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Perovskite heteroepitaxy for high-efficiency and stable pure-red LEDs

Nature volume 638, pages 949–956 (2025)Cite this article

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Abstract

Ultrasmall CsPbI3 perovskite quantum dots (QDs) are the most promising candidates for realizing efficient and stable pure-red perovskite light-emitting diodes (PeLEDs)1,2,3,4,5. However, it is challenging for ultrasmall CsPbI3 QDs to retain their solution-phase properties when they assemble into conductive films, greatly hindering their device application3,6. Here we report an approach for in situ deposit stabilized ultrasmall CsPbI3 QD conductive solids, by constructing CsPbI3 QD/quasi-two-dimensional (quasi-2D) perovskite heteroepitaxy. The well-aligned periodic array of edge-oriented ligands at heterointerface triggers a substantial octahedral tilting in a critical layer thickness of CsPbI3 QDs, which heightens the Gibbs free energy difference between the tilted-CsPbI3 and δ-CsPbI3 leading to thermodynamic stabilization of CsPbI3 QDs. The approach allows us to fabricate stabilized CsPbI3 QD conductive films with tunable emission covering the entire red spectral region from 600 nm to 710 nm. Here we report the pure-red PeLEDs with narrow electroluminescence peak centred at 630 nm, matching the Rec. 2100 standard for ultrahigh-definition display. The champion device exhibits a certified external quantum efficiency of 24.6% and a half-lifetime of 6,330 min, ranking as one of the most efficient and stable pure-red PeLED reported to date. The approach is also compatible with large-area manufacturing, enabling 1 cm2 PeLED to exhibit the best external quantum efficiency of 20.5% at 630 nm.

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Fig. 1: The synthesis of CsPbI3 QD se-epitaxy.
Fig. 2: Quasi-2D/CsPbI3 QD/quasi-2D perovskite heteroepitaxy in de-epitaxy film.
Fig. 3: Octahedral tilting.
Fig. 4: The pure-red PeLED performances and operational stability based on CsPbI3 QD de-epitaxy films.

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Data availability

All data generated or analysed during this study are included in this paper and the Supplementary Information. Other data that support the findings of this study are available from the corresponding author upon reasonable request. The open-source StatSTEM software is available on GitHub (https://github.com/quantitativeTEM/StatSTEM).

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Acknowledgements

This work is financially supported by the National Science Fund for Distinguished Young Scholars (grant no T2225024), Foundation for Innovative Research Groups of the National Natural Science Foundation of China (Grant No. 22121005), National Science Foundation (Grant No. 62261160389 and 52072185). The authors extend their appreciation to the Deputyship for Research and Innovation, Ministry of Education in Saudi Arabia for funding this research work through the project no. (IFKSU-DSR-NS2). We thank the staff of beamlines BL17B1, BL14B1, BL03HB and BL02U2 at SSRF for providing the beam time and User Experiment Assist System of SSRF for their help. We thank the staff at the State Key Laboratory of Medicinal Chemical Biology of Nankai University for their assistance with collecting cryo-EM data. This work was partly supported by Analysis Platform of New Matter Structure at Nankai University.

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Author notes

  1. Tong Zhou

    Present address: Hubei Key Laboratory of Energy Storage and Power Battery, School of Mathematics, Physics and Optoelectronic Engineering, Hubei University of Automotive Technology, Shiyan, People’s Republic of China

  2. These authors contributed equally: Keyu Wei, Tong Zhou, Yuanzhi Jiang

Authors and Affiliations

  1. State Key Laboratory of Advanced Chemical Power Sources, Frontiers Science Center for New Organic Matter, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin, People’s Republic of China

    Keyu Wei, Tong Zhou, Yuanzhi Jiang, Changjiu Sun, Saisai Li, Xinliang Fu, Cejun Hu, Wei Zhang, Jun Chen & Mingjian Yuan

  2. Haihe Laboratory of Sustainable Chemical Transformations, Tianjin, People’s Republic of China

    Yuanzhi Jiang, Wei Zhang, Jun Chen & Mingjian Yuan

  3. College of Chemistry, Key Laboratory of Theoretical and Computational Photochemistry of Ministry of Education, Beijing Normal University, Beijing, People’s Republic of China

    Yulong Liu & Run Long

  4. Ultrafast Electron Microscopy Laboratory, Key Laboratory of Weak-Light Nonlinear Photonics (Ministry of Education), School of Physics, Nankai University, Tianjin, People’s Republic of China

