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Photophysics of J-Aggregate-Mediated Energy Transfer on DNA
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2017-11-16 00:00:00 , DOI: 10.1021/acs.jpclett.7b01898
James L. Banal 1 , Toru Kondo 1 , Rémi Veneziano 1 , Mark Bathe 1 , Gabriela S. Schlau-Cohen 1
Affiliation  

Achieving nanoscale spatial and electronic control over the formation of dye aggregates is a major synthetic challenge due to their typically inhomogeneous self-assembly, which limits control over their higher-order organization. To address these challenges, synthetic DNA-templated pseudoisocyanine (PIC) J-aggregates were recently introduced. However, the dependence of the photophysics of the superradiant exciton on the underlying DNA template length and the impact of static disorder on energy transfer through these PIC J-aggregates remain unknown. We examine the delocalization length progression of superradiant PIC excitons by varying the length of poly-A DNA tracts that template PIC J-aggregates. We then investigate the energy-transfer efficiency from PIC J-aggregates with DNA duplex template length, which we found to be limited by static disorder. Utilizing the self-assembled and selective formation of superradiant excitons on DNA provides a platform to determine the function of delocalized excitons in the context of nanoscale energy transport.

中文翻译:

J聚集体介导的DNA能量转移的光物理

由于它们通常不均一的自组装,实现对染料聚集体形成的纳米级空间和电子控制是一项主要的合成挑战,这限制了对其高阶结构的控制。为了解决这些挑战,最近引入了合成的以DNA为模板的伪异氰酸(PIC)J聚集体。然而,超辐射激子的光物理对下层DNA模板长度的依赖性以及通过这些PIC J聚集体对能量转移的静态紊乱的影响仍然未知。我们通过改变模板PIC J聚集体的poly-A DNA片段的长度来检查超辐射PIC激子的离域长度进展。然后,我们研究具有DNA双链模板长度的PIC J聚集体的能量转移效率,我们发现它受到静电障碍的限制。利用DNA上超辐射激子的自组装和选择性形成提供了一个平台,可在纳米级能量传输的背景下确定离域激子的功能。
更新日期:2017-11-16
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