Comparative Dynamics and Sequence Dependence of DNA and RNA Binding to Single Walled Carbon Nanotubes.

Comparative Dynamics and Sequence Dependence of DNA and RNA Binding to Single Walled Carbon Nanotubes.
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DOI:
10.1021/jp511448e
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发表时间:
2015-05-07
期刊:
The journal of physical chemistry. C, Nanomaterials and interfaces
影响因子:
--
通讯作者:
Strano MS
Strano MS
中科院分区:
其他
文献类型:
--
作者:
Landry MP;Vuković L;Kruss S;Bisker G;Landry AM;Islam S;Jain R;Schulten K;Strano MS

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非共价聚合物-单壁碳纳米管(SWCNT)缀合物由于其普遍用作电化学和光学传感器、基于SWCNT的治疗剂以及用于SWCNT分离而获得最近的兴趣。然而,很少有人知道这些共轭物的功能特性的聚合物-单壁碳纳米管分子相互作用的影响。在这项工作中,我们表明,与相关的多核苷酸聚合物(DNA,RNA)复合的单壁碳纳米管具有显着不同的荧光稳定性。令人惊讶的是,我们发现,与最不荧光稳定的复合物(AT)7A-(GU)7 G DNA-RNA hybrid-SWCNT相比,最荧光稳定的DNA-SWCNT复合物C30 DNA-SWCNT的荧光发射相差近2500倍。我们进一步揭示了三个制度的存在,其中单壁碳纳米管荧光随单壁碳纳米管浓度的非单调变化。我们利用分子动力学模拟来阐明单壁碳纳米管-冠相相互作用的构象和原子细节。我们的研究结果表明,在多核苷酸序列或糖骨架的变化可以导致大的变化的构象稳定性的聚合物单壁碳纳米管冠和单壁碳纳米管的光学响应。最后,我们证明了冠状动脉对最近开发的多巴胺纳米传感器的响应的影响,基于(GT)15 DNA和(GU)15 RNA-SWCNT复合物。我们的研究结果澄清了多核苷酸吸附到单壁碳纳米管产生的电晕相的序列依赖性的几个特征,以及在这些阶段的分子识别的影响。
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 dopamine nanosensor, based on (GT)15 DNA- and (GU)15 RNA-SWCNT complexes. Our results clarify several features of the sequence dependence of corona phases produced by polynucleotides adsorbed to single walled carbon nanotubes, and the implications for molecular recognition in such phases.
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