NDLI: Single-Molecule Fluorescence Spectroscopy of Perylene Diimide Dyes in a Î³-Cyclodextrin Film: Manifestation of Photoinduced H-Atom Transfer via Higher Triplet (n, π*) Excited States.

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Single-Molecule Fluorescence Spectroscopy of Perylene Diimide Dyes in a Î³-Cyclodextrin Film: Manifestation of Photoinduced H-Atom Transfer via Higher Triplet (n, π*) Excited States.

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Mitsui, Masaaki Fukui, Hiroki Mizukami, Toshinari Takahashi, Ryoya Takakura, Yasushi
Description	Author Affiliation: Mitsui M ( Department of Chemistry, College of Science, Rikkyo University , 3-34-1, Nishiikebukuro, Toshima-ku, Tokyo 171-8501, Japan.); Fukui H ( Department of Chemistry, Faculty of Science, Shizuoka University , 836 Ohya, Suruga-ku, Shizuoka 422-8529, Japan.); Takahashi R ( Department of Chemistry, Faculty of Science, Shizuoka University , 836 Ohya, Suruga-ku, Shizuoka 422-8529, Japan.); Takakura Y ( Department of Chemistry, College of Science, Rikkyo University , 3-34-1, Nishiikebukuro, Toshima-ku, Tokyo 171-8501, Japan.); Mizukami T ( Department of Chemistry, College of Science, Rikkyo University , 3-34-1, Nishiikebukuro, Toshima-ku, Tokyo 171-8501, Japan.)
Abstract	Supramolecular complexation of Î³-cyclodextrin (Î³-CD) with N,N'-bis(2,6-dimethylphenyl)perylene-3,4,9,10-tetracarboxylic diimide (DMP-PDI) or N,N'-bis(2,6-dioctyl)perylene-3,4,9,10-tetracarboxylic diimide (C8-PDI) dye in an aqueous solution and in a Î³-CD solid film were investigated via ensemble and single-molecule fluorescence spectroscopy. These two perylene diimide derivatives possess almost the same electronic structure but have different terminal functional groups. This structural difference leads to formation of an inclusion complex of Î³-CD with DMP-PDI but not with C8-PDI in aqueous solution. In a Î³-CD solid film, the distributions of the wavelengths of emission maximum (λ ) are strikingly different between these two dyes; a much narrower and blue-shifted λ distribution was observed for C8-PDI relative to DMP-PDI. This difference is attributed to the fact that the C8-PDI molecules are bound at the Î³-CD/glass interface as a result of spin-coating of the sample solution, whereas the DMP-PDI molecules form 1:1 and 1:2 inclusion complexes with conformational heterogeneities in the film. In comparison to the case for C8-PDI, more frequent on-off blinking events were observed for DMP-PDI. The blinking statistics of DMP-PDI in the Î³-CD film exhibit both single-exponential and nonexponential (i.e., dispersive) kinetics, revealed by robust statistical analysis. Energetic consideration with the aid of theoretical calculations suggests that the underlying photophysics most probably involves hydrogen atom transfer (HAT) between the DMP-PDI guest and Î³-CD host via higher excited (n, π*) triplet states. The hypothesis of HAT in the inclusion complex reasonably explains the experimental results; however, a charge transfer hypothesis cannot explain the results. The dispersive kinetics is attributable to the effect of thermal fluctuation in the forward and backward HAT reactions.
ISSN	10895639
Issue Number	8
Journal	The Journal of Physical Chemistry A
Volume Number	121
e-ISSN	15205215
Language	English
Publisher	American Chemical Society (United States)
Publisher Date	2017-03-02
Publisher Place	United States
Access Restriction	One Nation One Subscription (ONOS)
Subject Keyword	Physical chemistry
Content Type	Text
Resource Type	Article
Subject	Medicine Physical and Theoretical Chemistry

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Single-Molecule Fluorescence Spectroscopy of Perylene Diimide Dyes in a Î³-Cyclodextrin Film: Manifestation of Photoinduced H-Atom Transfer via Higher Triplet (n, π*) Excited States.

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