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Comparative Dynamics and Sequence Dependence of DNA and RNA Bindingto Single Walled Carbon Nanotubes

机译:DNA和RNA结合的比较动力学和序列依赖性到单壁碳纳米管

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摘要

Noncovalent polymer-single walled carbon nanotube (SWCNT) conjugates have gained recent interest due to their prevalent use as electrochemical and optical sensors, SWCNT-based therapeutics, and for SWCNT separation. However, little is known about the effects of polymer-SWCNT molecular interactions on functional properties of these conjugates. In this work, we show that SWCNT complexed with related polynucleotide polymers (DNA, RNA) have dramatically different fluorescence stability. Surprisingly, we find a difference of nearly 2500-fold in fluorescence emission between the most fluorescently stable DNA-SWCNT complex, C30 DNA-SWCNT, compared to the least fluorescently stable complex, (AT)7A-(GU)7G DNA-RNA hybrid-SWCNT. We further reveal the existence of three regimes in which SWCNT fluorescence varies nonmonotonically with SWCNT concentration. We utilize molecular dynamics simulations to elucidate the conformation and atomic details of SWCNT-corona phase interactions. Our results show that variations in polynucleotide sequence or sugar backbone can lead to large changes in the conformational stability of the polymer SWCNT corona and the SWCNT optical response. Finally, we demonstrate the effect of the coronae on the response of a recently developed dopaminenanosensor, based on (GT)15 DNA- and (GU)15 RNA-SWCNTcomplexes. Our results clarify several features of the sequence dependence ofcorona phases produced by polynucleotides adsorbed to single walled carbonnanotubes, and the implications for molecular recognition in such phases.
机译:非共价聚合物-单壁碳纳米管(SWCNT)共轭物因其广泛用作电化学和光学传感器,基于SWCNT的治疗剂以及用于SWCNT分离而获得了新的关注。但是,关于聚合物-SWCNT分子相互作用对这些结合物的功能性质的影响知之甚少。在这项工作中,我们表明与相关的多核苷酸聚合物(DNA,RNA)复合的SWCNT具有显着不同的荧光稳定性。出乎意料的是,我们发现,与荧光稳定性最低的(AT)7A-(GU)7G DNA-RNA杂种相比,荧光最稳定的DNA-SWCNT复合物C30 DNA-SWCNT之间的荧光发射差异近2500倍-SWCNT。我们进一步揭示了存在三种模式,其中SWCNT荧光随SWCNT浓度非单调变化。我们利用分子动力学模拟来阐明SWCNT-电晕相相互作用的构象和原子细节。我们的结果表明,多核苷酸序列或糖主链中的变异可导致聚合物SWCNT电晕的构象稳定性和SWCNT光学响应发生较大变化。最后,我们证明了日冕对最近开发的多巴胺反应的影响纳米传感器,基于(GT)15 DNA和(GU)15 RNA-SWCNT复合体。我们的结果阐明了序列依赖性的几个特征多核苷酸吸附到单壁碳上产生的电晕相纳米管及其在此类阶段对分子识别的意义。

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