The Rule of Thirds: Controlling Junction Chirality and Polarity in 3D DNA Tiles

The Rule of Thirds: Controlling Junction Chirality and Polarity in 3D DNA Tiles
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三分法:控制 3D DNA 块中的连接手性和极性

DOI:
10.1002/smll.202206511
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发表时间:
2022
期刊:
影响因子:
13.3
通讯作者:
Sha, Ruojie
Sha, Ruojie
中科院分区:
材料科学1区
文献类型:
--
作者:
Vecchioni, Simon;Lu, Brandon;Janowski, Jordan;Woloszyn, Karol;Jonoska, Nataša;Seeman, Nadrian C.;Mao, Chengde;Ohayon, Yoel P.;Sha, Ruojie

文献摘要

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张拉整体三角形DNA晶体的成功自组装预示着从合理设计的纳米级组件可编程地构建宏观结晶纳米材料的能力。这种3D DNA瓦片的“张力整体性”性质归因于其三个旋转堆叠的双螺旋通过中心链的拉伸缠绕锁定在一起,该中心链被分成7个碱基对(bp)的交叉区域,对应于DNA螺旋圈的三分之二。到目前为止,所有报告的张拉整体三角形都采用了(Z+2/3)\[\left({Z{\bm{ + }}2{\bf /}3} \right)\]转弯的交叉段,产生了右旋、反平行的“J1”连接。这里报道了一个由3 bp连接间片段或三分之一螺旋转角组成的最小DNA三角形基序。结果发现,最小的基序表现出一个反向的形态与左手的三级结构介导的局部平行霍利迪连接的“L1”连接。这种平行的交界处产生一个预测的螺旋槽匹配模式,打破瓷砖面之间的伪对称,和交界处的形态进一步表明折叠机制。三分之一规则,其中超分子手性可以通过连接DNA片段长度进行编程。这些结果强调了全局拓扑力在确定局部DNA结构中的作用,并最终指出了一类未被探索的自组装手性纳米材料,用于生物系统中的拓扑过程。
The successful self‐assembly of tensegrity triangle DNA crystals heralded the ability to programmably construct macroscopic crystalline nanomaterials from rationally‐designed, nanoscale components. This 3D DNA tile owes its “tensegrity” nature to its three rotationally stacked double helices locked together by the tensile winding of a center strand segmented into 7 base pair (bp) inter‐junction regions, corresponding to two‐thirds of a helical turn of DNA. All reported tensegrity triangles to date have employed (Z+2/3)\[\left( {Z{\bm{ + }}2{\bf /}3} \right)\] turn inter‐junction segments, yielding right‐handed, antiparallel, “J1” junctions. Here a minimal DNA triangle motif consisting of 3‐bp inter‐junction segments, or one‐third of a helical turn is reported. It is found that the minimal motif exhibits a reversed morphology with a left‐handed tertiary structure mediated by a locally‐parallel Holliday junction—the “L1” junction. This parallel junction yields a predicted helical groove matching pattern that breaks the pseudosymmetry between tile faces, and the junction morphology further suggests a folding mechanism. A Rule of Thirds by which supramolecular chirality can be programmed through inter‐junction DNA segment length is identified. These results underscore the role that global topological forces play in determining local DNA architecture and ultimately point to an under‐explored class of self‐assembling, chiral nanomaterials for topological processes in biological systems.