Li Xinmeng, Buda Francesco, de Groot Huub J M, Sevink G J Agur
Leiden Institute of Chemistry, Leiden University, Einsteinweg 55, 2300 RA Leiden, South Holland, the Netherlands.
Department of Chemistry and Hylleraas Centre for Quantum Molecular Sciences, P.O.Box 1033, Blindern, Oslo, 0315 Oslo, Norway.
iScience. 2021 Dec 11;25(1):103618. doi: 10.1016/j.isci.2021.103618. eCollection 2022 Jan 21.
The most efficient light-harvesting antennae found in nature, chlorosomes, are molecular tubular aggregates (TMAs) assembled by pigments without protein scaffolds. Here, we discuss a classification of chlorosomes as a unique tubular plastic crystal and we attribute the robust energy transfer in chlorosomes to this unique nature. To systematically study the role of supramolecular tube chirality by molecular simulation, a role that has remained unresolved, we share a protocol for generating realistic tubes at atomic resolution. We find that both the optical and the mechanical behavior are strongly dependent on chirality. The optical-chirality relation enables a direct interpretation of experimental spectra in terms of overall tube chirality. The mechanical response shows that the overall chirality regulates the hardness of the tube and provides a new characteristic for relating chlorosomes to distinct chirality. Our protocol also applies to other TMA systems and will inspire other systematic studies beyond lattice models.
自然界中发现的最有效的光捕获天线——叶绿体，是由没有蛋白质支架的色素组装而成的分子管状聚集体（TMA）。在此，我们讨论将叶绿体分类为独特的管状塑性晶体，并将叶绿体中强大的能量转移归因于这种独特性质。为了通过分子模拟系统地研究超分子管手性的作用（这一作用尚未得到解决），我们分享了一种在原子分辨率下生成逼真管子的方案。我们发现光学和机械行为都强烈依赖于手性。光学 - 手性关系能够根据整体管手性直接解释实验光谱。机械响应表明整体手性调节管的硬度，并为将叶绿体与不同手性联系起来提供了一个新特性。我们的方案也适用于其他TMA系统，并将激发超越晶格模型的其他系统研究。
