Chain-Length-Dependent Exciton Dynamics in Linear Oligothiophenes Probed Using Ensemble and Single-Molecule Spectroscopy

The Journal of Physical Chemistry Letters
Tae-Woo KimDongho Kim

Abstract

Exciton dynamics in π-conjugated molecular systems is highly susceptible to conformational disorder. Using time-resolved and single-molecule spectroscopic techniques, the effect of chain length on the exciton dynamics in a series of linear oligothiophenes, for which the conformational disorder increased with increasing chain length, was investigated. As a result, extraordinary features of the exciton dynamics in longer-chain oligothiophene were revealed. Ultrafast fluorescence depolarization processes were observed due to exciton self-trapping in longer and bent chains. Increase in exciton delocalization during dynamic planarization processes was also observed in the linear oligothiophenes via time-resolved fluorescence spectra but was restricted in L-10T because of its considerable conformational disorder. Exciton delocalization was also unexpectedly observed in a bent chain using single-molecule fluorescence spectroscopy. Such delocalization modulates the fluorescence spectral shape by attenuating the 0-0 peak intensity. Collectively, these results provide significant insights into the exciton dynamics in conjugated polymers.

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Citations

Mar 30, 2017·The Journal of Physical Chemistry Letters·Lena Simine, Peter J Rossky
Dec 10, 2016·The Journal of Physical Chemistry Letters·Laura Alfonso HernandezSebastian Fernandez-Alberti
Oct 31, 2020·Chemistry of Materials : a Publication of the American Chemical Society·Lisa PeterhansSophia C Hayes

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