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Strategies towards rational design of gold(iii) complexes for high-performance organic light-emitting devices

Abstract

Gold(iii) complexes are attractive candidates as phosphorescent dopants in organic light-emitting devices for high-luminance full-colour displays. However, no data on the stability of such devices have been reported to date. Through rational molecular design and synthesis, we have successfully generated a new class of cyclometalated gold(iii) C^C^N complexes with tunable emission colours spanning from sky-blue to red. These complexes exhibit high photoluminescence quantum yields of up to 80% in solid-state thin films, excellent solubility and high thermal stability. Solution-processable and vacuum-deposited organic light-emitting devices based on these complexes operate with external quantum efficiencies of up to 11.9% and 21.6%, respectively, and operational half-lifetimes of up to 83,000 h at 100 cd m−2.

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Fig. 1: Schematic of potential energy profiles of the deactivation pathway via the 3DS.
Fig. 2: Molecular structures of the investigated complexes.
Fig. 3: Electrochemical and photophysical properties of gold(iii) complexes.
Fig. 4: Optimized ground-state geometries, selected structural parameters and orbital energy diagrams of 2–5.
Fig. 5: Key parameters of the fabricated OLEDs based on 1–5.
Fig. 6: Operational stability.

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The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

V.W.-W.Y. acknowledges UGC funding administrated by The University of Hong Kong (HKU) for supporting the Electrospray Ionization Quadrupole Time-of-Flight Mass Spectrometry Facilities under the Support for Interdisciplinary Research in Chemical Science, the HKU Development Fund and the Dr. Hui Wai Haan Fund for funding the X-Ray Diffractometer Facilities, and the support from HKU University Research Committee (URC) Strategically Oriented Research Theme on Functional Materials for Molecular Electronics Towards Materials and Energy Applications. The work described in this paper was fully supported by a grant from the University Grants Committee Areas of Excellence (AoE) Scheme from the Hong Kong Special Administrative Region, China (project no. AoE/P-03/08). L.-K.L. acknowledges the receipt of postgraduate studentships from HKU. The computations were performed using the HKU ITS research computing facilities. W.-L. Cheung is acknowledged for his assistance in the preparation of solution-processable OLED fabrication. K.-H. Low is acknowledged for his assistance in X-ray crystal structure data collection, and L.-Y. Yao and C.-H. Lee are acknowledged for their assistance in X-ray crystal structure determination.

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Contributions

V.W.-W.Y. initiated and designed the research. V.W.-W.Y., M.-C.T. and L.-K.L. designed the gold(iii) complexes. L.-K.L., M.-C.T. and W.-K.K. conducted the synthesis, characterization, electrochemical and photophysical measurements of the gold(iii) complexes. S.-L.L. and M.-Y.C. carried out the OLED fabrication and characterizations. M.N. performed and analysed the computational calculations. V.W.-W.Y. supervised the work. All authors discussed the results and contributed to the manuscript.

Corresponding authors

Correspondence to Mei-Yee Chan or Vivian Wing-Wah Yam.

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Competing interests

V.W.-W.Y., M.-C.T., M.-Y.C and L.-K.L. have filed the following patent applications: The University of Hong Kong, Hong Kong; V.W.-W.Y., M.-C.T., M.-Y.C. and C.-H. Lee, Molecular design and OLED application. US provisional patent application no. 62/403,799 (pending); The University of Hong Kong, Hong Kong; V.W.-W.Y., M.-C.T., M.-Y.C., C.-H. Lee and L.-K.L. Molecular design and OLED application. PCT patent application no. PCT/CN2017/105241 (pending).

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Li, LK., Tang, MC., Lai, SL. et al. Strategies towards rational design of gold(iii) complexes for high-performance organic light-emitting devices. Nature Photon 13, 185–191 (2019). https://doi.org/10.1038/s41566-018-0332-z

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