    Siyu Liu & Xuewen Fu

  5. Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland

    Shun Tian & Mohammad Khaja Nazeeruddin

  6. School of Microelectronics, Fudan University, Shanghai, People’s Republic of China

    Yingguo Yang

  7. Department of Chemistry, College of Science, Princess Nourah bint Abdulrahman University, Riyadh, Saudi Arabia

    Najla AlMasoud

  8. Department of Physics and Astronomy, College of Science, King Saud University, Riyadh, Saudi Arabia

    Saif M. H. Qaid

  9. School of Energy and Environment and Department of Materials Science and Engineering and Centre for Functional Photonics (CFP), City University of Hong Kong, Hong Kong, People’s Republic of China

    Hsien-Yi Hsu

  10. Department of Mechanical Engineering, The University of Hong Kong, Hong Kong, People’s Republic of China

    Wen-Di Li & Ji Tae Kim

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  1. Keyu Wei
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  2. Tong Zhou
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  3. Yuanzhi Jiang
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Contributions

M.Y. conceived the idea. M.Y., J.C. and W.Z. guided the project. K.W., Y.J. and M.Y. developed the approach for the fabrication of perovskite heteroepitaxy. K.W. synthesized the materials and perovskite films. K.W., S.Li, Xinliang Fu, C.H., Y.J., H.-Y.H., W.-D.L. and J.T.K. characterized the materials and perovskite films. Y.Y. carried out the GIWAXS measurements and provided the analyses. S. Liu, Xuewen Fu, N.A. and S.M.H.Q. performed the transient absorption and analysed the data. K.W. prepared the TEM samples. T.Z. and W.Z. carried out the TEM characterizations and analyses. K.W. and C.S. carried out the device fabrication and characterizations. S.T. and M.K.N. performed the optical simulations of PeLEDs. Y.L. and R.L. carried out theoretical calculations. K.W., T.Z., W.Z., J.C. and M.Y. co-wrote the paper. All authors discussed the results and commented on the paper.

Corresponding authors

Correspondence to Wei Zhang, Jun Chen or Mingjian Yuan.

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Extended data figures and tables

Extended Data Fig. 1 Photoluminescence spectra of se-epitaxy films.

a, The se-epitaxy films exhibited tunable photoluminescence wavelength by varying the Br-DMA+ ligand concentrations from 0.02 M to 0.28 M with incorporation of PEA+ co-ligands. b,c, Photoluminescence spectra of se-epitaxy films with photoluminescence peak at 631 nm (b) and 645 nm (c) plotting in linear scale (light dashed lines) and log scale (dark solid lines).

Extended Data Fig. 2 Ultrafast transient absorption (TA) spectra and corresponding photoluminescence spectra for se-epitaxy and de-epitaxy films with different bandgap.

a-c, Transient absorption spectra of se-epitaxy films with photoluminescence peak at 634 nm (a), 672 nm (b), and 700 nm (c). d-f, Corresponding absorption (grey solid lines) and photoluminescence spectra of se-epitaxy films, where the photoluminescence spectra were plotted in linear scale (green dashed lines) and log scale (green solid lines). g-i, Transient absorption spectra of de-epitaxy films with photoluminescence peak at 633 nm (g), 670 nm (h), and 700 nm (i). j-l, Corresponding absorption (grey solid lines) and photoluminescence spectra of de-epitaxy films, where the photoluminescence spectra were plotted in linear scale (blue dashed lines) and log scale (blue solid lines).

Extended Data Fig. 3 Wide-field HAADF images of se-epitaxy film and de-epitaxy film.

a,b Wide-field HAADF images of se-epitaxy film (a) and de-epitaxy film (b), reprinted from Fig. 1f and Fig. 2f. Inset: enlarged HAADF images from regions 1–4 marked by the white dashed boxes in both (a) and (b), respectively.

Extended Data Fig. 4 Electron tomography (ET) reconstruction of se-epitaxy composite.

a, Schematic of ET structure reconstruction. b, HRTEM image of a representative se-epitaxy composite. c-e, 3D reconstruction images for the representative se-epitaxy composite under various viewing angles. Inset: schematic illustrations of se-epitaxy composites. The reconstruction images reveal a complete nanoparticle in the blue region with size of 7.4 nm × 7.0 nm × 11.4 nm and a single-edge-attached nanoplate in red region, identifying as CsPbI3 QD/quasi-2D perovskite single-edge attached epitaxy (se-epitaxy).

