DNA-Carbon Nanotube Complexation Affinity and Photoluminescence Modulation Are Independent.
DNA-Carbon Nanotube Complexation Affinity and Photoluminescence Modulation Are Independent.
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DOI：
10.1021/acsami.7b05678
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发表时间：
2017-06-28
影响因子：
9.5
通讯作者：
Roxbury D
中科院分区：
文献类型：
--
作者：
Jena PV;Safaee MM;Heller DA;Roxbury D
短单链DNA （ssDNA）已成为非共价功能化光致发光单壁碳纳米管的天然聚合物选择。此外，特定的经验鉴定DNA序列可用于分离具有极高纯度的单种（手性）纳米管。目前，只有有限的一般原则存在于设计DNA-纳米管杂合体适合分离过程，部分原因是对DNA序列和特定纳米管结构之间的基本相互作用的理解不完全，而在设计具有确定光学性质的纳米管传感器方面所知的更少。因此，我们开发了一个基于时间分辨近红外荧光光谱的联合实验和分析平台，以提取表征dna -纳米管杂交体的完整光致发光参数。在这里，我们系统地研究了d(GT)n寡核苷酸家族对结构定义的碳纳米管的亲和力，通过测量碳纳米管在寡核苷酸位移时的光致发光响应。我们发现，令人惊讶的是，寡核苷酸的位移率与纳米管上的覆盖无关，这是通过杂化物的固有光学性质推断出来的。强度调制的动力学本质上是单指数，而时间常数，量化DNA结合的稳定性，跨越一个数量级。令人惊讶的是，这些时间常数并不依赖于杂交体内部的固有光学参数，这表明DNA-纳米管的稳定性不是由于DNA对纳米管表面覆盖的增加。此外，对激发和发射位移的主成分分析，以及平衡时强度的增强，准确地确定了（8,6）纳米管是（GT）6 ssDNA的手性伴侣。结合手性分辨平衡和动力学数据，可以指导具有可调稳定性和光学调制的dna -纳米管对的开发。此外，这种高通量光学平台可以作为绘制dna手性识别相空间的主屏幕。
Short single-stranded DNA (ssDNA) has emerged as the natural polymer of choice for non-covalently functionalizing photoluminescent single-walled carbon nanotubes. In addition, specific empirically identified DNA sequences can be used to separate single species (chiralities) of nanotubes with exceptionally high purity. Currently, only limited general principles exist for designing DNA-nanotube hybrids amenable to separation processes, due in part to an incomplete understanding of the fundamental interactions between a DNA sequence and a specific nanotube structure, while even less is known in the design of nanotube-based sensors with determined optical properties. We therefore developed a combined experimental and analysis platform, based on time-resolved near-infrared fluorescence spectroscopy, to extract the complete set of photoluminescence parameters that characterize DNA-nanotube hybrids. Here, we systematically investigated the affinity of the d(GT)n oligonucleotide family for structurally-defined carbon nanotubes by measuring photoluminescence response of the nanotube upon oligonucleotide displacement. We found, surprisingly, that the rate of displacement of oligonucleotides is independent of the coverage on the nanotube, as inferred through intrinsic optical properties of the hybrid. The kinetics of intensity modulation are essentially single exponentials, and the time constants, which quantify the stability of DNA binding, span an order of magnitude. Surprisingly, these time constants do not depend on the intrinsic optical parameters within the hybrids, suggesting that DNA-nanotube stability is not due to increased nanotube surface coverage by DNA. Further, a principal component analysis of the excitation and emission shifts, along with intensity enhancement at equilibrium accurately identified the (8,6) nanotube as the partner chirality to (GT)6 ssDNA. Combined, the chirality-resolved equilibrium and kinetics data can guide the development of DNA-nanotube pairs with tunable stability and optical modulation. Additionally, this high-throughput optical platform could function as a primary screen for mapping the DNA-chirality recognition phase space.
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影响因子：
4.6
作者：
Roxbury D;Jena PV;Williams RM;Enyedi B;Niethammer P;Marcet S;Verhaegen M;Blais-Ouellette S;Heller DA
通讯作者：
Heller DA
影响因子：
56.9
作者：
O'Connell, MJ;Bachilo, SM;Smalley, RE
通讯作者：
Smalley, RE
影响因子：
3.9
作者：
Shankar, Akshaya;Mittal, Jeetain;Jagota, Anand
通讯作者：
Jagota, Anand
影响因子：
--
作者：
Prasek, Jan;Drbohlavova, Jana;Kizek, Rene
通讯作者：
Kizek, Rene
影响因子：
64.8
作者：
Tu, Xiaomin;Manohar, Suresh;Zheng, Ming
通讯作者：
Zheng, Ming