Connecting rare DNA conformations and surface dynamics using single-molecule resonance energy transfer.
Connecting rare DNA conformations and surface dynamics using single-molecule resonance energy transfer.
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DOI：
10.1021/nn2035389
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发表时间：
2011-12-27
期刊：
影响因子：
17.1
通讯作者：
Schwartz DK
中科院分区：
文献类型：
--
作者：
Kastantin M;Schwartz DK
从机理上理解单链DNA(SsDNA)在近表面环境中的行为对于发展DNA定向自组装纳米材料是至关重要的。描述了一种利用全内反射荧光显微镜在单分子水平上测量共振能量转移的新方法，提供了对胺修饰表面附近分子构象和界面动力学之间的联系的机理的理解。观察到大量的单链DNA轨迹(>；105)，允许分子构象与脱附和表面迁移率的动态关联。在动态行为的基础上，分子可以被指定为更常见的盘绕群体的成员，或者是罕见的弱结合构象。卷曲状态的分子通常表现出缓慢的扩散和构象波动，随着平均端到端距离的增加而减小。吸附自回避聚合物的晶格模拟成功地预测了这些趋势。相反，在约5%的分子中观察到的弱结合构象具有较大的端到端距离，但显示的构象波动远高于吸附柔性链的模拟预测。这种构象与解吸事件正相关，并导致快速扩散，表明表面缔合较弱。了解弱结合构象在DNA杂交中的作用，以及溶液条件和表面性质如何有利于它，可能会导致改进的自组装纳米材料。
A mechanistic understanding of single-stranded DNA (ssDNA) behavior in the near-surface environment is critical to advancing DNA-directed self-assembled nanomaterials. A new approach is described that uses total internal reflection fluorescence microscopy to measure resonance energy transfer at the single-molecule level, providing a mechanistic understanding of the connection between molecular conformation and interfacial dynamics near amine-modified surfaces. Large numbers (>105) of ssDNA trajectories were observed, permitting dynamic correlation of molecular conformation with desorption and surface mobility. On the basis of dynamic behavior, molecules could be designated as members of the more common coiled population or a rare, weakly bound conformation. Molecules in the coiled state generally exhibited slow diffusion and conformational fluctuations that decreased with increasing average end-to-end distance. Lattice simulations of adsorbed self-avoiding polymers successfully predicted these trends. In contrast, the weakly bound conformation, observed in about 5% of molecules, had a large end-to-end distance but demonstrated conformational fluctuations that were much higher than predicted by simulations for adsorbed flexible chains. This conformation correlated positively with desorption events and led to fast diffusion, indicating weak surface associations. Understanding the role of the weakly bound conformation in DNA hybridization, and how solution conditions and surface properties may favor it, could lead to improved self-assembled nanomaterials.
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影响因子：
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