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Efficient all-thermally evaporated perovskite light-emitting diodes for active-matrix displays

Nature Photonics volume 17, pages 435–441 (2023)Cite this article

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Abstract

Perovskite light-emitting diodes (PeLEDs) have recently demonstrated great potential for next-generation displays. Fabricating PeLEDs by scalable and well-established thermal evaporation—the technique used for industrial manufacturing of organic light-emitting diodes—should accelerate the development of perovskite displays; however, thermal evaporation of perovskites produces films with a high density of defects due to fast and uncontrollable crystal growth during evaporation. As a result, the performance of evaporated PeLEDs is lagging behind their solution-processed counterparts. Here we develop a tri-source co-evaporation strategy to introduce a multifunctional Lewis-base additive that reduces the perovskite grain size while confining charge carriers and passivating surface defects. The process enables the in situ formation of high-quality perovskite nanocrystal films with improved crystallinity, enhanced photoluminescence quantum yield and suppressed defects. A peak external quantum efficiency of 16.4% is achieved for green PeLEDs with an all-thermally evaporated device architecture. We further fabricate active-matrix PeLED displays by integrating top-emitting PeLEDs on a 6.67-inch thin-film transistor backplane. The displays show high-definition images and videos with a resolution of 1,080 × 2,400 and continuous greyscale information. We anticipate that this work will stimulate the exploration of efficient vapour-deposited PeLEDs for industrial display applications.

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Fig. 1: Ligand-confined nanocrystals strategy for thermally evaporated perovskite.
Fig. 2: Characterizations of the thermally evaporated CsPbBr3 and CsPbBr3-TPPO films.
Fig. 3: Electroluminescence performance of the thermally evaporated PeLEDs.
Fig. 4: Demonstration of the AMPeLED display panel.

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The main data supporting the findings of this study are available within the article and its Supplementary Information. Additional data are available from the corresponding authors on 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 (grant nos. 61725401, 62104077, 61875211, 62050039, 62004075 and 62005089), the Fund for Innovative Research Groups of the Natural Science Foundation of Hubei Province (grant no. 2020CFA034), the Post-Doctoral Innovative Talent Support Program (grant no. BX20220119) and the Shanghai Pilot Program for Basic Research (grant no. 22JC1403200), CAS Interdisciplinary Innovation Team. We thank the Xiaomi Young Talents Program. We thank the Analytical and Testing Center of HUST and the SEM electron backscattered diffraction measurements from G. Huang at HUST. We appreciate the reaction energy calculations from H. Wang at Tianjin University, and the binding energy calculations from L. Gao and S. Liu at HUST. We thank the Wuhan Jingce Electronic Group for providing the Mura defect inspection. We appreciate helpful discussions from S. Li at Yale University and Prof. D.-W. Di and Prof. Y.-Z. Jin at Zhejiang University.

Author information

Author notes

  1. These authors contributed equally: Jinghui Li, Peipei Du, Qingxun Guo, Liang Sun.

Authors and Affiliations

  1. Wuhan National Laboratory for Optoelectronics (WNLO) and School of Optical and Electronic Information, Huazhong University of Science and Technology (HUST), Wuhan, China

    Jinghui Li, Peipei Du, Qingxun Guo, Liang Sun, Zixi Shen, Jiaxing Zhu, Chong Dong, Liang Wang, Luying Li, Bing Xia, Zewen Xiao, Boxiang Song, Jiajun Luo & Jiang Tang

  2. TCL China Star Optoelectronics Technology, Shenzhen, China

    Xin Zhang

  3. Wuhan China Star Optoelectronics Semiconductor Display Technology, Wuhan, China

    Chaoqun Yang & Jie Pan

  4. State Key Laboratory of High Field Laser Physics and CAS Center for Excellence in Ultra-Intense Laser Science, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai, China

    Zhengzheng Liu & Juan Du

  5. Optics Valley Laboratory, Wuhan, China

    Jiajun Luo & Jiang Tang

Authors
  1. Jinghui Li
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Contributions

J.T. and J. Luo supervised the whole project. J. Li, P.D. and Q.G. designed and performed most of the experiments, characterizations and analysis. L.S. designed the TFT backplanes based on requirements for display applications and was involved in the fabrication of PeLEDs and display panels. Z.S., J.Z., X.Z., C.Y. and J.P. assisted in device measurements. Z.L. and J.D. provided transient absorption measurements. Z.X. and B.X. supported the theoretical calculation and analysis. L.L., C.D. and L.W. measured the TEM and SEM. B.S. and L.S. assisted in experimental analysis. J. Luo, J. Li, P.D., Q.G. and J.T. wrote the paper. All of the authors discussed the results and commented on the paper.

