Multiexciton Dynamics Depending on Intramolecular Orientations in Pentacene Dimers: Recombination and Dissociation of Correlated Triplet Pairs

The Journal of Physical Chemistry Letters
Hayato SakaiTaku Hasobe

Abstract

Pentacene dimers bridged by a phenylene at ortho and meta positions [denoted as o-(Pc)2 and m-(Pc)2] were synthesized to examine intramolecular orientation-dependent multiexciton dynamics, especially focusing on singlet fission (SF) and recombination from correlated triplet pairs [(TT)]. Absorption and electrochemical measurements indicated strong intramolecular couplings of o-(Pc)2 relative to m-(Pc)2. Femtosecond and nanosecond TA measurements successfully demonstrated efficient SF in both dimers. In contrast, the dissociation process from the (TT) to the individual triplets [(2 × T)] was clearly observed in m-(Pc)2, which is in sharp contrast to a major recombination process in o-(Pc)2. Time-resolved electron spin resonance (TR-ESR) measurements demonstrated that the recombination and dissociation proceed from the quintet state of 5(TT) in m-(Pc)2. The rate constant of the SF was 2 orders of magnitude greater in o-(Pc)2 than that in m-(Pc)2 and was rationalized by enhanced electronic coupling between adjacent HOMOs of the Pc units.

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Citations

Nov 1, 2018·Chemistry, an Asian Journal·Akitsu HironoTaku Hasobe
Nov 30, 2018·Angewandte Chemie·Kiyonori KurodaMichito Yoshizawa
Oct 24, 2019·The Journal of Chemical Physics·Christopher GriecoJohn B Asbury
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Jun 17, 2021·Journal of the American Chemical Society·Lorenzo CattiMichito Yoshizawa
Nov 4, 2020·The Journal of Physical Chemistry. a·Kaia R ParentiLuis M Campos
Mar 13, 2019·Journal of Chemical Theory and Computation·Hung-Hsuan LinChao-Ping Hsu
Dec 19, 2020·The Journal of Physical Chemistry. B·Keisuke YoshinoTaku Hasobe
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Feb 1, 2022·Journal of the American Chemical Society·Robert M JacobbergerMichael R Wasielewski

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