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

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

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.

Original languageEnglish
Pages (from-to)1827-1832
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume9
Issue number8
Early online date27 Mar 2018
DOIs
Publication statusPublished - Apr 2018

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polarization (charge separation)
bacteria
vibration mode
synchronism
electron transfer
cascades
Ubiquinone
charge transfer
Excited states
Charge transfer
electronics
Spectroscopy
spectroscopy
excitation
Electrons

Cite this

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title = "Vibronic Coherence in the Charge Separation Process of the Rhodobacter sphaeroides Reaction Center",
abstract = "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.",
author = "Fei Ma and Elisabet Romero and Jones, {Michael R.} and Novoderezhkin, {Vladimir I.} and {van Grondelle}, Rienk",
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Vibronic Coherence in the Charge Separation Process of the Rhodobacter sphaeroides Reaction Center. / Ma, Fei; Romero, Elisabet; Jones, Michael R.; Novoderezhkin, Vladimir I.; van Grondelle, Rienk.

In: Journal of Physical Chemistry Letters, Vol. 9, No. 8, 04.2018, p. 1827-1832.

Research output: Contribution to JournalArticleAcademicpeer-review

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T1 - Vibronic Coherence in the Charge Separation Process of the Rhodobacter sphaeroides Reaction Center

AU - Ma, Fei

AU - Romero, Elisabet

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AU - Novoderezhkin, Vladimir I.

AU - van Grondelle, Rienk

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AB - 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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