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Vibrational Modes Promoting Exciton Relaxation in the B850 Band of LH2

Authors
Kim, J.Nguyen-Phan, T.C.Gardiner, A.T.Yoon, T.H.Cogdell, R.J.Cho, M.Scholes, G.D.
Issue Date
3-2월-2022
Publisher
NLM (Medline)
Citation
The journal of physical chemistry letters, v.13, no.4, pp.1099 - 1106
Indexed
SCIE
SCOPUS
Journal Title
The journal of physical chemistry letters
Volume
13
Number
4
Start Page
1099
End Page
1106
URI
https://scholar.korea.ac.kr/handle/2021.sw.korea/136597
DOI
10.1021/acs.jpclett.1c03868
ISSN
1948-7185
Abstract
Exciton relaxation dynamics in multichromophore systems are often modeled using Redfield theory, where bath fluctuations mediate the relaxation among the exciton eigenstates. Identifying the vibrational or phonon modes that are implicated in exciton relaxation allows more detailed understanding of exciton dynamics. Here we focus on a well-studied light-harvesting II complex (LH2) isolated from the photosynthetic purple bacterium Rhodoblastus acidophilus strain 10050. Using two synchronized mode-locked lasers, we carried out a polarization-dependent two-dimensional electronic spectroscopy (2DES) study of an ultrafast exciton relaxation in the B850 band of LH2. 2DES data with different polarization configurations enable us to investigate the exciton relaxation between the k = ±1 exciton states. Then, we identify vibrational modes coupled to the exciton relaxation by analyzing the coherent wavepackets in the 2DES signals. Focusing on the coherent vibrational wavepackets, the data suggest that certain symmetry-breaking modes of monomeric units play a key role in exciton relaxation.
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