Ultralarge Modulation of Fluorescence by Neuromodulators in Carbon Nanotubes Functionalized with Self-Assembled Oligonucleotide Rings.
Ultralarge Modulation of Fluorescence by Neuromodulators in Carbon Nanotubes Functionalized with Self-Assembled Oligonucleotide Rings.
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DOI：
10.1021/acs.nanolett.8b02937
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发表时间：
2018-11-14
期刊：
影响因子：
10.8
通讯作者：
Landry MP
中科院分区：
文献类型：
--
作者：
Beyene AG;Alizadehmojarad AA;Dorlhiac G;Goh N;Streets AM;Král P;Vuković L;Landry MP
单链DNA（ssDNA）寡核苷酸和单壁碳纳米管（SWNT）之间的非共价相互作用为各种应用提供了一类独特的可调化学。然而，缺乏对它们的实用性背后的生物物理和分子间现象的机械洞察，导致产生基于ssDNA-SWNT的技术的专性启发式方法。在这项工作中，我们提出了一种用于神经调节剂多巴胺和去甲肾上腺素的超灵敏“开启”纳米传感器，其荧光强度的相对变化（ΔF/F0）高达3500%，这是一种适用于体内神经成像的信号，揭示了由（GT）的自发自组装合成的纳米传感器的分子识别和荧光调制的物理机制和分子间相互作用单壁碳纳米管上有6个单链DNA环。的ssDNA-SWNT共轭物的荧光调制显示出显着的敏感性ssDNA序列的化学，长度和表面密度，提供了一组参数，其中调整纳米传感器的动态范围和强度的荧光turn-on. We采用经典和量子力学分子动力学模拟合理化我们的实验结果。计算表明，（GT）6 ssDNA形成有序的环周围的单壁碳纳米管，诱导周期性的表面电位，调制激子复合寿命。进一步的证据来阐明多巴胺分析物结合如何调节单壁碳纳米管荧光。我们讨论了我们的研究结果的影响，单壁碳纳米管为基础的分子成像应用。
Non-covalent interactions between single-stranded DNA (ssDNA) oligonucleotides and single wall carbon nanotubes (SWNTs) have provided a unique class of tunable chemistries for a variety of applications. However, mechanistic insight into both the photophysical and intermolecular phenomena underlying their utility is lacking, resulting in obligate heuristic approaches for producing ssDNA-SWNT based technologies. In this work, we present an ultrasensitive “turn-on” nanosensor for neuromodulators dopamine and norepinephrine with strong relative change in fluorescence intensity (ΔF/F0) of up to 3500%, a signal appropriate for in vivo neuroimaging, and uncover the photophysical principles and intermolecular interactions that govern the molecular recognition and fluorescence modulation of this nanosensor synthesized from the spontaneous self-assembly of (GT)6 ssDNA rings on SWNTs. The fluorescence modulation of the ssDNA-SWNT conjugate is shown to exhibit remarkable sensitivity to the ssDNA sequence chemistry, length, and surface density, providing a set of parameters with which to tune nanosensor dynamic range and strength of fluorescence turn-on. We employ classical and quantum mechanical molecular dynamics simulations to rationalize our experimental findings. Calculations show that (GT)6 ssDNA form ordered rings around SWNT, inducing periodic surface potentials that modulate exciton recombination lifetimes. Further evidence is presented to elucidate how dopamine analyte binding modulates SWNT fluorescence. We discuss the implications of our findings for SWNT-based molecular imaging applications.
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