肽共轭苝二亚胺自组装的计算引导调谐,Langmuir

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肽共轭苝二亚胺自组装的计算引导调谐
Langmuir ( IF 3.7 ) Pub Date : 2021-07-02 , DOI: 10.1021/acs.langmuir.1c01213
Sayak Subhra Panda ₁ , Kirill Shmilovich ₂ , Nicholas S M Herringer ₂ , Nicolas Marin ₁ , Andrew L Ferguson ₂ , John D Tovar _{1,

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Affiliation

肽-π-共轭材料由于它们的水相容性和长程π-电子网络的形成，对于生物界面电荷传输应用很重要。苝二酰亚胺 (PDI) 是一种成熟的电荷传输 π 系统，当与氨基酸结合时，可以在水溶液中自组装。在这项工作中，我们利用之前工作的计算指导来访问来自 PDI-氨基酸缀合物的两种不同的自组装架构。此外，我们将设计规则扩展到其他序列，以了解最接近 π 核心的氨基酸对所得组件的光物理特性有显着影响。通过在最接近的残基位置简单地将甘氨酸改变为丙氨酸，我们观察到了显着不同的电子特性，如通过 UV-vis、光致发光、和圆二色光谱。伴随的分子动力学模拟揭示了两种不同类型的自组装结构：当较小的甘氨酸残基位于最接近 π 核的残基位置时的共面结构与当甘氨酸被较大的丙氨酸取代时旋转移位的结构。这项研究说明了使用串联计算和实验来发掘和理解超分子材料的新设计规则，并揭示了适度的氨基酸取代作为可预测地调节超分子组织和设计 π 共轭肽材料的光物理特性的一种手段。当较小的甘氨酸残基位于最接近 π 核的残基位置时的共面结构与当甘氨酸取代较大的丙氨酸时旋转移位的结构。这项研究说明了使用串联计算和实验来发掘和理解超分子材料的新设计规则，并揭示了适度的氨基酸取代作为可预测地调节超分子组织和设计 π 共轭肽材料的光物理特性的一种手段。当较小的甘氨酸残基位于最接近 π 核的残基位置时的共面结构与当甘氨酸取代较大的丙氨酸时旋转移位的结构。这项研究说明了使用串联计算和实验来发掘和理解超分子材料的新设计规则，并揭示了适度的氨基酸取代作为可预测地调节超分子组织和设计 π 共轭肽材料的光物理特性的一种手段。

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Computationally Guided Tuning of Peptide-Conjugated Perylene Diimide Self-Assembly

Peptide−π-conjugated materials are important for biointerfacing charge-transporting applications due to their aqueous compatibility and formation of long-range π-electron networks. Perylene diimides (PDIs), well-established charge-transporting π systems, can self-assemble in aqueous solutions when conjugated with amino acids. In this work, we leveraged computational guidance from our previous work to access two different self-assembled architectures from PDI–amino acid conjugates. Furthermore, we expanded the design rule to other sequences to learn that the closest amino acids to the π core have a significant effect on the photophysical properties of the resulting assemblies. By simply altering glycine to alanine at the closest residue position, we observed significantly different electronic properties as revealed through UV–vis, photoluminescence, and circular dichroism spectroscopies. Accompanying molecular dynamics simulations revealed two distinct types of self-assembled architectures: cofacial structures when the smaller glycine residue is at the closest residue position to the π core versus rotationally shifted structures when glycine is substituted for the larger alanine. This study illustrates the use of tandem computations and experiments to unearth and understand new design rules for supramolecular materials and exposes a modest amino acid substitution as a means to predictably modulate the supramolecular organization and engineer the photophysical properties of π-conjugated peptidic materials.

更新日期：2021-07-20

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