Structure of the light-harvesting bacteriochlorophyll c assembly in chlorosomes from Chlorobium limicola determined by solid-state NMR

被引:89
作者
Egawa, Ayako
Fujiwara, Toshimichi
Mizoguchi, Tadashi
Kakitani, Yoshinori
Koyama, Yasushi
Akutsu, Hideo
机构
[1] Osaka Univ, Inst Prot Res, Suita, Osaka 5650871, Japan
[2] Kwansei Gakuin Univ, Fac Sci & Technol, Sanda 6691337, Japan
关键词
spin diffusion; distance analysis; photosynthesis; antenna complex; excitation transfer;
D O I
10.1073/pnas.0605911104
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
We have determined the atomic structure of the bacteriochlorophyll c (BChl c) assembly in a huge light-harvesting organelle, the chlorosome of green photosynthetic bacteria, by solid-state NMR. Previous electron microscopic and spectroscopic studies indicated that chlorosomes have a cylindrical architecture with a diameter of approximate to 10 nm consisting of layered BChl molecules. Assembly structures in huge noncrystalline chlorosomes have been proposed based mainly on structure-dependent chemical shifts and a few distances acquired by solid-state NMR, but those studies did not provide a definite structure. Our approach is based on C-13 dipolar spin-diffusion solid-state NMR of uniformly C-13-labeled chlorosomes under magic-angle spinning. Approximately 90 intermolecular C-C distances were obtained by simultaneous assignment of distance correlations and structure optimization preceded by polarization-transfer matrix analysis. it was determined from the approximate to 90 intermolecular distances that BChl c molecules form piggyback-dimer-based parallel layers. This finding rules out the well known monomer-based structures. A molecular model of the cylinder in the chlorosome was built by using this structure. It provided insights into the mechanisms of efficient light harvesting and excitation transfer to the reaction centers. This work constitutes an important advance in the structure determination of huge intact systems that cannot be crystallized.
引用
收藏
页码:790 / 795
页数:6
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