Engineering couplings for exciton transport using synthetic DNA scaffolds
Engineering couplings for exciton transport using synthetic DNA scaffolds
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DOI：
10.1016/j.chempr.2020.12.020
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发表时间：
2021-03-11
期刊：
影响因子：
23.5
通讯作者：
Schlau-Cohen, Gabriela S.
中科院分区：
文献类型：
--
作者：
Hart, Stephanie M.;Chen, Wei Jia;Schlau-Cohen, Gabriela S.
对激子的控制使得电子能量能够被利用和传输用于光捕获和分子电子学。这种控制需要对分子组分进行纳米级的精确度。自然光捕获系统通过复杂的蛋白质机制实现了这种精度，这对合成复制具有挑战性。在这里，我们介绍了一个基于DNA的平台，空间组织花青生色团构建可调激子系统。我们合成了DNA-发色团纳米结构，并用系综超快和单分子光谱学以及基于结构的建模对其进行了表征。这种合成方法促进了对发色团之间以及发色团与环境之间的偶联的独立控制。我们证明了发色团和环境之间的耦合可以提高激子输运效率，突出了环境在驱动激子动力学中的关键作用。控制激子，如这里所报道的，提供了一条通往设计师纳米光子器件发展的道路。
Control over excitons enables electronic energy to be harnessed and transported for light harvesting and molecular electronics. Such control requires nanoscale precision over the molecular components. Natural light-harvesting systems achieve this precision through sophisticated protein machinery, which is challenging to replicate synthetically. Here, we introduce a DNA-based platform that spatially organizes cyanine chromophores to construct tunable excitonic systems. We synthesized DNA-chromophore nanostructures and characterized them with ensemble ultrafast and single-molecule spectroscopy and structure-based modeling. This synthetic approach facilitated independent control over the coupling among the chromophores and between the chromophores and the environment. We demonstrated that the coupling between the chromophores and the environment could enhance exciton transport efficiency, highlighting the key role of the environment in driving exciton dynamics. Control over excitons, as reported here, offers a path toward the development of designer nanophotonic devices.