Singlet-Fission-Born Quintet State: Sublevel Selections and Trapping by Multiexciton Thermodynamics

The Journal of Physical Chemistry Letters
Hiroki NagashimaYasuhiro Kobori

Abstract

Singlet fission (SF) is expected to exceed the theoretical limit of the solar cell efficiency. Quintet (Q) state generation in triplet-triplet pair is essential for preventing the unwanted loss of SF-born multiexciton through singlet channels, although little is known on the primary multiexciton spin dynamics following the intermolecular SF. In this study, time-resolved EPR revealed the intermolecular multiexciton dynamics, energetics and geometries in aggregated 6,13-bis(triisopropylsilylethynyl)pentacene and 2-phenyl-6,11-bis(triisopropylsilylethynyl)tetracene in diluted frozen solution. We have demonstrated sublevel selective generations of excited quintet states (|Q0⟩, |Q-1⟩ and |Q-2⟩) by singlet-quintet (SQ) mixings during triplet-exciton diffusions within geminate multiexcitons. The present fundamental characteristics of the quintet generations shows strong impact of coexistence of molecularly ordered "hot spot" and disordered regions for exergonic SQ mixings driven by entropy, thereby paving a new avenue for rational designs of organic devices with controlled multiexciton dynamics by optimizing film morphologies.

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Citations

Apr 6, 2019·Proceedings of the National Academy of Sciences of the United States of America·Michelle ChenMichael R Wasielewski
Nov 5, 2019·The Journal of Chemical Physics·Miles I CollinsMurad J Y Tayebjee
Jan 27, 2021·Chemical Society Reviews·Tobias UllrichDirk M Guldi
Oct 30, 2020·Scientific Reports·Kori E Smyser, Joel D Eaves
Feb 6, 2019·Chemical Reviews·Kiyoshi MiyataX-Y Zhu
Oct 12, 2019·Journal of the American Chemical Society·Antonios M AlvertisAndrew J Musser
Jun 23, 2020·The Journal of Physical Chemistry. a·Ilias PapadopoulosDirk M Guldi
Jul 10, 2019·The Journal of Physical Chemistry Letters·Yuri E KandrashkinJianzhang Zhao
Oct 30, 2020·The Journal of Physical Chemistry. B·Nikolaus WollscheidTiago Buckup
Sep 24, 2020·The Journal of Physical Chemistry. B·Nicolo AlagnaTiago Buckup

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