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Effect of Core Oligomer Length on the Phase Behavior and Assembly of pi-Conjugated Peptides

机译：核心低聚物长度对PI缀合肽相行为和组装的影响

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摘要

Biohybrid molecules are a versatile class of materials for controlling the assembly behavior and functional properties of electronically active organics. In this work, we study the effect of the size of the pi-conjugated core on the assembly and phase behavior for a series of pi-conjugated peptides consisting of oligothiophene cores of defined lengths flanked by sequence-defined peptides (OTX, where X = 4, 5, 6 is the number of thiophene core units). Interestingly, we find that pi-conjugated peptides with relatively short OT4 cores assemble into ordered, high aspect ratio, one-dimensional (1D) structures, whereas pi-conjugated peptides with longer OT5 and OT6 cores assemble into disordered structures or lower aspect ratio 1D structures depending on assembly conditions. Phase diagrams for assembled materials are experimentally determined as a function of ionic strength, pH, temperature, and peptide concentration, revealing the impact of molecular sequence and pi-conjugated core length on assembled morphologies. Molecular dynamics (MD) simulations are further used to probe the origins of microscale differences in assembly that arise from subtle changes in molecular identity. Broadly, our work elucidates the mechanisms governing the assembly of pi-conjugated peptides, which will aid in efficient materials processing for soft electronic applications. Overall, these results highlight the complex phase behavior of biohybrid materials, including the impact of molecular sequence on assembly behavior and morphology.
机译：生物冬小分子是一种多功能的材料，用于控制电子活性有机物的组装行为和功能性。在这项工作中，我们研究了由序列定义的肽（OTX，其中x =的一系列Pi-缀合的肽组成的组装和相行为对组装和相行为的效果。 4,5,6是噻吩核心单元的数量）。有趣的是，我们发现具有相对短的OT4芯的PI-缀合的肽组装成有序，高纵横比，一维（1D）结构，而具有较长的OT5和OT6芯的PI-缀合的肽组装成无序结构或更低的纵横比1D结构根据组装条件。组装材料的相图是由离子强度，pH，温度和肽浓度的函数确定的，揭示了分子序列和Pi缀合的芯长对组装形态的影响。分子动力学（MD）模拟进一步用于探测来自微妙变化的组装中的微观差异的起源。广泛地，我们的工作阐明了治疗PI缀合肽大会的机制，这将有助于为软电子应用提供有效的材料加工。总体而言，这些结果突出了生物冬小材料的复杂相行为，包括分子序列对组装行为和形态的影响。

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