The presence of quantum coherence in light-harvesting complex II (LHCII) as a mechanism to understand the efficiency of the light-harvesting function in natural photosynthetic systems is still debated due to its structural complexity and weak-amplitude coherent oscillations. Here, we revisit the coherent dynamics and clarify different types of coherences in the energy transfer processes of LHCII using a joint method of the high-S/N transient grating and two-dimensional electronic spectroscopy. We find that the electronic coherence decays completely within 50 fs at room temperature. The vibrational coherences of chlorophyll a dominate over oscillations within 1 ps, whereas a low-frequency mode of 340 cm−1 with a vibronic mixing character may participate in vibrationally assisted energy transfer between chlorophylls a. Our results may suggest that vibronic mixing is relevant for rapid energy transfer processes among chlorophylls in LHCII.
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28 March 2022
Research Article|
March 24 2022
Vibrational and vibronic coherences in the energy transfer process of light-harvesting complex II revealed by two-dimensional electronic spectroscopy
Special Collection:
Time-resolved Vibrational Spectroscopy
Ruidan Zhu
;
Ruidan Zhu
1
Beijing National Laboratory for Condensed Matter Physics, Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
2
University of Chinese Academy of Sciences
, Beijing 100049, China
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Meixia Ruan;
Meixia Ruan
1
Beijing National Laboratory for Condensed Matter Physics, Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
2
University of Chinese Academy of Sciences
, Beijing 100049, China
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Hao Li;
Hao Li
1
Beijing National Laboratory for Condensed Matter Physics, Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
2
University of Chinese Academy of Sciences
, Beijing 100049, China
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Xuan Leng
;
Xuan Leng
1
Beijing National Laboratory for Condensed Matter Physics, Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
2
University of Chinese Academy of Sciences
, Beijing 100049, China
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Jiading Zou;
Jiading Zou
1
Beijing National Laboratory for Condensed Matter Physics, Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
2
University of Chinese Academy of Sciences
, Beijing 100049, China
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Jiayu Wang
;
Jiayu Wang
1
Beijing National Laboratory for Condensed Matter Physics, Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
2
University of Chinese Academy of Sciences
, Beijing 100049, China
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Hailong Chen;
Hailong Chen
1
Beijing National Laboratory for Condensed Matter Physics, Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
3
Songshan Lake Materials Laboratory
, Dongguan, Guangdong 523808, China
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Zhuan Wang;
Zhuan Wang
1
Beijing National Laboratory for Condensed Matter Physics, Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
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Yuxiang Weng
Yuxiang Weng
a)
1
Beijing National Laboratory for Condensed Matter Physics, Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences
, Beijing 100190, China
2
University of Chinese Academy of Sciences
, Beijing 100049, China
3
Songshan Lake Materials Laboratory
, Dongguan, Guangdong 523808, China
a)Author to whom correspondence should be addressed: yxweng@iphy.ac.cn
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a)Author to whom correspondence should be addressed: yxweng@iphy.ac.cn
Note: This paper is part of the JCP Special Topic on Time-resolved Vibrational Spectroscopy.
J. Chem. Phys. 156, 125101 (2022)
Article history
Received:
December 14 2021
Accepted:
March 07 2022
Citation
Ruidan Zhu, Meixia Ruan, Hao Li, Xuan Leng, Jiading Zou, Jiayu Wang, Hailong Chen, Zhuan Wang, Yuxiang Weng; Vibrational and vibronic coherences in the energy transfer process of light-harvesting complex II revealed by two-dimensional electronic spectroscopy. J. Chem. Phys. 28 March 2022; 156 (12): 125101. https://doi.org/10.1063/5.0082280
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