Elucidation of an aggregate excited state in the electrochemiluminescence and chemiluminescence of a thermally activated delayed fluorescence (TADF) emitter

Kenneth Chu; Jonathan R Adsetts; Zackry Whitworth; Shiv Kumar; Eli Zysman-Colman; Zhifeng Ding

doi:10.1021/acs.langmuir.2c03391

Elucidation of an aggregate excited state in the electrochemiluminescence and chemiluminescence of a thermally activated delayed fluorescence (TADF) emitter

Kenneth Chu, Jonathan R Adsetts, Zackry Whitworth, Shiv Kumar, Eli Zysman-Colman^*, Zhifeng Ding^*

^*Corresponding author for this work

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

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Abstract

The electrochemistry, electrochemiluminescence (ECL), and chemiluminescence (CL) properties of a thermally activated delayed fluorescence (TADF) emitter 4,4′-(1,2-dihydroacenaphthylene-5,6-diyl)bis(N,N-diphenylaniline) (TPA-ace-TRZ) and three of its analogues were investigated. TPA-ace-TRZ exhibits both (a) delayed onset of ECL and (b) long-persistent luminescence, which we have attributed to the formation of an aggregate excited state in excimer or exciplex form. The evidence of this aggregate excited state was consistent across ECL annihilation and coreactant pathways as well as in CL. The absolute ECL efficiency of TPA-ace-TRZ using benzoyl peroxide (BPO) as a coreactant was found to be 0.028%, which was 9-fold stronger than the [Ru(bpy)₃]²⁺/BPO reference coereactant system. Furthermore, the absolute CL quantum efficiency of TPA-ace-TRZ was determined to be 0.92%. The performance and flexibility of the TADF emitter TPA-ace-TRZ under these various emissive pathways are highly desirable toward applications in sensing, imaging, and light-emitting devices.

Original language	English
Pages (from-to)	2829-2837
Number of pages	9
Journal	Langmuir
Volume	39
Issue number	7
Early online date	10 Feb 2023
DOIs	https://doi.org/10.1021/acs.langmuir.2c03391
Publication status	Published - 21 Feb 2023

Keywords

Cyclic voltammogram
ECL - voltage curve
Differential pulse
ECL accumulation
Voltammograms
TPA-ace
TPA-ace-CN
2TPA-ace

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10.1021/acs.langmuir.2c03391Licence: CC BY

Chu_2023_Langmuir_Elucidation_CC
Copyright © 2023 American Chemical Society. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
Final published version, 3.85 MBLicence: CC BY

THF-OLED: H2020 MSCA Fellowship 2016 THF-OLED
Zysman-Colman, E. (PI)
European Commission
1/05/17 → 31/10/19
Project: Fellowship

Cite this

@article{48a667e1b5674e9d89c15d314c0c2435,

title = "Elucidation of an aggregate excited state in the electrochemiluminescence and chemiluminescence of a thermally activated delayed fluorescence (TADF) emitter",

abstract = "The electrochemistry, electrochemiluminescence (ECL), and chemiluminescence (CL) properties of a thermally activated delayed fluorescence (TADF) emitter 4,4′-(1,2-dihydroacenaphthylene-5,6-diyl)bis(N,N-diphenylaniline) (TPA-ace-TRZ) and three of its analogues were investigated. TPA-ace-TRZ exhibits both (a) delayed onset of ECL and (b) long-persistent luminescence, which we have attributed to the formation of an aggregate excited state in excimer or exciplex form. The evidence of this aggregate excited state was consistent across ECL annihilation and coreactant pathways as well as in CL. The absolute ECL efficiency of TPA-ace-TRZ using benzoyl peroxide (BPO) as a coreactant was found to be 0.028%, which was 9-fold stronger than the [Ru(bpy)3]2+/BPO reference coereactant system. Furthermore, the absolute CL quantum efficiency of TPA-ace-TRZ was determined to be 0.92%. The performance and flexibility of the TADF emitter TPA-ace-TRZ under these various emissive pathways are highly desirable toward applications in sensing, imaging, and light-emitting devices.",

keywords = "Cyclic voltammogram, ECL - voltage curve, Differential pulse, ECL accumulation, Voltammograms, TPA-ace, TPA-ace-CN, 2TPA-ace",

author = "Kenneth Chu and Adsetts, {Jonathan R} and Zackry Whitworth and Shiv Kumar and Eli Zysman-Colman and Zhifeng Ding",

