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Multivalent-effect immobilization of reduced-dimensional perovskites for efficient and spectrally stable deep-blue light-emitting diodes

Nature Nanotechnology volume 20, pages 507–514 (2025)Cite this article

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Abstract

Despite substantial advances in green and red metal halide perovskite light-emitting diodes (PeLEDs), blue PeLEDs, particularly deep-blue ones (defined as Commission International de l’Eclairage y coordinate (CIEy) less than 0.06) that meet the latest Rec. 2020 colour gamut standard, lag dramatically behind owing to a severe phase segregation-induced electroluminescent spectral shift and low exciton utilization in broadened bandgap perovskite emitters. Here we propose a multivalent immobilization strategy to realize high-efficiency and spectrally stable deep-blue PeLEDs by introducing a polyfluorinated oxygen-containing molecule. Systematic experiments and extensive 5,000 fs ab initio molecular dynamics simulations reveal that a crucial role of the multivalent effect stemming from three kinds of interaction of hydrogen bond (F···H–N), ionic bond (F–Pb) and coordination bond (C=O:Pb) with perovskite is to synergistically stabilize the perovskite phase and enhance exciton radiative recombination. The resultant exciton concentration and exciton recombination rate of the deep-blue perovskite emitter are increased by factors of 1.66 and 1.64, respectively. In this context, our target PeLEDs demonstrate a peak external quantum efficiency of up to 15.36% at a deep-blue emission wavelength of 459 nm and a half-lifetime of 144 min at a constant current density of 0.45 mA cm−2. Moreover, the deep-blue PeLEDs maintain a constant spectrum peak with CIE chromaticity coordinates of (0.136, 0.051) under a steady driving current for 60 min.

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Fig. 1: Device performance and self-consistent photoelectric simulations of deep-blue PeLEDs.
Fig. 2: Optical and electrical characterizations of the RDP films.
Fig. 3: Multivalent effect between organic species and RDPs.
Fig. 4: Immobilization mechanism of deep-blue perovskite emitters by multivalent effect.

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The main data supporting the findings of this study are available within the article and its Supplementary Information. Extra data are available from the corresponding authors upon reasonable request.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (NSFC 51972137, 62174104 and 62321166653), the National Key Research and Development Program of China (2022YFE0200200), the Science and Technology Planning Project of Jilin Province (grant numbers 20190201306JC and 20230101020JC), the Innovative Capacity Building Foundation of Jilin Province Development and Reform Commission (2023C034-5), the start-up funding and Excellent Youth Faculty Program of Jilin University, the Fundamental Research Funds for the Central Universities and the Program of Shanghai Academic/Technology Research Leader (22XD1421200). We thank the staff of beamlines BL17B1, BL02U2 and BL19U2 at SSRF for providing the beam time and User Experiment Assist System of SSRF for their help.

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Authors and Affiliations

  1. College of Physics, Jilin University, Changchun, China

    Jianchao Dong, Bin Zhao, Huiyu Ji, Ziang Zang, Dongyuan Han, Jie Wang & Ning Wang

  2. Key Laboratory of Advanced Display and System Applications of Ministry of Education, Shanghai University, Shanghai, China

    Lingmei Kong & Xuyong Yang

  3. School of Electronic and Information Engineering, Hebei University of Technology, Tianjin, China

    Chunshuang Chu & Zi-Hui Zhang

  4. State Key Laboratory of Superhard Materials, Key Laboratory of Automobile Materials of MOE, School of Materials Science and Engineering, Jilin University, Changchun, China

    Yuhao Fu & Lijun Zhang

  5. Shanghai Synchrotron Radiation Facility (SSRF), Zhangjiang Lab, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, China

    Yingguo Yang

  6. School of Microelectronics, Fudan University, Shanghai, China

    Yingguo Yang

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Contributions

J.D. and H.J. designed and fabricated the deep-blue PeLEDs under the guidance of N.W. Y.Y. carried out the GIWAXS measurements and analysed the results. B.Z. carried out the calculations. C.C. and Z.-H.Z. conducted the semiconductor physical simulations. Z.Z. carried out the PLQY measurements. J.W. and D.H. assisted with the preparation of diagrams and carried out the optical measurements. J.D. and H.J. performed the transient absorption and electrical measurements. J.D., H.J., B.Z., L.K., Y.Y., Y.F., L.Z., X.Y. and N.W. prepared and polished the paper. All authors discussed the results and commented on the paper.

Corresponding authors

Correspondence to Xuyong Yang or Ning Wang.

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Nature Nanotechnology thanks Jung-Yong Lee, Tae-Woo Lee and Guichuan Xing for their contribution to the peer review of this work.

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Supplementary Figs. 1–38, discussion and Tables 1–5.

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Dong, J., Zhao, B., Ji, H. et al. Multivalent-effect immobilization of reduced-dimensional perovskites for efficient and spectrally stable deep-blue light-emitting diodes. Nat. Nanotechnol. 20, 507–514 (2025). https://doi.org/10.1038/s41565-024-01852-6

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