Quantitative evaluation of energy migration between identical chromophores enabled by breaking symmetry

Hiromu Kashida; Hayato Kawai; Ryoko Maruyama; Yuta Kokubo; Yasuyuki Araki; Takehiko Wada; Hiroyuki Asanuma

doi:10.1038/s42004-018-0093-0

Quantitative evaluation of energy migration between identical chromophores enabled by breaking symmetry

Hiromu Kashida, Hayato Kawai, Ryoko Maruyama, Yuta Kokubo, Yasuyuki Araki, Takehiko Wada, Hiroyuki Asanuma

IMRAM - Division of Organic- and Biomaterials Research

Nagoya University

Research output: Contribution to journal › Article › peer-review

15 Citations (Scopus)

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.

Original language	English
Article number	91
Journal	Communications Chemistry
Volume	1
Issue number	1
DOIs	https://doi.org/10.1038/s42004-018-0093-0
Publication status	Published - 2018 Dec 1

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title = "Quantitative evaluation of energy migration between identical chromophores enabled by breaking symmetry",

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 F{\"o}rster 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.",

author = "Hiromu Kashida and Hayato Kawai and Ryoko Maruyama and Yuta Kokubo and Yasuyuki Araki and Takehiko Wada and Hiroyuki Asanuma",

note = "Funding Information: This work was supported by JSPS KAKENHI grant numbers JP18H03933 (H.A.), JP16H05925 (H.K.), JP17H05150 (H.K.) and JP16H04127 (Y.A.), and by PRESTO grant number JPMJPR14F7 (H.K.) and A-STEP (H.A.) from Japan Science and Technology Agency. Supports from the JSPS A3 Fore-sight Programme and the Asahi Glass Foundation (H.A.) are also acknowledged. Publisher Copyright: {\textcopyright} 2018, The Author(s).",

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AU - Kashida, Hiromu

AU - Kawai, Hayato

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AU - Kokubo, Yuta

AU - Araki, Yasuyuki

AU - Wada, Takehiko

AU - Asanuma, Hiroyuki

N1 - Funding Information: This work was supported by JSPS KAKENHI grant numbers JP18H03933 (H.A.), JP16H05925 (H.K.), JP17H05150 (H.K.) and JP16H04127 (Y.A.), and by PRESTO grant number JPMJPR14F7 (H.K.) and A-STEP (H.A.) from Japan Science and Technology Agency. Supports from the JSPS A3 Fore-sight Programme and the Asahi Glass Foundation (H.A.) are also acknowledged. Publisher Copyright: © 2018, The Author(s).

PY - 2018/12/1

Y1 - 2018/12/1

N2 - 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.

AB - 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.

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Quantitative evaluation of energy migration between identical chromophores enabled by breaking symmetry

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