Department of Chemistry, Ludwig-Maximilians-Universität München, Butenandtstr. 5-13, München, Germany.
Center for NanoScience, Ludwig-Maximilians-Universität München, Schellingstraße 4, München, Germany.
Nat Commun. 2024 Sep 10;15(1):7894. doi: 10.1038/s41467-024-51721-y.
Allostery is a hallmark of cellular function and important in every biological system. Still, we are only starting to mimic it in the laboratory. Here, we introduce an approach to study aspects of allostery in artificial systems. We use a DNA origami domino array structure which-upon binding of trigger DNA strands-undergoes a stepwise allosteric conformational change. Using two FRET probes placed at specific positions in the DNA origami, we zoom in into single steps of this reaction cascade. Most of the steps are strongly coupled temporally and occur simultaneously. Introduction of activation energy barriers between different intermediate states alters this coupling and induces a time delay. We then apply these approaches to release a cargo DNA strand at a predefined step in the reaction cascade to demonstrate the applicability of this concept in tunable cascades of mechanochemical coupling with both spatial and temporal control.
变构作用是细胞功能的标志，在每个生物系统中都很重要。尽管如此，我们才刚刚开始在实验室中对其进行模拟。在这里，我们介绍了一种在人工系统中研究变构作用的方法。我们使用 DNA 折纸多米诺骨牌阵列结构，该结构在结合触发 DNA 链后会经历逐步的变构构象变化。通过在 DNA 折纸的特定位置放置两个 FRET 探针，我们可以详细研究该反应级联中的单个步骤。大多数步骤在时间上紧密耦合并且同时发生。在不同中间状态之间引入激活能垒会改变这种耦合并导致时间延迟。然后，我们将这些方法应用于在反应级联的预定步骤中释放货物 DNA 链，以证明该概念在具有空间和时间控制的机械化学耦联的可调谐级联中的适用性。
