Diindolocarbazole – achieving multiresonant thermally activated delayed fluorescence without the need for acceptor units

David Hall; Kleitos Stavrou; Eimantas Duda; Andrew Danos; Sergey Bagnich; Stuart Warriner; Alexandra M. Z. Slawin; David Beljonne; Anna Köhler; Andrew Monkman; Yoann Olivier; Eli Zysman-Colman

doi:10.1039/d1mh01383a

Diindolocarbazole – achieving multiresonant thermally activated delayed fluorescence without the need for acceptor units

David Hall^*, Kleitos Stavrou, Eimantas Duda, Andrew Danos, Sergey Bagnich, Stuart Warriner, Alexandra M. Z. Slawin, David Beljonne, Anna Köhler^*, Andrew Monkman^*, Yoann Olivier^*, Eli Zysman-Colman^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

Abstract

In this work we present a new multi-resonance thermally activated delayed fluorescence (MR-TADF) emitter paradigm, demonstrating that the structure need not require the presence of acceptor atoms. Based on an in silico design, the compound DiICzMes₄ possesses a red-shifted emission, enhanced photoluminescence quantum yield, and smaller singlet-triplet energy gap, ΔE_ST, than the parent indolocarbazole that induces MR-TADF properties. Coupled cluster calculations accurately predict the magnitude of the ΔE_ST when the optimized singlet and triplet geometries are used. Slow yet optically detectable reverse intersystem crossing contributes to low efficiency in organic light-emitting diodes using DiICzMes₄ as the emitter. However, when used as a terminal emitter in combination with a TADF assistant dopant within a hyperfluorescence device architecture, maximum external quantum efficiencies of up to 16.5% were achieved at CIE (0.15, 0.11). This represents one of the bluest hyperfluorescent devices reported to date. Simultaneously, recognising that MR-TADF emitters do not require acceptor atoms reveals an unexplored frontier in materials design, where yet greater performance may yet be discovered.

Original language	English
Number of pages	13
Journal	Materials Horizons
Volume	Advance Article
Early online date	24 Jan 2022
DOIs	https://doi.org/10.1039/d1mh01383a
Publication status	E-pub ahead of print - 24 Jan 2022

Access to Document

10.1039/d1mh01383aLicence: CC BY

Hall_2022_MH_Diindolocarbazole_CC
Copyright © 2022 The Author(s). Open Access. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
Final published version, 4.86 MBLicence: CC BY

Eli Zysman-colman SRF: New Frontiers in Multi-Resonance Thermally Activated Delayed Fluorescence Emitter Design for Organic Light-Emitting Diodes
Zysman-Colman, E. (PI)
The Royal Society
18/01/21 → 18/03/22
Project: Fellowship
H2020 - ITN ELI ZYSMAN-COLMAN: H2020 MSCA ITN TADFlife
Zysman-Colman, E. (PI)
European Commission
1/10/18 → 30/09/22
Project: Standard
Blue-Emitting TADF Materials: Blue-Emitting TADF Materials for OLEDs Based on a Lewis Acid-Containing Acceptor
Zysman-Colman, E. (PI)
The Leverhulme Trust
1/08/16 → 30/04/22
Project: Standard

Diindolocarbazole – Achieving Multiresonant Thermally Activated Delayed Fluorescence Without The Need for Acceptor Units (dataset)
Hall, D. L. S. (Creator), Stavrou, K. (Creator), Duda, E. (Creator), Danos, A. (Creator), Bagnich, S. (Creator), Warriner, S. (Creator), Slawin, A. M. Z. (Creator), Beljonne, D. (Creator), Köhler, A. (Creator), Monkman, A. (Creator), Olivier, Y. (Creator) & Zysman-Colman, E. (Creator), University of St Andrews, 8 Feb 2022
DOI: 10.17630/915048c3-9d32-43ee-a18d-b49f95042a55
Dataset

