Quantitative evaluation of energy migration between identical chromophores enabled by breaking symmetry
Quantitative evaluation of energy migration between identical chromophores enabled by breaking symmetry
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DOI：
10.1038/s42004-018-0093-0
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发表时间：
2018-12
影响因子：
5.9
通讯作者：
H. Kashida;Hayato Kawai;Ryoko Maruyama;Yuta Kokubo;Y. Araki;T. Wada;H. Asanuma
中科院分区：
文献类型：
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作者：
H. Kashida;Hayato Kawai;Ryoko Maruyama;Yuta Kokubo;Y. Araki;T. Wada;H. Asanuma
相同发色团之间的能量迁移是自然光合作用和人工光合作用的一个必要过程。能量迁移的距离和取向依赖性还没有详细的实验研究。在这里，我们提出了一种方法来研究能量迁移。将两个荧光团引入DNA双链体的一条链中，猝灭剂与荧光团之一相对放置。这种设计能够使相同的荧光团不对称，并允许一个荧光团作为受体。发射强度和寿命的降低取决于能量迁移的效率。距离和取向的依赖性被成功地量化，测量的激发能迁移效率与Förster理论计算的结果非常一致。我们还证明了四个荧光团之间的多步能量迁移可以从理论上估计。这些结果为设计和制备高效的光捕获光子器件和化学探针提供了依据。
Energy migration between the identical chromophores is a necessary process in both natural and artificial photosynthesis. The distance and orientation dependence of energy migration have not been experimentally investigated in detail. Here we propose a method to investigate energy migration. Two fluorophores are introduced into one strand of a DNA duplex with a quencher placed opposite one of fluorophores. This design enables asymmetrization of identical fluorophores and allows one fluorophore to behave as an acceptor. The emission intensities and lifetimes decrease depending on the efficiency of energy migration. Distance and orientation dependence are successfully quantified, and the excitation energy migration efficiencies measured are in excellent agreement with those calculated based on Förster theory. We also demonstrate that multi-step energy migration among four fluorophores can be estimated from the theory. These results may provide a basis for design and preparation of efficient light-harvesting photonic devices and chemical probes.