Excited-State Dynamic Planarization of Cyclic Oligothiophenes in the Vicinity of a Ring-to-Linear Excitonic Behavioral Turning Point

Angewandte Chemie
Kyu Hyung ParkDongho Kim

Abstract

Excited-state dynamic planarization processes play a crucial role in determining exciton size in cyclic systems, as reported for π-conjugated linear oligomers. Herein, we report time-resolved fluorescence spectra and molecular dynamics simulations of π-conjugated cyclic oligothiophenes in which the number of subunits was chosen to show the size-dependent dynamic planarization in the vicinity of a ring-to-linear behavioral turning point. Analyses on the evolution of the total fluorescence intensity and the ratio between 0-1 to 0-0 vibronic bands suggest that excitons formed in a cyclic oligothiophene composed of six subunits fully delocalize over the cyclic carbon backbone, whereas those formed in larger systems fail to achieve complete delocalization. With the aid of molecular dynamics simulations, it is shown that distorted structures unfavorable for efficient exciton delocalization are more easily populated as the size of the cyclic system increases.

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Citations

Jul 14, 2016·Inorganic Chemistry·Mitsuhiko MorisueJoji Ohshita
Oct 27, 2015·The Journal of Physical Chemistry Letters·Woojae KimDongho Kim
Aug 6, 2016·Physical Chemistry Chemical Physics : PCCP·Taeyeon KimDongho Kim
Jul 7, 2020·Physical Chemistry Chemical Physics : PCCP·B Rodríguez-HernándezS Fernandez-Alberti
Sep 10, 2020·Macromolecular Rapid Communications·Huijie WangWenke Zhang
May 12, 2016·Chemistry : a European Journal·Nagaraju BarsuBasker Sundararaju
Mar 8, 2019·Nature Communications·Bowen ShenMyongsoo Lee
Mar 28, 2020·The Journal of Physical Chemistry Letters·JunWoo KimMinhaeng Cho
Jul 10, 2019·The Journal of Physical Chemistry Letters·Sang Hyeon LeeDongho Kim

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