Corresponding authors

Correspondence to Jiajun Luo or Jiang Tang.

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Nature Photonics thanks Michele Saba, Jun Xing and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Extended data

Extended Data Fig. 1 Features of thermally evaporated PeLEDs and reaction coordinate diagram for vapour-deposited CsPbBr3 film.

a, Comparisons between thermally evaporated and spin-coated PeLED. Thermally evaporated PeLED enjoys significant advantages in pixelation, large-area, mass fabrication, and industry compatibility; and the only bottleneck is relatively low device efficiency. b, Reaction coordinate diagram of CsPbBr3 crystal formation by thermal co-evaporation of CsBr and PbBr2. The released energy of the reaction between gaseous CsBr and PbBr2 molecules is calculated to be 385.8 kJ·mol−1, far beyond that of the reaction between solid-state CsBr and PbBr2 (28.9 kJ·mol−1).

Extended Data Fig. 2 Understanding the interaction between TPPO and CsPbBr3.

a, Density functional theory calculation: TPPO binding with the unsaturated lead at the perovskite edge through P = O:Pb. The binding energy is 0.73 eV with a bond length of 2.4 Å. b, Calculated binding energy between CsPbBr3 and different Lewis-base additives (TPPO, TPPS: triphenylphosphine sulfide, and TPMM: triphenylmethyl mercaptan) with lone pair electrons. c, Calculated density of state for CsPbBr3 and CsPbBr3-TPPO. The red region represents the density of the passivated defect state. The calculated density of states (DOS) indicates that TPPO could act as an electron-pair donor to bind with the unsaturated lead dangling bonds, and thus eliminate the trap states that existed in the band edge of CsPbBr3, inhibiting the trap-assisted non-radiative recombination processes. d, Fourier transform infrared (FTIR) spectra of thermally evaporated pure TPPO, PbBr2-TPPO, CsPbBr3-TPPO, and CsPbBr3 films. The infrared peak at 1192 cm−1 of TPPO arises from the P = O stretching vibration, and shifts to 1185 cm−1 in the case of PbBr2-TPPO and CsPbBr3-TPPO, confirming the chemical bonding of P = O:Pb. e, Pb 4 f core-level XPS spectra of CsPbBr3 and CsPbBr3-TPPO films. Once again, the shift of XPS spectrum for TPPO-incorporated film confirms the chemical bonding of P = O:Pb. f, Photoluminescence spectra of the perovskite films with various TPPO contents. For instance, 40% TPPO represents the deposition rates ratio of TPPO/CsPbBr3 40%.

Source data

Extended Data Fig. 3 XRD and transient absorption spectra of thermally evaporated CsPbBr3 and CsPbBr3-TPPO films.

a, XRD patterns for CsPbBr3 and CsPbBr3-TPPO films. CsPbBr3-TPPO exhibits improved crystallinity and orientation. b, The shifts of bleach peak wavelength over time. c, Initial PL intensity (IPL) as a function of carrier density. The IPL shows a quadratic dependence with carrier density for both CsPbBr3 and CsPbBr3-TPPO films, which reveals that the carriers’ radiative recombination process is bimolecular, conforming to the free carrier semiconductor characteristics. d-e, TA bleaching kinetics at emission peaks monitored under various initial carrier densities for CsPbBr3 and CsPbBr3-TPPO films, respectively. Time zero for different TA decay is shifted to overlay absolute values with the respective next higher initial carrier density (marked with different symbols). f, Squares represent the perovskite film’s PLQYs measured under 400 nm pulse excitation as a function of carrier density, and lines represent the predicted radiative efficiency η from the recombination rate model. Carrier density is estimated from the pump power absorption of the perovskite films (details see Method).