Extended Data Fig. 5 Orientation instructions in se-epitaxy and de-epitaxy.

a, Unit cell model of γ-CsPbI3 viewed along the \([1\bar{1}0]\) zone axis. b, Unit cell model of α-CsPbI3 viewed along the [\(001\)] zone axis. c, Unit cell model of PEA+-based quasi-2D perovskites viewed along the [\(110\)] zone axis. d, Atomic-scale HAADF image of the Br-DMA+-based γ-CsPbI3 and PEA+-based quasi-2D perovskites obtained from Fig. 1j. The unit cell model is consistent with the microstructure, indicating that \([1\bar{1}0]\)γ-CsPbI3 is parallel to [\(110\)]PEA+ based quasi-2D perovskites. This orientation relationship indicates that (110)γ-CsPbI3 is parallel to \((1\bar{1}0)\)PEA+ based quasi-2D perovskites. e, Unit cell model of Br-PEA+-based quasi-2D perovskites viewed along the [\(110\)] zone axis. f,g, Atomic-scale HAADF images of the Br-DMA+-based γ-CsPbI3 and Br-PEA+-based quasi-2D perovskites obtained from the bottom (f) and top (g) heterointerface area in Fig. 2g. The unit cell model is consistent with the microstructure, indicating that \([1\bar{1}0]\)γ-CsPbI3 is parallel to [\(110\)]Br-PEA+ based quasi-2D perovskites. This orientation relationship indicates that (110)γ-CsPbI3 is parallel to \((1\bar{1}0)\)Br-PEA+ based quasi-2D perovskites.

Extended Data Fig. 6 Heteroepitaxial interface structure and corresponding strain analysis in se-epitaxy and de-epitaxy composites.

a, Low-dose HRTEM image of representative se-epitaxy composite. b, Enlarged HRTEM image of the region marked by white solid box in (a). c, Simulation model of the heterointerface in se-epitaxy composite. d, The εxx strain mapping of CsPbI3 QD (marked by blue dashed boxes) in se-epitaxy (a) composite. e, The εxx strain mapping of CsPbI3 QD (marked by blue dashed boxes) in de-epitaxy composite (Fig. 2k).

Extended Data Fig. 7 Structural characterizations of the de-epitaxy composites.

a,b, Atomic-scale HAADF images of de-epitaxy composite with various particle sizes. c,d, Corresponding plots of octahedral tilting angle as a function of the [PbI6]4− unit cell across the CsPbI3 QDs (along the x-direction), with corresponding 95% confidence bands. The data presented as mean ± standard deviation of twelve [PbI6]4− unit cells in the y-direction.

Extended Data Fig. 8 Excitation power density-dependent PLQYs of de-epitaxy film with photoluminescence peak at 630 nm

.

Extended Data Fig. 9 The de-epitaxy PeLED with electroluminescence peak at 600 nm.

a,b, The current density-voltage-luminescence (J-V-L) curves (a), and EQE-J curve (b) of PeLED with active area of 8.6 mm2. Inset to (b): electroluminescence spectrum of PeLED. c, The photograph of large-area (4 cm2) PeLED with electroluminescence peak at 600 nm. d, The luminance mapping of large-area PeLED under operating voltage of 4.5 V (c).

Extended Data Fig. 10 Device performance of large-area (1 cm2) de-epitaxy PeLEDs.

a-f, Device performance of PeLED with electroluminescence peak centered at 630 nm. The corresponding J-V-L curves (a), EQE-J curve (b), electroluminescence spectra at different voltage bias (c), angle-dependent electroluminescence intensity (d), histogram of EQE (e) and luminance mapping under operating voltage of 5.0 V (f). g, Photograph of large-area (1 cm2) PeLEDs with electroluminescence peak ranging from 600 nm to 660 nm.

Extended Data Table 1 Summary of efficient pure-halide red PeLEDs reported to date3,4,5,7,8,9,10,11,12,13,19,21,22,27,64
Full size table

Supplementary information

Supplementary Information

Supplementary Notes 1–8, including Supplementary Figs. 1–22 and Supplementary Tables 1–3.

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Wei, K., Zhou, T., Jiang, Y. et al. Perovskite heteroepitaxy for high-efficiency and stable pure-red LEDs. Nature 638, 949–956 (2025). https://doi.org/10.1038/s41586-024-08503-9

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