Vibrational and vibronic coherences in the energy transfer process of light-harvesting complex II revealed by two-dimensional electronic spectroscopy

Author:

Zhu Ruidan12ORCID,Ruan Meixia12,Li Hao12,Leng Xuan12ORCID,Zou Jiading12,Wang Jiayu12ORCID,Chen Hailong13,Wang Zhuan1,Weng Yuxiang123ORCID

Affiliation:

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

Abstract

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.

Funder

Ministry of Science and Technology of the People’s Republic of China

Key Project of Frontier Science Research of Chinese Academy of Sciences

Strategic Priority Research Program of Chinese Academy of Sciences

Publisher

AIP Publishing

Subject

Physical and Theoretical Chemistry,General Physics and Astronomy

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