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Originally published as Biophys J. BioFAST on March 24, 2006.
doi:10.1529/biophysj.105.076612
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Biophysical Journal 90:4145-4154 (2006)
© 2006 The Biophysical Society

Ultrafast Carotenoid-to-Chlorophyll Singlet Energy Transfer in the Cytochrome b6f Complex from Bryopsis corticulans

Ping Zuo *, Bin-Xing Li {dagger}, Xiao-Hui Zhao *, Yi-Shi Wu *, Xi-Cheng Ai *, Jian-Ping Zhang *, Liang-Bi Li {dagger} and Ting-Yun Kuang {dagger}

* State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100080, People's Republic of China; and {dagger} Key Laboratory of Photosynthesis and Environmental Molecular Physiology, Institute of Botany, Chinese Academy of Sciences, Beijing 100093, People's Republic of China

Correspondence: Address reprint requests to Prof. Jian-Ping Zhang, No. 2, 1st North St., Zhongguancun, Beijing, People's Republic of China. Tel.: 86-10-82616163; Fax: 86-10-82616163; E-mail: jpzhang{at}mail.iccas.ac.cn; or Prof. Liang-Bi Li, No. 20, Nanxincun, Xiangshan, Beijing, People's Republic of. China. Tel.: 86-10-62836248; Fax: 86-10-82594106; E-mail: lbli{at}ibcas.ac.cn.

Ultrafast carotenoid-to-chlorophyll (Car-to-Chl) singlet excitation energy transfer in the cytochrome b6f (Cyt b6f) complex from Bryopsis corticulans is investigated by the use of femtosecond time-resolved absorption spectroscopy. For all-trans-{alpha}-carotene free in n-hexane, the lifetimes of the two low-lying singlet excited states, S1(2Ag–) and S2(1Bu+), are determined to be 14.3 ± 0.4 ps and 230 ± 10 fs, respectively. For the Cyt b6f complex, to which 9-cis-{alpha}-carotene is bound, the lifetime of the S1(2Ag–) state remains unchanged, whereas that of the S2(1Bu+) state is significantly reduced. In addition, a decay-to-rise correlation between the excited-state dynamics of {alpha}-carotene and Chl a is clearly observed. This spectroscopic evidence proves that the S2(1Bu+) state is able to transfer electronic excitations to the Qx state of Chl a, whereas the S1(2Ag–) state remains inactive. The time constant and the partial efficiency of the energy transfer are determined to be 240 ± 40 fs and (49 ± 4)%, respectively, which supports the overall efficiency of 24% determined with steady-state fluorescence spectroscopy. A scheme of the {alpha}-carotene-to-Chl a singlet energy transfer is proposed based on the excited-state dynamics of the pigments.




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