DNA hairpin stabilization on a hydrophobic surface.

DNA hairpin stabilization on a hydrophobic surface.
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DOI:
10.1002/smll.201202335
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发表时间:
2013-03-25
期刊:
影响因子:
13.3
通讯作者:
Schwartz, Daniel K.
Schwartz, Daniel K.
中科院分区:
材料科学1区
文献类型:
--
作者:
Kastantin, Mark;Schwartz, Daniel K.

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表面附近的DNA杂交是自组装纳米阵列、超晶格和生物传感器的基本过程。人们普遍认为,固体表面改变相对于本体溶液的分子力,这些影响可以有利于或不利于杂交状态,这取决于特定的序列和表面。本文提供的结果为亲水性低聚乙二醇(OEG)和疏水性三甲基硅烷(TMS)表面附近的DNA发夹卷曲构象转变动力学提供了新的见解。单分子方法被用来观察吸附物种的正向和反向杂交发夹线圈过渡,同时测量分子表面扩散,以深入了解表面与单个DNA碱基的相互作用。在每种类型的表面上至少观察到35,000个单独的分子轨迹。我们发现,尽管TMS和未配对的核碱基之间有更强的吸引力,但相对于OEG,TMS的展开速度减慢,折叠速率增加。这些速率差异导致在疏水TMS上几乎完全形成发夹,在亲水OEG上显著展开,从而得出令人惊讶的结论,即疏水表面涂层对于依赖于表面附近的DNA杂交的纳米技术应用是优选的。
DNA hybridization in the vicinity of surfaces is a fundamental process for self-assembled nanoarrays, nanocrystal superlattices, and biosensors. It is widely recognized that solid surfaces alter molecular forces governing hybridization relative to bulk solution, and these effects can either favor or disfavor the hybridized state depending on the specific sequence and surface. Results presented here provide new insights into the dynamics of DNA hairpin-coil conformational transitions in the vicinity of hydrophilic oligo(ethylene glycol) (OEG) and hydrophobic trimethylsilane (TMS) surfaces. Single-molecule methods are used to observe the forward and reverse hybridization hairpin-coil transition of adsorbed species while simultaneously measuring molecular surface diffusion in order to gain insight into surface interactions with individual DNA bases. At least 35,000 individual molecular trajectories are observed on each type of surface. We find that unfolding slows and the folding rate increases on TMS relative to OEG despite stronger attractions between TMS and unpaired nucleobases. These rate differences lead to nearly complete hairpin formation on hydrophobic TMS and significant unfolding on hydrophilic OEG, resulting in the surprising conclusion that hydrophobic surface coatings are preferable for nanotechnology applications that rely on DNA hybridization near surfaces.
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