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Thermally Activated Delayed Fluorescence (TADF) and Enhancing Photoluminescence Quantum Yields of [CuI(diimine)(diphosphine)]+ Complexes—Photophysical, Structural, and Computational Studies
Open accessAbstract
The complexes [Cu(I)(POP)(dmbpy)][BF4] (1) and [Cu(I)(POP)(tmbpy)][BF4] (2) (dmbpy = 4,4'-dimethyl-2,2'-bipyridyl; tmbpy = 4,4',6,6'-tetramethyl-2,2'-bipyridyl; POP = bis[2-(diphenylphosphino)-phenyl]ether) have been studied in a wide temperature range by steady-state and time-resolved emission spectroscopy in fluid solution, frozen solution, and as solid powders. Emission quantum yields of up to 74% were observed for 2 in a rigid matrix (powder), substantially higher than for 1 of around 9% under the same conditions. Importantly, it was found that the emission of 2 at ambient temperature represents a thermally activated delayed fluorescence (TADF) which renders the compound to be a good candidate for singlet harvesting in OLEDs. The role of steric constraints within the complexes, in particular their influences on the emission quantum yields, were investigated by hybrid-DFT calculations for the excited triplet state of 1 and 2 while manipulating the torsion angle between the bipyridyl and POP ligands. Both complexes showed similar flexibility within a ±10° range of the torsion angle; however, 2 appeared limited to this range, whereas 1 could be further twisted with little energy demand. It is concluded that a restricted flexibility leads to a reduction of nonradiative deactivation and thus an increase of emission quantum yield.
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Cited by
Leitl, M. J., Krylova, V. A., Djurovich, P. I., Thompson, M. E., & Yersin, H. (2014) · Journal of the American Chemical Society · doi:10.1021/ja508155x · Cited by 470
Self-citationNandy, A., Duan, C., Taylor, M. G., Liu, F., Steeves, A. H., & Kulik, H. J. (2021) · Chemical Reviews · doi:10.1021/acs.chemrev.1c00347 · Cited by 358
Janet, J. P., Liu, F., Nandy, A., Duan, C., Yang, T., Lin, S., & Kulik, H. J. (2019) · Inorganic Chemistry · doi:10.1021/acs.inorgchem.9b00109 · Cited by 114
Duan, C., Janet, J. P., Liu, F., Nandy, A., & Kulik, H. J. (2019) · Journal of Chemical Theory and Computation · doi:10.1021/acs.jctc.9b00057 · Cited by 87
Liu, F., Duan, C., & Kulik, H. J. (2020) · The Journal of Physical Chemistry Letters · doi:10.1021/acs.jpclett.0c02288 · Cited by 58
Metadata
- Authors
- Linfoot, C. L., Leitl, M. J., Richardson, P., Rausch, A. F., Chepelin, O., White, F. J., Yersin, H., & Robertson, N.
- Venue
- Inorganic Chemistry
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-07-23
- Volume
- 53
- Issue
- 20
- Pages
- 10854-10861
- ISSN
- 0020-1669 (ISSN-L)
- 1520-510X
- OpenAlex
- W2125376928
- Cited by
- 223
- References
- 0
- FWCI
- 13.62
- Type
- journal article
- Language
- en
- Open access
- green
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- The paper
- Linfoot, C. L., Leitl, M. J., Richardson, P., Rausch, A. F., Chepelin, O., White, F. J., Yersin, H., & Robertson, N. (2014). Thermally Activated Delayed Fluorescence (TADF) and Enhancing Photoluminescence Quantum Yields of [CuI(diimine)(diphosphine)]+ Complexes—Photophysical, Structural, and Computational Studies. Inorganic Chemistry. https://doi.org/10.1021/ic500889s
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