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Upconverting Nanoparticle Relays for Resonance Energy Transfer Networks

机译：用于共振能量传输网络的上转换纳米粒子继电器

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摘要

Networks of fluorophores arranged at the nanoscale can perform basic computation using resonance energy transfer (RET) to transport and manipulate information in the form of excitons. As excitons travel through RET circuits, they are red-shifted due to vibrational energy loss at each transfer event. This loss prohibits RET circuits from being cascaded to form larger, more computationally complex systems. To address this issue, a nanoassembly capable of converting three or more low energy excitons into a single high energy exciton is designed and fabricated. Deemed the RET relay, this device uses upconverting nanoparticles to achieve anti-Stokes energy transfer from near-infrared excited fluorophores to visibly excited fluorophores. In this work, the relay is explored by first breaking it into its halves. Each fluorophore's ability to donate energy to or from the nanoparticle is characterized by a series of photoluminescence experiments. The adsorption of these fluorophores to the particle is modeled as a Langmuir process, revealing the fractional occupancy of each dye that optimizes energy transfer. A fully functional relay is then demonstrated by exciting the near-infrared dye and extracting the visible dye's fluorescence. Lastly, the performance of the entire construct is optimized over a small sampling of assembly reaction coordinates.
机译：布置在纳米级的荧光团网络可以使用共振能量转移（RET）进行基本计算，以激子形式传输和操纵信息。当激子穿过RET回路时，由于每次传递事件时的振动能量损失，它们会发生红移。这种损耗会阻止RET电路级联形成更大，计算更复杂的系统。为了解决这个问题，设计并制造了能够将三个或更多个低能激子转换为单个高能激子的纳米组件。该设备被认为是RET继电器，它使用上转换纳米粒子来实现反斯托克斯能量从近红外激发荧光团到可见激发荧光团的转移。在这项工作中，首先将继电器分成两半进行探索。每个荧光团向纳米粒子或从纳米粒子供能的能力通过一系列的光致发光实验来表征。这些荧光团在颗粒上的吸附被模拟为Langmuir过程，揭示了每种染料的分数占有率，从而优化了能量转移。然后，通过激发近红外染料并提取可见染料的荧光来演示全功能继电器。最后，通过少量的组装反应坐标采样，可以优化整个构建体的性能。

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  • 来源
    《Advanced Functional Materials》 |2016年第17期|2866-2874|共9页
  • 作者

    LaBoda Craig D.; Dwyer Chris L.;

  • 作者单位

    Duke Univ, Dept Elect & Comp Engn, Durham, NC 27708 USA;

    Duke Univ, Dept Elect & Comp Engn, Durham, NC 27708 USA;

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