File

Cite this

Hall, D., Stavrou, K., Duda, E., Danos, A., Bagnich, S., Warriner, S., Slawin, A. M. Z., Beljonne, D., Köhler, A., Monkman, A., Olivier, Y., & Zysman-Colman, E. (2022). Diindolocarbazole – achieving multiresonant thermally activated delayed fluorescence without the need for acceptor units. Materials Horizons, Advance Article. Advance online publication. https://doi.org/10.1039/d1mh01383a

@article{4a94b2af8fc24024ac08b73a47a911c7,

title = "Diindolocarbazole – achieving multiresonant thermally activated delayed fluorescence without the need for acceptor units",

abstract = "In this work we present a new multi-resonance thermally activated delayed fluorescence (MR-TADF) emitter paradigm, demonstrating that the structure need not require the presence of acceptor atoms. Based on an in silico design, the compound DiICzMes4 possesses a red-shifted emission, enhanced photoluminescence quantum yield, and smaller singlet-triplet energy gap, ΔEST, than the parent indolocarbazole that induces MR-TADF properties. Coupled cluster calculations accurately predict the magnitude of the ΔEST when the optimized singlet and triplet geometries are used. Slow yet optically detectable reverse intersystem crossing contributes to low efficiency in organic light-emitting diodes using DiICzMes4 as the emitter. However, when used as a terminal emitter in combination with a TADF assistant dopant within a hyperfluorescence device architecture, maximum external quantum efficiencies of up to 16.5% were achieved at CIE (0.15, 0.11). This represents one of the bluest hyperfluorescent devices reported to date. Simultaneously, recognising that MR-TADF emitters do not require acceptor atoms reveals an unexplored frontier in materials design, where yet greater performance may yet be discovered.",

author = "David Hall and Kleitos Stavrou and Eimantas Duda and Andrew Danos and Sergey Bagnich and Stuart Warriner and Slawin, {Alexandra M. Z.} and David Beljonne and Anna K{\"o}hler and Andrew Monkman and Yoann Olivier and Eli Zysman-Colman",

note = "The St Andrews team would like to thank the Leverhulme Trust (RPG-2016-047) for financial support. Computational resources have been provided by the Consortium des {\'E}quipements de Calcul Intensif (C{\'E}CI), funded by the Fonds de la Recherche Scientifiques de Belgique (F. R. S.-FNRS) under Grant No. 2.5020.11, as well as the Tier-1 supercomputer of the F{\'e}d{\'e}ration Wallonie-Bruxelles, infrastructure funded by the Walloon Region under the grant agreement n1117545. We acknowledge support from the European Union's Horizon 2020 research and innovation programme under the ITN TADFlife (GA 812872). Y.O. acknowledges funding by the Fonds de la Recherche Scientifique-FNRS under Grant no. F.4534.21 (MIS-IMAGINE). D. B. is a FNRS Research Director. EZ-C is a Royal Society Leverhulme Trust Senior Research fellow (SRF\R1\201089).",

year = "2022",

month = jan,

day = "24",

doi = "10.1039/d1mh01383a",

language = "English",

volume = "Advance Article",

journal = "Materials Horizons",

issn = "2051-6347",

publisher = "Royal Society of Chemistry",

}

TY - JOUR

T1 - Diindolocarbazole – achieving multiresonant thermally activated delayed fluorescence without the need for acceptor units

AU - Hall, David

AU - Stavrou, Kleitos

AU - Duda, Eimantas

AU - Danos, Andrew

AU - Bagnich, Sergey

AU - Warriner, Stuart

AU - Slawin, Alexandra M. Z.

