Low-Frequency Vibronic Mixing Modulates the Excitation Energy Flow in Bacterial Light-Harvesting Complex II

Junwoo Kim; Tu C. Nguyen-Phan; Alastair T. Gardiner; Richard J. Cogdell; Gregory D. Scholes; Minhaeng Cho

doi:10.1021/acs.jpclett.1c01782

Low-Frequency Vibronic Mixing Modulates the Excitation Energy Flow in Bacterial Light-Harvesting Complex II

Junwoo Kim, Tu C. Nguyen-Phan, Alastair T. Gardiner, Richard J. Cogdell, Gregory D. Scholes, Minhaeng Cho

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

12 Citations (Scopus)

Abstract

Oscillatory features observed in two-dimensional electronic spectroscopy (2DES) manifest coherent vibrational and electronic dynamics and even the interplay of them. Recently, we developed a 2DES technique utilizing a pair of synchronized repetition-frequency-stabilized lasers, which enables the wide dynamic range measurements of 2DES signals rapidly. Here, we apply this dual-laser 2DES technique to investigate the electronic energy transfer (EET) process in bacterial light-harvesting complex II consisting of B800 and B850 circular aggregates at ambient temperature, and the coherent vibrational wavepakcet associated with the EET between the two aggregates are measured. Examining the principal component analysis of the time-resolved 2DES signal, we found that the EET from B800 to low-lying B850 states is modulated by a low-frequency (156 cm-1) vibrational mode of the exciton donor (B800). This observation suggests that the donor transition density is modulated by this vibration, which, in turn, modulates the energy transfer dynamics.

Original language	English
Pages (from-to)	6292-6298
Number of pages	7
Journal	Journal of Physical Chemistry Letters
Volume	12
Issue number	27
DOIs	https://doi.org/10.1021/acs.jpclett.1c01782
Publication status	Published - 2021 Jul 15

Bibliographical note

Funding Information:
This work was supported by the W. M. Keck Foundation through Award No. 1005586 (J.K. and G.D.S.) and by IBS-R023-D1 (M.C.). C.T.N. and R.J.C. were supported by BBRSC Grant No. BB/N016734/1. A.T.G. and R.J.C. gratefully acknowledge funding from the Photosynthetic Antenna Research Center, an Energy Frontier Research Center funded by the Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award No. DE-SC0001035.

Publisher Copyright:
©

ASJC Scopus subject areas

General Materials Science
Physical and Theoretical Chemistry

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title = "Low-Frequency Vibronic Mixing Modulates the Excitation Energy Flow in Bacterial Light-Harvesting Complex II",

abstract = "Oscillatory features observed in two-dimensional electronic spectroscopy (2DES) manifest coherent vibrational and electronic dynamics and even the interplay of them. Recently, we developed a 2DES technique utilizing a pair of synchronized repetition-frequency-stabilized lasers, which enables the wide dynamic range measurements of 2DES signals rapidly. Here, we apply this dual-laser 2DES technique to investigate the electronic energy transfer (EET) process in bacterial light-harvesting complex II consisting of B800 and B850 circular aggregates at ambient temperature, and the coherent vibrational wavepakcet associated with the EET between the two aggregates are measured. Examining the principal component analysis of the time-resolved 2DES signal, we found that the EET from B800 to low-lying B850 states is modulated by a low-frequency (156 cm-1) vibrational mode of the exciton donor (B800). This observation suggests that the donor transition density is modulated by this vibration, which, in turn, modulates the energy transfer dynamics. ",

author = "Junwoo Kim and Nguyen-Phan, {Tu C.} and Gardiner, {Alastair T.} and Cogdell, {Richard J.} and Scholes, {Gregory D.} and Minhaeng Cho",

note = "Funding Information: This work was supported by the W. M. Keck Foundation through Award No. 1005586 (J.K. and G.D.S.) and by IBS-R023-D1 (M.C.). C.T.N. and R.J.C. were supported by BBRSC Grant No. BB/N016734/1. A.T.G. and R.J.C. gratefully acknowledge funding from the Photosynthetic Antenna Research Center, an Energy Frontier Research Center funded by the Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award No. DE-SC0001035. Publisher Copyright: {\textcopyright} ",

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N2 - Oscillatory features observed in two-dimensional electronic spectroscopy (2DES) manifest coherent vibrational and electronic dynamics and even the interplay of them. Recently, we developed a 2DES technique utilizing a pair of synchronized repetition-frequency-stabilized lasers, which enables the wide dynamic range measurements of 2DES signals rapidly. Here, we apply this dual-laser 2DES technique to investigate the electronic energy transfer (EET) process in bacterial light-harvesting complex II consisting of B800 and B850 circular aggregates at ambient temperature, and the coherent vibrational wavepakcet associated with the EET between the two aggregates are measured. Examining the principal component analysis of the time-resolved 2DES signal, we found that the EET from B800 to low-lying B850 states is modulated by a low-frequency (156 cm-1) vibrational mode of the exciton donor (B800). This observation suggests that the donor transition density is modulated by this vibration, which, in turn, modulates the energy transfer dynamics.

AB - Oscillatory features observed in two-dimensional electronic spectroscopy (2DES) manifest coherent vibrational and electronic dynamics and even the interplay of them. Recently, we developed a 2DES technique utilizing a pair of synchronized repetition-frequency-stabilized lasers, which enables the wide dynamic range measurements of 2DES signals rapidly. Here, we apply this dual-laser 2DES technique to investigate the electronic energy transfer (EET) process in bacterial light-harvesting complex II consisting of B800 and B850 circular aggregates at ambient temperature, and the coherent vibrational wavepakcet associated with the EET between the two aggregates are measured. Examining the principal component analysis of the time-resolved 2DES signal, we found that the EET from B800 to low-lying B850 states is modulated by a low-frequency (156 cm-1) vibrational mode of the exciton donor (B800). This observation suggests that the donor transition density is modulated by this vibration, which, in turn, modulates the energy transfer dynamics.

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Low-Frequency Vibronic Mixing Modulates the Excitation Energy Flow in Bacterial Light-Harvesting Complex II

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