41557-018-0060-5

M3 - Article

VL - 10

SP - 780

EP - 786

JO - Nature Chemistry

JF - Nature Chemistry

SN - 1755-4330

IS - 7

ER -

ID: 62750927