AU - Beljonne, David

AU - Köhler, Anna

AU - Monkman, Andrew

AU - Olivier, Yoann

AU - Zysman-Colman, Eli

N1 - The St Andrews team would like to thank the Leverhulme Trust (RPG-2016-047) for financial support. Computational resources have been provided by the Consortium des Équipements de Calcul Intensif (CÉCI), funded by the Fonds de la Recherche Scientifiques de Belgique (F. R. S.-FNRS) under Grant No. 2.5020.11, as well as the Tier-1 supercomputer of the Fédération Wallonie-Bruxelles, infrastructure funded by the Walloon Region under the grant agreement n1117545. We acknowledge support from the European Union's Horizon 2020 research and innovation programme under the ITN TADFlife (GA 812872). Y.O. acknowledges funding by the Fonds de la Recherche Scientifique-FNRS under Grant no. F.4534.21 (MIS-IMAGINE). D. B. is a FNRS Research Director. EZ-C is a Royal Society Leverhulme Trust Senior Research fellow (SRF\R1\201089).

PY - 2022/1/24

Y1 - 2022/1/24

N2 - In this work we present a new multi-resonance thermally activated delayed fluorescence (MR-TADF) emitter paradigm, demonstrating that the structure need not require the presence of acceptor atoms. Based on an in silico design, the compound DiICzMes4 possesses a red-shifted emission, enhanced photoluminescence quantum yield, and smaller singlet-triplet energy gap, ΔEST, than the parent indolocarbazole that induces MR-TADF properties. Coupled cluster calculations accurately predict the magnitude of the ΔEST when the optimized singlet and triplet geometries are used. Slow yet optically detectable reverse intersystem crossing contributes to low efficiency in organic light-emitting diodes using DiICzMes4 as the emitter. However, when used as a terminal emitter in combination with a TADF assistant dopant within a hyperfluorescence device architecture, maximum external quantum efficiencies of up to 16.5% were achieved at CIE (0.15, 0.11). This represents one of the bluest hyperfluorescent devices reported to date. Simultaneously, recognising that MR-TADF emitters do not require acceptor atoms reveals an unexplored frontier in materials design, where yet greater performance may yet be discovered.

AB - In this work we present a new multi-resonance thermally activated delayed fluorescence (MR-TADF) emitter paradigm, demonstrating that the structure need not require the presence of acceptor atoms. Based on an in silico design, the compound DiICzMes4 possesses a red-shifted emission, enhanced photoluminescence quantum yield, and smaller singlet-triplet energy gap, ΔEST, than the parent indolocarbazole that induces MR-TADF properties. Coupled cluster calculations accurately predict the magnitude of the ΔEST when the optimized singlet and triplet geometries are used. Slow yet optically detectable reverse intersystem crossing contributes to low efficiency in organic light-emitting diodes using DiICzMes4 as the emitter. However, when used as a terminal emitter in combination with a TADF assistant dopant within a hyperfluorescence device architecture, maximum external quantum efficiencies of up to 16.5% were achieved at CIE (0.15, 0.11). This represents one of the bluest hyperfluorescent devices reported to date. Simultaneously, recognising that MR-TADF emitters do not require acceptor atoms reveals an unexplored frontier in materials design, where yet greater performance may yet be discovered.

U2 - 10.1039/d1mh01383a

DO - 10.1039/d1mh01383a

M3 - Article

SN - 2051-6347

VL - Advance Article

JO - Materials Horizons

JF - Materials Horizons

ER -

Diindolocarbazole – achieving multiresonant thermally activated delayed fluorescence without the need for acceptor units

Abstract

Access to Document

Fingerprint

Projects

Eli Zysman-colman SRF: New Frontiers in Multi-Resonance Thermally Activated Delayed Fluorescence Emitter Design for Organic Light-Emitting Diodes

H2020 - ITN ELI ZYSMAN-COLMAN: H2020 MSCA ITN TADFlife

Blue-Emitting TADF Materials: Blue-Emitting TADF Materials for OLEDs Based on a Lewis Acid-Containing Acceptor

Datasets

Diindolocarbazole – Achieving Multiresonant Thermally Activated Delayed Fluorescence Without The Need for Acceptor Units (dataset)

Cite this