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Jun, Sunhong
나노물질 및 화학반응 연구단
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Exciton delocalization length in chlorosomes investigated by lineshape dynamics of two-dimensional electronic spectra

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Title
Exciton delocalization length in chlorosomes investigated by lineshape dynamics of two-dimensional electronic spectra
Author(s)
Sunhong Jun; Cheolhee Yang; Choi, Seungjoo; Isaji, Megumi; Tamiaki, Hitoshi; Hyotcherl Ihee; Kim, Jeongho
Publication Date
2021-11-03
Journal
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, v.23, no.42, pp.24111 - 24117
Publisher
ROYAL SOC CHEMISTRY
Abstract
A chlorosome, a photosynthetic light-harvesting complex found in green sulfur bacteria, is an aggregate of self-assembled pigments and is optimized for efficient light harvesting and energy transfer under dim-light conditions. In this highly-disordered aggregate, the absorption and transfer of photoexcitation energy are governed by the degree of disorder. To describe the disorder, the number of molecules forming excitons, which is termed exciton delocalization length (EDL), is a relevant parameter because the EDL sensitively changes with the disorder of the constituent molecules. In this work, we determined the EDL in chlorosomes using two-dimensional electronic spectroscopy (2D-ES). Since spectral features correlated with EDL are spread out in the two-dimensional (2D) electronic spectra, we were able to determine the EDL accurately without the effects of homogeneous and inhomogeneous line broadening. In particular, by taking advantage of the multi-dimensionality and the time evolution of 2D spectra, we not only determined the excitation frequency dependence of EDL but also monitored the temporal change of EDL. We found that the EDL is similar to 7 at 77 K and similar to 6 at 298 K and increases with the excitation frequency, with the maximum located well above the maximum of the absorption spectrum of chlorosomes. The spectral profile of EDL changes rapidly within 100 fs and becomes flat over time due to dephasing of initial exciton coherence. From the coherent oscillations superimposed on the decay of EDL, it was learned that high-frequency phonons are more activated at 298 K than at 77 K.
URI
https://pr.ibs.re.kr/handle/8788114/10340
DOI
10.1039/d1cp03413h
ISSN
1463-9076
Appears in Collections:
Center for Nanomaterials and Chemical Reactions(나노물질 및 화학반응 연구단) > 1. Journal Papers (저널논문)
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