期刊
ADVANCED MATERIALS
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202212064
关键词
curved nanographenes; multiple emission; phosphorescence; thermally activated delayed fluorescence (TADF)
The photophysical properties of three curved nanographenes (CNG 6, 7, and 8) are investigated using time-resolved and temperature-dependent photoluminescence spectroscopy. Dual fluorescence and phosphorescence are observed in CNG 7 and 8 at low temperatures. Thermally activated delayed fluorescence (TADF) is observed in a narrow temperature range, and non-Kasha behavior is observed due to the optimization of higher-lying S-2 minimum. The presence of higher-lying dark triplet states provides mechanistic evidence for the observed TADF phenomena.
The intriguing and rich photophysical properties of three curved nanographenes (CNG 6, 7, and 8) are investigated by time-resolved and temperature-dependent photoluminescence (PL) spectroscopy. CNG 7 and 8 exhibit dual fluorescence, as well as dual phosphorescence at low temperature in the main PL bands. In addition, hot bands are detected in fluorescence as well as phosphorescence, and, in the narrow temperature range of 100-140 K, thermally activated delayed fluorescence (TADF) with lifetimes on the millisecond time-scale is observed. These findings are rationalized by quantum-chemical simulations, which predict a single minimum of the S-1 potential of CNG 6, but two S-1 minima for CNG 7 and CNG 8, with considerable geometric reorganization between them, in agreement with the experimental findings. Additionally, a higher-lying S-2 minimum close to S-1 is optimized for the three CNG, from where emission is also possible due to thermal activation and, hence, non-Kasha behavior. The presence of higher-lying dark triplet states close to the S-1 minima provides mechanistic evidence for the TADF phenomena observed. Non-radiative decay of the T-1 state appears to be thermally activated with activation energies of roughly 100 meV and leads to disappearance of phosphorescence and TADF at T > 140 K.
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