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Nanosurface-reconstructed perovskite for highly efficient and stable active-matrix light-emitting diode display

Nature Nanotechnology (2024)Cite this article

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Abstract

Perovskite quantum dots (QDs) are promising for various photonic applications due to their high colour purity, tunable optoelectronic properties and excellent solution processability. Surface features impact their optoelectronic properties, and surface defects remain a major obstacle to progress. Here we develop a strategy utilizing diisooctylphosphinic acid-mediated synthesis combined with hydriodic acid-etching-driven nanosurface reconstruction to stabilize CsPbI3 QDs. Diisooctylphosphinic acid strongly adsorbs to the QDs and increases the formation energy of halide vacancies, enabling nanosurface reconstruction. The QD film with nanosurface reconstruction shows enhanced phase stability, improved photoluminescence endurance under thermal stress and electric field conditions, and a higher activation energy for ion migration. Consequently, we demonstrate perovskite light-emitting diodes (LEDs) that feature an electroluminescence peak at 644 nm. These LEDs achieve an external quantum efficiency of 28.5% and an operational half-lifetime surpassing 30 h at an initial luminance of 100 cd m−2, marking a tenfold improvement over previously published studies. The integration of these high-performance LEDs with specifically designed thin-film transistor circuits enables the demonstration of solution-processed active-matrix perovskite displays that show a peak external quantum efficiency of 23.6% at a display brightness of 300 cd m−2. This work showcases nanosurface reconstruction as a pivotal pathway towards high-performance QD-based optoelectronic devices.

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Fig. 1: Characteristics of pure-red PeLEDs.
Fig. 2: Nanosurface reconstruction of CsPbI3 QDs.
Fig. 3: Improved optical properties and stability.
Fig. 4: Stability analysis in a device configuration.
Fig. 5: Performance of the active-matrix PeLED display.

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The data that support the findings of this study are available from the corresponding authors upon reasonable request. Source data are provided with this paper.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (52102188, X.D.; 52172159, J.H.), the Key Research and Development Program of Zhejiang Province (2021C01030, Z.Y.), the Natural Science Foundation of Zhejiang Province (LQ21F040005, X.D.), the Young Elite Scientists Sponsorship Program by CAST (YESS20210444, X.D.), the science and technology projects of the Institute of Wenzhou, Zhejiang University (XMGL-KJZX-202302, X.D.), the Fundamental Research Funds for the Central Universities (17241022301, X.D.) and the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering (2022SZ-TD004, H.H.). X.D. gratefully acknowledges the support of the Zhejiang University Education Foundation Qizhen Scholar Foundation. H.L. sincerely thanks J. Huang for his support. We thank J. Li and Y. He for their assistance in the synthesis of the QDs and device fabrication.

Author information

Authors and Affiliations

  1. School of Materials Science and Engineering, State Key Laboratory of Silicon and Advanced Semiconductor Materials, Zhejiang University, Hangzhou, People’s Republic of China

    Hongjin Li, Yifeng Feng, Meiyi Zhu, Yun Gao, Chao Fan, Qiaopeng Cui, Qiuting Cai, Haiping He, Xingliang Dai, Jingyun Huang & Zhizhen Ye

  2. Wenzhou Key Laboratory of Novel Optoelectronic and Nano Materials and Engineering Research Centre of Zhejiang Province, Institute of Wenzhou, Zhejiang University, Wenzhou, People’s Republic of China

    Meiyi Zhu, Chao Fan, Haiping He, Xingliang Dai, Jingyun Huang & Zhizhen Ye

  3. Department of Applied Physics, The Hong Kong Polytechnic University, Hong Kong, People’s Republic of China

    Ke Yang

  4. Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering, Taiyuan, People’s Republic of China

    Xingliang Dai & Zhizhen Ye

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Contributions

X.D. and H.L. conceived the idea and designed the experiments. X.D., J.H. and Z.Y. supervised the work. H.L. carried out the synthesis of nanocrystals, device fabrication and characterizations. Y.F. and Y.G. assisted in characterizations. M.Z., Q. Cui and Q. Cai participated in optical measurements. K.Y. and C.F. conducted the theoretical calculation. J.H. and H.H. provided helpful suggestions. X.D. and H.L. wrote the first draught of the manuscript. J.H. and Z.Y. provided major revisions. All authors discussed the results and commented on the manuscript.

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Correspondence to Xingliang Dai, Jingyun Huang or Zhizhen Ye.

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Extended data

Extended Data Fig. 1 Absorption and UPS spectra.

a, The plots of (αhν)2 versus the photon energy calculated from the absorption measurement. b, UPS spectra of the OA-QDs, DSPA-QDs, and NR-QDs: Photoemission cutoff region (left) and the valence-band-edge region (right). EVB and ECB are calculated with the formula: EVB = Ecutoff + ΔE; ECB = EVB – Eoptical bandgap. c, UPS spectra of PTAA/TAPC and PEDOT:PSS:PFI, showing photoemission cutoff region (up) and the valence-band-edge region (down).

