Strategies to enhance the excitation energy-transfer efficiency in a light-harvesting system using the intra-molecular charge transfer character of carotenoids

Nao Yukihira, Yuko Sugai, Masazumi Fujiwara, Daisuke Kosumi, Masahiko Iha, Kazuhiko Sakaguchi, Shigeo Katsumura, Alastair T. Gardiner, Richard J. Cogdell, Hideki Hashimoto

Research output: Contribution to journalArticlepeer-review

5 Citations (Scopus)

Abstract

Fucoxanthin is a carotenoid that is mainly found in light-harvesting complexes from brown algae and diatoms. Due to the presence of a carbonyl group attached to polyene chains in polar environments, excitation produces an excited intra-molecular charge transfer. This intra-molecular charge transfer state plays a key role in the highly efficient (∼95%) energy-transfer from fucoxanthin to chlorophyll a in the light-harvesting complexes from brown algae. In purple bacterial light-harvesting systems the efficiency of excitation energy-transfer from carotenoids to bacteriochlorophylls depends on the extent of conjugation of the carotenoids. In this study we were successful, for the first time, in incorporating fucoxanthin into a light-harvesting complex 1 from the purple photosynthetic bacterium, Rhodospirillum rubrum G9+ (a carotenoidless strain). Femtosecond pump-probe spectroscopy was applied to this reconstituted light-harvesting complex in order to determine the efficiency of excitation energy-transfer from fucoxanthin to bacteriochlorophyll a when they are bound to the light-harvesting 1 apo-proteins.

Original languageEnglish
Pages (from-to)59-71
Number of pages13
JournalFaraday Discussions
Volume198
DOIs
Publication statusPublished - 2017
Externally publishedYes

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

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