Tuning Optical Absorption and Emission Using Strongly Coupled Dimers in Programmable DNA Scaffolds
Tuning Optical Absorption and Emission Using Strongly Coupled Dimers in Programmable DNA Scaffolds
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DOI：
10.1021/acs.jpclett.1c03848
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发表时间：
2022-02-24
影响因子：
5.7
通讯作者：
Schlau-Cohen, Gabriela S.
中科院分区：
文献类型：
--
作者：
Hart, Stephanie M.;Wang, Xiao;Schlau-Cohen, Gabriela S.
用于光捕获、计算和荧光成像的分子材料需要电子活性亚基的纳米级集成。亚基光学吸收和发射特性的变化主要是通过化学结构的修改来实现的，这在合成上通常具有挑战性。在这里，我们介绍了一种通过改变双交叉 (DX) DNA 平铺上强耦合 Cy3 二聚体的几何形状来改变光学吸收和发射特性的简便方法。利用DNA的多功能性和可编程性，我们调整互补链的长度，使其“推”或“拉”二聚体，从而引起光物理学的巨大变化，包括在整体和单分子水平上观察到的寿命差异。可分离的寿命以及光物理学中观察到的环境敏感性表明 Cy3-DX 瓦片结构可以用作多重成像的荧光探针。更一般地说，这些结构通过耦合发色团的几何变化建立了一个易于控制的光物理学框架，可应用于光捕获装置和分子电子学。
Molecular materials for light harvesting, computing, and fluorescence imaging require nanoscale integration of electronically active subunits. Variation in the optical absorption and emission properties of the subunits has primarily been achieved through modifications to the chemical structure, which is often synthetically challenging. Here, we introduce a facile method for varying optical absorption and emission properties by changing the geometry of a strongly coupled Cy3 dimer on a double-crossover (DX) DNA tile. Leveraging the versatility and programmability of DNA, we tune the length of the complementary strand so that it "pushes" or "pulls" the dimer, inducing dramatic changes in the photophysics including lifetime differences observable at the ensemble and single-molecule level. The separable lifetimes, along with environmental sensitivity also observed in the photophysics, suggest that the Cy3-DX tile constructs could serve as fluorescence probes for multiplexed imaging. More generally, these constructs establish a framework for easily controllable photophysics via geometric changes to coupled chromophores, which could be applied in light-harvesting devices and molecular electronics.