Understanding Förster Resonance Energy Transfer in the Sheet Regime with DNA Brick-Based Dye Networks.
Understanding Förster Resonance Energy Transfer in the Sheet Regime with DNA Brick-Based Dye Networks.
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DOI：
10.1021/acsnano.1c05871
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发表时间：
2021-10-26
期刊：
影响因子：
17.1
通讯作者：
Medintz IL
中科院分区：
文献类型：
--
作者：
Mathur D;Samanta A;Ancona MG;Díaz SA;Kim Y;Melinger JS;Goldman ER;Sadowski JP;Ong LL;Yin P;Medintz IL
在分子水平上控制激子能量转移是将纳米光子学研究转变为可行设备的关键要求，其主要灵感来自生物光捕获天线，该天线使用Förster共振能量转移（FRET）以接近统一的效率收集和引导光能。在假定的FRET过程中，点到平面FRET之间的供体和受体排列在二维片被预测是特别有效的理论1/r4能量转移距离（r）的依赖性与1/r6的依赖性看到一个单一的供体-受体相互作用。然而，定量验证已经混淆了缺乏强大的实验方法，可以严格地将染料在所需的纳米级安排。为了创建这样的组件，我们利用DNA砖支架，称为DNA块，其包含多达5个二维平面，每个平面显示5种不同供体、受体或中间中继染料的1至12个拷贝。将纳米结构表征沿着稳态和时间分辨光谱数据与分子动力学建模和详细的数值模拟相结合，以将实验DNA块组件中观察到的能量转移效率与理论预期进行比较。总的来说，我们展示了明确的签名的片制度FRET，并从这一点，我们提供了一个更好的理解是什么需要实现这样的能量转移的好处，在人工染料网络沿着与FRET为基础的传感和成像。
Controlling excitonic energy transfer at the molecular level is a key requirement for transitioning nanophotonics research to viable devices with the main inspiration coming from biological light-harvesting antennas that collect and direct light energy with near-unity efficiency using Förster resonance energy transfer (FRET). Among putative FRET processes, point-to-plane FRET between donors and acceptors arrayed in two-dimensional sheets is predicted to be particularly efficient with a theoretical 1/r4 energy transfer distance (r) dependency versus the 1/r6 dependency seen for a single donor–acceptor interaction. However, quantitative validation has been confounded by a lack of robust experimental approaches that can rigidly place dyes in the required nanoscale arrangements. To create such assemblies, we utilize a DNA brick scaffold, referred to as a DNA block, which incorporates up to five two-dimensional planes with each displaying from 1 to 12 copies of five different donor, acceptor, or intermediary relay dyes. Nanostructure characterization along with steady-state and time-resolved spectroscopic data were combined with molecular dynamics modeling and detailed numerical simulations to compare the energy transfer efficiencies observed in the experimental DNA block assemblies to theoretical expectations. Overall, we demonstrate clear signatures of sheet regime FRET, and from this we provide a better understanding of what is needed to realize the benefits of such energy transfer in artificial dye networks along with FRET-based sensing and imaging.
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