Investigation of intramolecular through-space charge-transfer states in donor-acceptor charge-transfer systems

Shiv Kumar, Larissa Gomes Franca, Kleitos Stavrou, Ettore Crovini, David Bradford Cordes, Alexandra Martha Zoya Slawin, Andrew P. Monkman, Eli Zysman-Colman

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Abstract

Commonly, thermally activated delayed fluorescence (TADF) emitters present a twisted donor–acceptor structure. Here, electronic communication is mediated through-bond via π-conjugation between donor and acceptor groups. A second class of TADF emitters are those where electronic communication between donor and acceptor moieties is mediated through-space. In these through-space charge-transfer (TSCT) architectures, the donor and acceptor groups are disposed in a pseudocofacial orientation and linked via a bridging group that is typically an arene (or heteroarene). In most of these systems, there is no direct evidence that the TSCT is the dominant contributor to the communication between the donor and acceptor. Herein we investigate the interplay between through-bond localized excited (LE) and charge-transfer (CT) states and the TSCT in a rationally designed emitter, TPA-ace-TRZ, and a family of model compounds. From our photophysical studies, TSCT TADF in TPA-ace-TRZ is unambiguously confirmed and supported by theoretical modeling.
Original languageEnglish
Pages (from-to)2820-2830
Number of pages11
JournalJournal of Physical Chemistry Letters
Volume12
Early online date15 Mar 2021
DOIs
Publication statusE-pub ahead of print - 15 Mar 2021

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