Utilizing homogenous FRET to extend molecular photonic wires beyond 30 nm (Presentation Recording)

S. A. Díaz, Susan Buckhout‐White, M. Ancona, J. Melinger, Igor L. Medintz
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Abstract

Molecular photonic wires (MPWs) present interesting applications in energy harvesting, artificial photosynthesis, and nano-circuitry. MPWs allow the directed movement of energy at the nanoscopic level. Extending the length of the energy transfer with a minimal loss in efficiency would overcome an important hurdle in allowing MPWs to reach their potential. We investigated Homogenous Förster Resonance Energy Transfer (HomoFRET) as a means to achieve this goal. We designed a simple, self-assembled DNA nanostructure with specifically placed dyes (Alexa488-Cy3-Cy3.5-Alexa647-Cy5.5) at a distance of 3.4 nm, a separation at which energy transfer should theoretically be very high. The input of the wire was at 466 nm with an output up to 697 nm. Different structures were studied where the Cy3.5 section of the MPW was extended from one to six repeats. We found that though the efficiency cost is not null, HomoFRET can be extended up to six repeat dyes with only a 22% efficiency loss when compared to a single step system. The advantage is that these six repeats created a MPW which was 17 nm longer, almost 2.5 times the initial length. To confirm the existence of HomoFRET between the Cy3.5 repeats fluorescence lifetime and fluorescence lifetime anisotropy was measured. Under these conditions we are able to demonstrate the energy transfer over a distance of 30.4 nm, with an end-to-end efficiency of 2.0%, by utilizing a system with only five unique dyes.
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利用同质FRET将分子光子线延伸至30 nm以上(演示记录)
分子光子线(mpw)在能量收集、人工光合作用和纳米电路等方面有着有趣的应用。mpw允许能量在纳米级的定向运动。在效率损失最小的情况下延长能量传递的长度,将克服使mpw发挥其潜力的一个重要障碍。我们研究了均匀Förster共振能量转移(HomoFRET)作为实现这一目标的手段。我们设计了一个简单的、自组装的DNA纳米结构,将染料(Alexa488-Cy3-Cy3.5-Alexa647-Cy5.5)放置在3.4 nm的距离上,理论上能量转移应该非常高。导线的输入波长为466 nm,输出波长为697 nm。将MPW的Cy3.5片段从1个重复延长到6个重复,研究了不同的结构。我们发现,虽然效率成本不是零,但HomoFRET可以扩展到六个重复染料,与单步系统相比,效率损失仅为22%。优点是这六次重复产生的MPW长度增加了17纳米,几乎是初始长度的2.5倍。为了证实HomoFRET的存在,测量了Cy3.5重复序列的荧光寿命和荧光寿命的各向异性。在这些条件下,我们能够展示在30.4 nm的距离上的能量转移,端到端效率为2.0%,通过使用只有五种独特染料的系统。
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