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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >The supramolecular organization of self-assembling chlorosomal bacteriochlorophyll c, d, or e mimics
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The supramolecular organization of self-assembling chlorosomal bacteriochlorophyll c, d, or e mimics

机译：自组装绿体细菌叶绿素c，d或e的超分子组织

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摘要

Bacteriochlorophylls (BChls) c, d, and e are the main light-harvesting pigments of green photosynthetic bacteria that self-assemble into nanostructures within the chlorosomes forming the most efficient antennas of photosynthetic organisms. All previous models of the chlorosomal antennae, which are quite controversially discussed because no single crystals could be grown so far from these or-ganelles, involve a strong hydrogen-bonding interaction between the 3~1 hydroxyl group and the 13~1 carbonyl group. We have synthesized different self-assemblies of BChl c mimics having the same functional groups as the natural counterparts, that is, a hydroxyethyl substitu-ent, a carbonyl group and a divalent metal atom ligated by a tetrapyrrole. These artificial BChl mimics have been shown by single crystal x-ray diffraction to form extended stacks that are packed by hydrophobic interactions and in the absence of hydrogen bonding. Time-resolved photoluminescence proves the ordered nature of the self-assembled stacks. FT-IR spectra show that on self-assembly the carbonyl frequency is shifted by ≈30 cm~(-1) to lower wavenumbers. From the FT-IR data we can infer the proximal interactions between the BChls in the chlorosomes consistent with a single crystal x-ray structure that shows a weak electrostatic interaction between carbonyl groups and the central zinc atom.
机译：细菌叶绿素（BChls）c，d和e是绿色光合细菌的主要集光色素，它们在叶绿体内自组装成纳米结构，形成光合生物的最有效天线。以前所有的绿体触角模型都引起了很大争议，因为到目前为止，离这些有机碳纳米管还无法生长出单晶，它们涉及3〜1羟基和13〜1羰基之间强烈的氢键相互作用。我们合成了具有与天然对应物相同的官能团的BChl c模拟物的不同自组装体，即具有四吡咯连接的羟乙基取代基，羰基和二价金属原子。这些人造的BChl模拟物已经通过单晶X射线衍射显示出形成延伸的堆叠，这些堆叠通过疏水相互作用和在没有氢键的情况下堆积。时间分辨的光致发光证明了自组装堆叠的有序性质。 FT-IR光谱表明，自组装时羰基频率偏移≈30cm〜（-1）至较低的波数。根据FT-IR数据，我们可以推断出氯仿中BChl之间的近端相互作用，与单晶X射线结构一致，该结构显示出羰基与中心锌原子之间的弱静电相互作用。

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