Investigation of intramolecular through-space charge-transfer states in donor-acceptor charge-transfer systems
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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.
Kumar , S , Franca , L G , Stavrou , K , Crovini , E , Cordes , D B , Slawin , A M Z , Monkman , A P & Zysman-Colman , E 2021 , ' Investigation of intramolecular through-space charge-transfer states in donor-acceptor charge-transfer systems ' , Journal of Physical Chemistry Letters , vol. 12 , pp. 2820-2830 . https://doi.org/10.1021/acs.jpclett.1c00265
Journal of Physical Chemistry Letters
Copyright © 2021 The Authors. Published by American Chemical Society. ACS Author Choice. Open Access, licensed under a CC BY Attribution licence (https://creativecommons.org/licenses/by/4.0/).
DescriptionFunding: We thank EU horizon 2020 Grant Agreement No. 812872 (TADFlife) for funding. SK acknowledges the financial support from European Union’s Horizon 2020 research and innovation programme under Marie Skłodowska Curie Individual Fellowship (MCIF; Agreement No. 748430- THF-OLED).
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