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Coherent oscillations in chlorosome elucidated by two-dimensional electronic spectroscopy

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Title
Coherent oscillations in chlorosome elucidated by two-dimensional electronic spectroscopy
Author(s)
Sunhong Jun; Cheolhee Yang; Isaji M.; Tamiaki H.; Kim J.; Hyot Cherl Ihee
Publication Date
2014-04
Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, v.5, no.8, pp.1386 - 1392
Publisher
AMER CHEMICAL SOC
Abstract
Chlorosomes are the most efficient photosynthetic light-harvesting complexes found in nature and consist of many bacteriochlorophyll (BChl) molecules self-assembled into supramolecular aggregates. Here we elucidate the presence and the origin of coherent oscillations in chlorosome at cryogenic temperature using 2D electronic spectroscopy. We observe coherent oscillations of multiple frequencies superimposed on the ultrafast amplitude decay of 2D spectra. Comparison of oscillatory features in the rephasing and nonrephasing 2D spectra suggests that an oscillation of 620 cm-1 frequency arises from electronic coherence. However, this coherent oscillation can be enhanced by vibronic coupling with intermolecular vibrations of BChl aggregate, and thus it might originate from vibronic coherence rather than pure electronic coherence. Although the 620 cm-1 oscillation dephases rapidly, the electronic (or vibronic) coherence may still take part in the initial step of energy transfer in chlorosome, which is comparably fast. © 2014 American Chemical Society.
URI
https://pr.ibs.re.kr/handle/8788114/1174
ISSN
1948-7185
Appears in Collections:
Center for Nanomaterials and Chemical Reactions(나노물질 및 화학반응 연구단) > Journal Papers (저널논문)
Files in This Item:
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