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. 2021 Nov 2;12(44):14833-14844.
doi: 10.1039/d1sc03690d. eCollection 2021 Nov 17.

Highly efficient carbazolylgold(iii) dendrimers based on thermally activated delayed fluorescence and their application in solution-processed organic light-emitting devices

Affiliations

Highly efficient carbazolylgold(iii) dendrimers based on thermally activated delayed fluorescence and their application in solution-processed organic light-emitting devices

Lok-Kwan Li et al. Chem Sci. .

Abstract

A new class of C^C^N ligand-containing carbazolylgold(iii) dendrimers has been designed and synthesized. High photoluminescence quantum yields of up to 82% in solid-state thin films and large radiative decay rate constants in the order of 105 s-1 are observed. These gold(iii) dendrimers are found to exhibit thermally activated delayed fluorescence (TADF), as supported by variable-temperature emission spectroscopy, time-resolved photoluminescence decay and computational studies. Solution-processed organic light-emitting diodes (OLEDs) based on these gold(iii) dendrimers have been fabricated, which exhibit a maximum current efficiency of 52.6 cd A-1, maximum external quantum efficiency of 15.8% and high power efficiency of 41.3 lm W-1. The operational stability of these OLEDs has also been recorded, with the devices based on zero- and second-generation dendrimers showing maximum half-lifetimes of 1305 and 322 h at 100 cd m-2, respectively, representing the first demonstration of operationally stable solution-processed OLEDs based on gold(iii) dendrimers.

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Conflict of interest statement

The authors declare no competing finanical interest.

Figures

Scheme 1
Scheme 1. Synthetic route for the tridentate C^C^N ligand-containing carbazolylgold(iii) dendrimers 1–3.
Fig. 1
Fig. 1. Cyclic voltammograms showing the (a) reductive and (b) oxidative scans of 1–3 in dichloromethane (0.1 M nBu4NPF6).
Fig. 2
Fig. 2. (a) UV-vis absorption and (b) normalized emission spectra of 1–3 in toluene at 298 K. (c) Normalized emission spectra of thin films of 10 wt% 1–3 doped into mCP at 298 K.
Fig. 3
Fig. 3. (a) Emission spectra of the thin film of 20 wt% 1 doped in mCP upon increasing the temperature from 77 to 320 K. (b) Emission spectra of the neat film of 3 upon increasing the temperature from 77 to 300 K.
Fig. 4
Fig. 4. A plot of ln(kTADF) against 1/T in the temperature range of 200 to 320 K and its linear fit to eqn (1) for 20 wt% 1 doped in mCP according to the full kinetic model.
Fig. 5
Fig. 5. Calculated electrostatic potential surfaces (isovalue = 0.02) of (a) 1, (b) 2 and (c) 3.
Fig. 6
Fig. 6. (a) Normalized EL spectra and (b) CE against current densities of the solution-processed devices based on 1–3.

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