Structural and Spectroscopic Properties of Assemblies of Self-Replicating Peptide Macrocycles.
Structural and Spectroscopic Properties of Assemblies of Self-Replicating Peptide Macrocycles.
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DOI：
10.1021/acsnano.7b02211
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发表时间：
2017-08-22
期刊：
影响因子：
17.1
通讯作者：
Marrink SJ
中科院分区：
文献类型：
--
作者：
Frederix PWJM;Idé J;Altay Y;Schaeffer G;Surin M;Beljonne D;Bondarenko AS;Jansen TLC;Otto S;Marrink SJ
分子水平上的自我复制通常被认为是生命早期起源的必要条件。最近发现了一种自我复制机制，其中复制子自组装驱动了这一过程。我们已经研究了这种自组装自我复制分子的一个例子，以高水平的结构细节，使用计算和光谱技术的组合。自组装肽衍生复制子堆叠的分子动力学模拟提供了对系统结构特征的见解，并为反映堆叠的手性组织和肽二级结构的紫外-可见、圆二色（CD）和红外（IR）吸收光谱的半经验计算提供了基础。通过将计算光谱与电子显微镜、CD和IR光谱的实验数据进行比较，对两种提出的结构模型进行了测试，从而更好地了解了导致自我复制的特定超分子相互作用。具体来说，我们发现了一种协同自组装过程，其中β-片的形成导致了组织良好的结构，同时大环的芳香核在所得到的纤维的稳定性中起着重要作用。
Self-replication at the molecular level is often seen as essential to the early origins of life. Recently a mechanism of self-replication has been discovered in which replicator self-assembly drives the process. We have studied one of the examples of such self-assembling self-replicating molecules to a high level of structural detail using a combination of computational and spectroscopic techniques. Molecular Dynamics simulations of self-assembled stacks of peptide-derived replicators provide insights into the structural characteristics of the system and serve as the basis for semiempirical calculations of the UV–vis, circular dichroism (CD) and infrared (IR) absorption spectra that reflect the chiral organization and peptide secondary structure of the stacks. Two proposed structural models are tested by comparing calculated spectra to experimental data from electron microscopy, CD and IR spectroscopy, resulting in a better insight into the specific supramolecular interactions that lead to self-replication. Specifically, we find a cooperative self-assembly process in which β-sheet formation leads to well-organized structures, while also the aromatic core of the macrocycles plays an important role in the stability of the resulting fibers.
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