Source data

Extended Data Fig. 2 Nanosurface reconstruction of the blue-emitting CsPbBr3 QDs.

a–c, Absorption spectra (a), PL spectra (b), and time-resolved PL decay curves (c) of the purified CsPbBr3 QDs in solution. d–f, TEM images of the OA-BQDs (d), DSPA-BQDs (e), and NR-BQDs (f), respectively. The scale bar is 50 nm. Insets show the corresponding size distribution histograms of the QDs. g, The time-dependent PL intensity trajectory of the QD films at 100 oC. h, Typical current density–voltage–luminance (J-V-L) and i, EQE–luminance (EQE-L) characteristics of the PeLEDs based on OA-BQDs, DSPA-BQDs, and NR-BQDs, respectively. The results show successful nanosurface reconstruction of the ultrasmall CsPbBr3 QDs with the improved optoelectronic properties utilizing the diisooctylphosphinic acid-mediated synthesis combined with hydrobromic acid etching.

Source data

Extended Data Fig. 3 Performance of PeLEDs based on multi-layer NR-QD films.

a, J-V-L, b, EQE–L characteristics, and c, T50 for the PeLEDs with emitter thicknesses of 5-7 nm (monolayer), 10-12 nm, 16-18 nm, and 22-25 nm, respectively. The device performance decreases following the increase of thickness of QDs emissive layers.

Source data

Extended Data Fig. 4 In-situ PL monitoring during the synthesis process.

a, Schematic diagram of the in-situ PL monitoring setup, in which 365 nm ultraviolet light is irradiated onto the sample, and the fluorescence signal is collected using a fiber-coupled spectrometer after the injection of cesium precursor. b, c Colour map of spectral evolution of the DSPA-QDs (b) and OA-QDs (c), where the arrows indicate the moment of HI injection. The DSPA-QDs show an obvious spectra blue shift after HI injection while the OA-QDs show no spectra change. Note: The in-situ measured PL spectrum shows a slight redshift compared with the PL spectrum collected in dilute QDs solution, which is caused by the reabsorption effects of the crude QDs solution with a high concentration.

Source data

Extended Data Fig. 5 XPS analysis.

High-resolution XPS spectra of (a) Pb 4 f, (b) I 3d, and (c) Cs 1 s of the DSPA-QDs, NR-QDs (TMPI), and NR-QDs (TBAI: tetrabutylammonium iodide). For the NR-QDs, the results show a slight shift of Pb 4f towards high binding energy. The core-level spectra of I 3d and Cs 1 s remain nearly identical. Surface Pb in the DSPA-QDs is nonideally coordinated compared with the NR-QDs. The iodine is bonded with Pb and oleylammonium (NH3+) in both QDs. TMPI (phosphinium iodine) was added into the purified NR-QD solution to further passivate the surface halide vacancy. We replaced TMPI with TBAI and did not observe the difference in additional bonding or electrical interaction in core-level spectra of I 3d and Cs 1s. The result suggests that a slight amount of phosphinium does not influence the chemical circumstance of iodine in the NR-QDs.

Source data

Extended Data Fig. 6 Transient absorption measurements.

Full-timescale transient absorption plots in a pseudo-colour 2D representation of the (a) OA-QDs, (b) DSPA-QDs, and (c) NR-QDs, respectively. d–f, The femtosecond transient absorption spectra of the (d) OA-QDs, (e) DSPA-QDs, and (f) NR-QDs at different delay times.

Source data

Extended Data Fig. 7 Characteristics of PeLEDs under consecutive scans.

a, J-V-L, b, EQE–L characteristics for the OA-QD-based LEDs. c, J-V-L, d, EQE–L characteristics for the DSPA-QD-based LEDs. e, J-V-L, f, EQE–L characteristics for the NR-QD-based LEDs. The peak EQEs decrease following the consecutive scans.

Source data

Extended Data Fig. 8 Ion migration activation energy measurement.

a–c, The time-dependent currents from 248 K to 298 K by applying bias at 30 V for the (a) NR-QD film, (b) DSPA-QD film, and (c) OA-QD film, respectively. d–f, The fitting data from the current decay plots of the (d) NR-QD film, (e) DSPA-QD film, and (f) OA-QD film. The τ1 is independent of temperature, which relates to the equipment response. The τ2 represents the time constant of ion migration and is used for calculating the activation energy.

Source data

Extended Data Fig. 9 Performance of the active matrix PeLED based on NR-QDs.

a, Box plot of the peak CE and peak EQE of different pixels. n = 7 independent replicates. The box plots display the median and interquartile range, with the upper whiskers extending to largest value ≤ 1.5 × interquartile range from the 75th percentile and the lower whiskers extending to the smallest values ≤ 1.5 × interquartile range from the 25th percentile. b, Operational stability of eight active matrix PeLEDs measured at all-on state, showing a half lifetime around 12-22 h.

Source data

Supplementary information

Supplementary Information

Supplementary Figs. 1–18 and Tables 1–5.

Supplementary Video 1

HI injection into the OA reaction system.

Supplementary Video 2

HI injection into the DSPA reaction system.

Supplementary Video 3

Independently controllable emission of active-matrix displays.

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Li, H., Feng, Y., Zhu, M. et al. Nanosurface-reconstructed perovskite for highly efficient and stable active-matrix light-emitting diode display. Nat. Nanotechnol. (2024). https://doi.org/10.1038/s41565-024-01652-y

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