Abstract
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.
Highlights
Energy migration between the identical chromophores is a necessary process in both natural and artificial photosynthesis
Anthraquinone absorption has almost no overlap with perylene emission (Fig. 1b) so that hetero energy transfer from perylene to anthraquinone, which disturbs the quantitative analyses of energy migration, does not occur
A Dthreoninol linker was used to introduce these chromophore as it facilitates intercalation of these molecules into DNA duplex[36]
Summary
Energy migration between the identical chromophores is a necessary process in both natural and artificial photosynthesis. We 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. DNA has been widely used as a platform to prepare chromophoric arrays[7,8,9,10,11], and recently, photonic arrays and circuits based on DNA nano-structures have been reported[12,13,14,15] In these structures, EM and hetero FRET play crucial roles in efficient energy harvesting and transport[16,17,18,19,20,21,22,23,24,25,26]. This is the first study to experimentally reveal the distance and orientation dependence of energy migration among identical dyes
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