Source data

Extended Data Fig. 4 Optimization and evaluation of CsPbBr3-TPPO based PeLEDs.

a, Current density-voltage curves of hole-only (ITO/MoO3/NPB/CsPbBr3-TPPO/NPB/MoO3/Al) and electron-only (ITO/LiF/TPBi/CsPbBr3-TPPO/TPBi/LiF/Al) devices. The thicknesses of NPB, CsPbBr3-TPPO, TPBi, and Al layers are 50, 50, 40, and 80 nm, respectively. b, Histogram of peak EQEs of CsPbBr3-TPPO based PeLEDs. c, PL and EL spectra of CsPbBr3-TPPO based device.

Source data

Extended Data Fig. 5 Optical and electrical characteristics of 12 nm Mg:Ag electrodes with various molar ratios.

a, Structure diagram of top-emitting PeLED. b, Transmission spectra of Mg:Ag electrodes. c, d, Current density−voltage and luminance−voltage curves of top-emitting PeLEDs based on different Mg:Ag electrodes. The work functions of Ag, Mg:Ag (1:20 mol%), Mg:Ag (1:10 mol%), and Mg:Ag (1:5 mol%) electrodes are 4.50 eV, 4.30 eV, 4.14 eV, and 4.02 eV, respectively.

Source data

Extended Data Fig. 6 Microscopy images of the AMPeLED display panel and its working mechanism.

a–c, Top-view microscopy images of the fabricated perovskites characterized by the SEM, ordinary microscope, and fluorescence microscope. d, The driving circuit and its operating timing. Each pixel drive circuit consists of 7 TFTs and a capacitor, namely 7T1C. The operating timing of the driver circuit consists of three main parts, namely reset, writing-in and emitting. In each frame, T1 and T6 are reset first (region I), then the potential signal from the Data line is written to the gate of T1, the main drive TFT (region II). In the final emission region III, T5 and T6 are switched on to realize the current flowing through the PeLED to emit light. The current could be precisely controlled by the gate potential of T1. Voltage drain-to-drain (VDD) and Voltage source-to-source (VSS) are connected to the anode and cathode of the power source to provide stable positive and negative voltage for the TFTs and LEDs. In this panel, VDD and VSS are set to 4.6 V and −3.5 V, respectively.

Extended Data Fig. 7 Mura inspection and luminance measurements for the AMPeLED display panel.

a, The luminance of five selected spots (A-E) on the AMPeLED display panel. Five spots (A-E, 1 mm in diameter) were selected to measure the luminance (43% aperture ratio) with the assistance of PR655 SpectraScan, and the results demonstrated a uniform luminance distribution with negligible fluctuation. Note that the display panel was driven using a pattern generator controlled by computer software, in which VDD and VSS were set at 4.6 and −3.5 V, respectively. b, The Mura inspection of a bright rectangular area (6.88 × 11.62 cm) on the AMPeLED display panel by a CCD imaging luminance meter camera. c, An area with 62700 pixels was extracted to evaluate the pixel yield of the AMPeLED display panel. The pixel yield was defined as the area proportion of pixels without visual defects. The extracted area is about 1.21 × 2.13 cm, and the scale bar is 5 mm.

Source data

Extended Data Fig. 8 Hypothetical hybrid display panel of green PeLEDs and commercial blue/red OLEDs.

a, A potential approach for the realization of the future full-color display by combing green PeLED pixels with red and blue OLED pixels. b, EL spectra of green PeLED and commercial blue/red OLEDs. c, The color gamut of the resulting hybrid display panel and its comparison with the NTSC standard.

Source data

Extended Data Table 1 PLQYmax, monomolecular (k1), bimolecular (k2), and trimolecular (k3) coefficients of vapor-deposited CsPbBr3 and CsPbBr3-TPPO films
Full size table
Extended Data Table 2 Performance of the reported perovskite LEDs towards display application
Full size table

Supplementary information

Supplementary Information

Supplementary Figs. 1–6, Discussion and Tables 1–4.

Active-matrix PeLED displays with rich greyscale information.

Active-matrix PeLED displays with pin-sharp quality.

Supplementary Data 1

A single file containing all Supplementary Data.

Source data

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Li, J., Du, P., Guo, Q. et al. Efficient all-thermally evaporated perovskite light-emitting diodes for active-matrix displays. Nat. Photon. 17, 435–441 (2023). https://doi.org/10.1038/s41566-023-01177-1

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