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Article: Tetradentate C∧C∧N∧N Ligand-Containing Gold(III) Complexes with Orange to Deep-Red Thermally Activated Delayed Fluorescence (TADF) and Their Application in Organic Light-Emitting Devices

TitleTetradentate C∧C∧N∧N Ligand-Containing Gold(III) Complexes with Orange to Deep-Red Thermally Activated Delayed Fluorescence (TADF) and Their Application in Organic Light-Emitting Devices
Authors
Issue Date19-Apr-2023
PublisherAmerican Chemical Society
Citation
Journal of the American Chemical Society, 2023, v. 145, n. 17, p. 9584-9595 How to Cite?
Abstract

A new class of thermally activated delayed fluorescence (TADF) tetradentate C<^>C<^>N<^>N ligand-containing gold(III) complexes containing acridinyl moieties has been designed and synthesized. These complexes exhibit orange-red to deep-red emission with photoluminescence quantum yields (PLQYs) of up to 0.76 in solid-state thin films. Short excited-state lifetimes of <= 2.0 mu s and large radiative decay rate constants (kr) in the order of 105 s-1 have also been found in the complexes. High-performance solution-processed and vacuum-deposited organic light-emitting devices (OLEDs) based on these complexes have been fabricated, demonstrating high maximum external quantum efficiencies (EQEs) of 12.2 and 12.7%, respectively, which are among the best values ever reported for red-emitting gold(III)-based OLEDs. In addition, satisfactory operational half-lifetime (LT50) values of up to 34,058 h have been attained in these red-emitting devices. It is found that the operational stability is strongly dependent on the choice of functional groups on the acridinyl moieties, of which the incorporation of -O- and -S- linkers can effectively prolong the LT50 value by an order of magnitude. The TADF properties of the complexes are substantiated by the hypsochromic shift in emission energies and the remarkable enhancement in the emission intensity upon increasing temperature. The TADF properties have also been supported by temperature-dependent ultrafast transient absorption studies, with the direct observation of reverse intersystem crossing (RISC) and the determination of the activation parameters for the very first time, together with their excited-state dynamics.


Persistent Identifierhttp://hdl.handle.net/10722/331615
ISSN
2023 Impact Factor: 14.4
2023 SCImago Journal Rankings: 5.489
ISI Accession Number ID

 

DC FieldValueLanguage
dc.contributor.authorKwok, Wing-Kei-
dc.contributor.authorLi, Lok-Kwan-
dc.contributor.authorLai, Shiu-Lun-
dc.contributor.authorLeung, Ming-Yi-
dc.contributor.authorTang, Wai Kit-
dc.contributor.authorCheng, Shun-Cheung-
dc.contributor.authorTang, Man-Chung-
dc.contributor.authorCheung, Wai-Lung-
dc.contributor.authorKo, Chi-Chiu-
dc.contributor.authorChan, Mei-Yee-
dc.contributor.authorYam, Vivian Wing-Wah-
dc.date.accessioned2023-09-21T06:57:23Z-
dc.date.available2023-09-21T06:57:23Z-
dc.date.issued2023-04-19-
dc.identifier.citationJournal of the American Chemical Society, 2023, v. 145, n. 17, p. 9584-9595-
dc.identifier.issn0002-7863-
dc.identifier.urihttp://hdl.handle.net/10722/331615-
dc.description.abstract<p>A new class of thermally activated delayed fluorescence (TADF) tetradentate C<^>C<^>N<^>N ligand-containing gold(III) complexes containing acridinyl moieties has been designed and synthesized. These complexes exhibit orange-red to deep-red emission with photoluminescence quantum yields (PLQYs) of up to 0.76 in solid-state thin films. Short excited-state lifetimes of <= 2.0 mu s and large radiative decay rate constants (kr) in the order of 105 s-1 have also been found in the complexes. High-performance solution-processed and vacuum-deposited organic light-emitting devices (OLEDs) based on these complexes have been fabricated, demonstrating high maximum external quantum efficiencies (EQEs) of 12.2 and 12.7%, respectively, which are among the best values ever reported for red-emitting gold(III)-based OLEDs. In addition, satisfactory operational half-lifetime (LT50) values of up to 34,058 h have been attained in these red-emitting devices. It is found that the operational stability is strongly dependent on the choice of functional groups on the acridinyl moieties, of which the incorporation of -O- and -S- linkers can effectively prolong the LT50 value by an order of magnitude. The TADF properties of the complexes are substantiated by the hypsochromic shift in emission energies and the remarkable enhancement in the emission intensity upon increasing temperature. The TADF properties have also been supported by temperature-dependent ultrafast transient absorption studies, with the direct observation of reverse intersystem crossing (RISC) and the determination of the activation parameters for the very first time, together with their excited-state dynamics.<br></p>-
dc.languageeng-
dc.publisherAmerican Chemical Society-
dc.relation.ispartofJournal of the American Chemical Society-
dc.titleTetradentate C∧C∧N∧N Ligand-Containing Gold(III) Complexes with Orange to Deep-Red Thermally Activated Delayed Fluorescence (TADF) and Their Application in Organic Light-Emitting Devices-
dc.typeArticle-
dc.identifier.doi10.1021/jacs.2c13820-
dc.identifier.scopuseid_2-s2.0-85153971420-
dc.identifier.volume145-
dc.identifier.issue17-
dc.identifier.spage9584-
dc.identifier.epage9595-
dc.identifier.eissn1520-5126-
dc.identifier.isiWOS:000975419800001-
dc.identifier.issnl0002-7863-

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