The degradation mechanism of multi-resonance thermally activated delayed fluorescence materials
Abstract 1,4-Azaborine-based arenes are promising electroluminescent emitters with thermally activated delayed fluorescence (TADF), offering narrow emission spectra and high quantum yields due to a multi-resonance (MR) effect. However, their practical application is constrained by their limited oper...
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-55620-0 |
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| author | Byung Hak Jhun Yerin Park Hwang Suk Kim Ji Hye Baek Joonghyuk Kim Eunji Lee Hyejin Moon Changjin Oh Yongsik Jung Seunghee Choi Mu-Hyun Baik Youngmin You |
| author_facet | Byung Hak Jhun Yerin Park Hwang Suk Kim Ji Hye Baek Joonghyuk Kim Eunji Lee Hyejin Moon Changjin Oh Yongsik Jung Seunghee Choi Mu-Hyun Baik Youngmin You |
| author_sort | Byung Hak Jhun |
| collection | DOAJ |
| description | Abstract 1,4-Azaborine-based arenes are promising electroluminescent emitters with thermally activated delayed fluorescence (TADF), offering narrow emission spectra and high quantum yields due to a multi-resonance (MR) effect. However, their practical application is constrained by their limited operational stability. This study investigates the degradation mechanism of MR-TADF molecules. Electroluminescent devices incorporating these compounds display varied operational lifetimes, uncorrelated with excitonic stability or external quantum efficiency roll-off. Bulk electrolysis reveals significant instability in the radical cationic forms of MR-TADF compounds, with device lifetime linked to the Faradaic yield of oxidation. Comprehensive chemical analyses corroborate that the degradation byproducts originated from intramolecular cyclization of radical cation, followed by hydrogen atom transfer. The mechanism is further supported by enhanced stability observed in a deuterated MR-TADF emitter, attributed to a secondary kinetic isotope effect. These findings provide insights into the stabilizing effects of deuteration and mechanism-driven strategies for designing MR-TADF compounds with improved operational longevity. |
| format | Article |
| id | doaj-art-1ca62cebfe3f48d5b7cb7fc164b077d3 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-1ca62cebfe3f48d5b7cb7fc164b077d32025-01-05T12:37:32ZengNature PortfolioNature Communications2041-17232025-01-0116111410.1038/s41467-024-55620-0The degradation mechanism of multi-resonance thermally activated delayed fluorescence materialsByung Hak Jhun0Yerin Park1Hwang Suk Kim2Ji Hye Baek3Joonghyuk Kim4Eunji Lee5Hyejin Moon6Changjin Oh7Yongsik Jung8Seunghee Choi9Mu-Hyun Baik10Youngmin You11Department of Chemical and Biomolecular Engineering, Yonsei UniversityDepartment of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)Samsung Advanced Institute of Technology, Samsung Electronics Co. LtdDepartment of Chemical and Biomolecular Engineering, Yonsei UniversitySamsung Advanced Institute of Technology, Samsung Electronics Co. LtdDepartment of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)Samsung Advanced Institute of Technology, Samsung Electronics Co. LtdDivision of Chemical Engineering and Materials Science, Ewha Womans UniversityDepartment of Chemistry, Korea Advanced Institute of Science and Technology (KAIST)Department of Chemical and Biomolecular Engineering, Yonsei UniversityAbstract 1,4-Azaborine-based arenes are promising electroluminescent emitters with thermally activated delayed fluorescence (TADF), offering narrow emission spectra and high quantum yields due to a multi-resonance (MR) effect. However, their practical application is constrained by their limited operational stability. This study investigates the degradation mechanism of MR-TADF molecules. Electroluminescent devices incorporating these compounds display varied operational lifetimes, uncorrelated with excitonic stability or external quantum efficiency roll-off. Bulk electrolysis reveals significant instability in the radical cationic forms of MR-TADF compounds, with device lifetime linked to the Faradaic yield of oxidation. Comprehensive chemical analyses corroborate that the degradation byproducts originated from intramolecular cyclization of radical cation, followed by hydrogen atom transfer. The mechanism is further supported by enhanced stability observed in a deuterated MR-TADF emitter, attributed to a secondary kinetic isotope effect. These findings provide insights into the stabilizing effects of deuteration and mechanism-driven strategies for designing MR-TADF compounds with improved operational longevity.https://doi.org/10.1038/s41467-024-55620-0 |
| spellingShingle | Byung Hak Jhun Yerin Park Hwang Suk Kim Ji Hye Baek Joonghyuk Kim Eunji Lee Hyejin Moon Changjin Oh Yongsik Jung Seunghee Choi Mu-Hyun Baik Youngmin You The degradation mechanism of multi-resonance thermally activated delayed fluorescence materials Nature Communications |
| title | The degradation mechanism of multi-resonance thermally activated delayed fluorescence materials |
| title_full | The degradation mechanism of multi-resonance thermally activated delayed fluorescence materials |
| title_fullStr | The degradation mechanism of multi-resonance thermally activated delayed fluorescence materials |
| title_full_unstemmed | The degradation mechanism of multi-resonance thermally activated delayed fluorescence materials |
| title_short | The degradation mechanism of multi-resonance thermally activated delayed fluorescence materials |
| title_sort | degradation mechanism of multi resonance thermally activated delayed fluorescence materials |
| url | https://doi.org/10.1038/s41467-024-55620-0 |
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