Kai Lin Woon
Intramolecular Dimerization Quenching of Delayed Emission in Asymmetric D-D’-A TADF Emitters
Woon, Kai Lin; Yi, Chih-Lun; Pan, Kuan-Chung; Etherington, Marc K.; Wu, Chung-Chih; Wong, Ken-Tsung; Monkman, Andrew P.
Authors
Chih-Lun Yi
Kuan-Chung Pan
Marc K. Etherington
Chung-Chih Wu
Ken-Tsung Wong
Professor Andrew Monkman a.p.monkman@durham.ac.uk
Professor
Abstract
Understanding the excited-state dynamics and conformational relaxation in thermallyactivated delayed fluorescence (TADF) molecules, including conformations that potentially support intramolecular through-space charge transfer, can open new avenues for TADF molecular design as well as elucidate complex photophysical pathways in structurally complex molecules. Emissive molecules comprising a donor (triphenylamine, TPA) and an acceptor (triphenyltriazine, TRZ) bridged by a second donor (9,9 dimethyl-9-10- dihydroacridin, DMAC or phenoxazine, PXZ) are synthesized and characterized. In solution, the flexibility of the sp3-hybridized carbon atom in DMAC of DMAC-TPA-TRZ, compared to the rigid PXZ, allows significant conformational reorganisation giving rise to multiple charge-transfer excited states. As a result of such reorganization, the TRZ and TPA moieties become co-facially aligned, driven by strong dipole-dipole attraction between the TPA and TRZ units, forming a weakly charge transfer dimer state, in stark contrast to the case of PXZTPA- TRZ where the rigid PXZ bridge only supports a single PXZ-TRZ CT state. The low energy TPA-TRZ dimer, is found to have a high energy dimer local triplet state, which quenches delayed emission because the resultant singlet CT local triplet energy gap is too large to mediate efficient reverse intersystem crossing. However, organic light emitting diodes using PXZ-TPA-TRZ as an emitting dopant resulted in EQE as high as 22%, more than 2 times higher than that of DMAC-TPA-TRZ-based device showing the impact that such intramolecular reorganization and donor acceptor dimerization has on TADF performance.
Citation
Woon, K. L., Yi, C., Pan, K., Etherington, M. K., Wu, C., Wong, K., & Monkman, A. P. (2019). Intramolecular Dimerization Quenching of Delayed Emission in Asymmetric D-D’-A TADF Emitters. Journal of Physical Chemistry C, 123(19), 12400-12410. https://doi.org/10.1021/acs.jpcc.9b01900
Journal Article Type | Article |
---|---|
Acceptance Date | Apr 17, 2019 |
Online Publication Date | Apr 17, 2019 |
Publication Date | May 17, 2019 |
Deposit Date | May 1, 2019 |
Publicly Available Date | May 21, 2019 |
Journal | Journal of Physical Chemistry C |
Print ISSN | 1932-7447 |
Electronic ISSN | 1932-7455 |
Publisher | American Chemical Society |
Peer Reviewed | Peer Reviewed |
Volume | 123 |
Issue | 19 |
Pages | 12400-12410 |
DOI | https://doi.org/10.1021/acs.jpcc.9b01900 |
Public URL | https://durham-repository.worktribe.com/output/1302827 |
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Copyright Statement
This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
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