note = "Funding: Natural Sciences and Engineering Research Council Canada (NSERC, DG RGPIN-2018-06556 and SPG STPGP2016-493924), Canada Foundation of Innovation/Ontario Innovation Trust (CFI/OIT, 9040), and The University of Western Ontario. The authors acknowledge financial support from the European Union{\textquoteright}s Horizon 2020 research and innovation program under a Marie Sk{\l}odowska Curie Individual Fellowship to S.K. (MCIF; agreement no. 748430-THF-OLED).",

year = "2023",

month = feb,

day = "21",

doi = "10.1021/acs.langmuir.2c03391",

language = "English",

volume = "39",

pages = "2829--2837",

journal = "Langmuir",

issn = "0743-7463",

publisher = "American Chemical Society (ACS)",

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TY - JOUR

T1 - Elucidation of an aggregate excited state in the electrochemiluminescence and chemiluminescence of a thermally activated delayed fluorescence (TADF) emitter

AU - Chu, Kenneth

AU - Adsetts, Jonathan R

AU - Whitworth, Zackry

AU - Kumar, Shiv

AU - Zysman-Colman, Eli

AU - Ding, Zhifeng

N1 - Funding: Natural Sciences and Engineering Research Council Canada (NSERC, DG RGPIN-2018-06556 and SPG STPGP2016-493924), Canada Foundation of Innovation/Ontario Innovation Trust (CFI/OIT, 9040), and The University of Western Ontario. The authors acknowledge financial support from the European Union’s Horizon 2020 research and innovation program under a Marie Skłodowska Curie Individual Fellowship to S.K. (MCIF; agreement no. 748430-THF-OLED).

PY - 2023/2/21

Y1 - 2023/2/21

N2 - The electrochemistry, electrochemiluminescence (ECL), and chemiluminescence (CL) properties of a thermally activated delayed fluorescence (TADF) emitter 4,4′-(1,2-dihydroacenaphthylene-5,6-diyl)bis(N,N-diphenylaniline) (TPA-ace-TRZ) and three of its analogues were investigated. TPA-ace-TRZ exhibits both (a) delayed onset of ECL and (b) long-persistent luminescence, which we have attributed to the formation of an aggregate excited state in excimer or exciplex form. The evidence of this aggregate excited state was consistent across ECL annihilation and coreactant pathways as well as in CL. The absolute ECL efficiency of TPA-ace-TRZ using benzoyl peroxide (BPO) as a coreactant was found to be 0.028%, which was 9-fold stronger than the [Ru(bpy)3]2+/BPO reference coereactant system. Furthermore, the absolute CL quantum efficiency of TPA-ace-TRZ was determined to be 0.92%. The performance and flexibility of the TADF emitter TPA-ace-TRZ under these various emissive pathways are highly desirable toward applications in sensing, imaging, and light-emitting devices.

AB - The electrochemistry, electrochemiluminescence (ECL), and chemiluminescence (CL) properties of a thermally activated delayed fluorescence (TADF) emitter 4,4′-(1,2-dihydroacenaphthylene-5,6-diyl)bis(N,N-diphenylaniline) (TPA-ace-TRZ) and three of its analogues were investigated. TPA-ace-TRZ exhibits both (a) delayed onset of ECL and (b) long-persistent luminescence, which we have attributed to the formation of an aggregate excited state in excimer or exciplex form. The evidence of this aggregate excited state was consistent across ECL annihilation and coreactant pathways as well as in CL. The absolute ECL efficiency of TPA-ace-TRZ using benzoyl peroxide (BPO) as a coreactant was found to be 0.028%, which was 9-fold stronger than the [Ru(bpy)3]2+/BPO reference coereactant system. Furthermore, the absolute CL quantum efficiency of TPA-ace-TRZ was determined to be 0.92%. The performance and flexibility of the TADF emitter TPA-ace-TRZ under these various emissive pathways are highly desirable toward applications in sensing, imaging, and light-emitting devices.

KW - Cyclic voltammogram

KW - ECL - voltage curve

KW - Differential pulse

KW - ECL accumulation

KW - Voltammograms

KW - TPA-ace

KW - TPA-ace-CN

KW - 2TPA-ace

U2 - 10.1021/acs.langmuir.2c03391

DO - 10.1021/acs.langmuir.2c03391

M3 - Article

SN - 0743-7463

VL - 39

SP - 2829

EP - 2837

JO - Langmuir

JF - Langmuir

IS - 7

ER -

Elucidation of an aggregate excited state in the electrochemiluminescence and chemiluminescence of a thermally activated delayed fluorescence (TADF) emitter

Abstract

Keywords

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Projects

THF-OLED: H2020 MSCA Fellowship 2016 THF-OLED

Cite this