Compositional design of spectrally stable blue mixed-halide perovskite LEDs

FENG Jiyu; LIU Min; QU Zhengguo; ZHAO Dongnan; LI Daopeng; SHI Tongfei

doi:10.7498/aps.74.20250297

Abstract

This study tackles the significant challenge of phase separation in mixed halide (Br^–/Cl^–) perovskite systems, which severely affects the spectral stability of blue perovskite light-emitting diodes (PeLEDs). A compositional engineering strategy is proposed, precisely controlling the Cs:Pb molar ratio (1∶1 to 1.1∶1) in precursor solutions to construct a CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆ composite phase structure. Transmission electron microscopy (TEM) mapping and X-ray diffraction (XRD) analysis confirm that Cs₄Pb(Br_1–xCl_x)₆ nanocrystals (5–8 nm in diameter) grow in situ and uniformly encapsulate CsPb(Br_1–xCl_x)₃ microparticles (50–100 nm). This composite architecture has double functional advantages: 1) the Cs₄PbX₆ shell acts as a physical barrier, reducing halide ion migration activation energy and suppressing phase segregation during continuous operation; 2) the wide-bandgap (3.9–4.3 eV) Cs₄PbX₆ induces quantum confinement effects, confining carriers within CsPbX₃ while passivating defect states, thereby improving perovskite performance. The optimized PeLED achieves notable improvements in brightness, external quantum efficiency, and operational stability, maintaining stable emission at 478 nm under a 50 mA/cm² current density. This is achieved by inhibiting halide phase separation and enhancing the efficiency of carrier recombination achieved by the cesium-lead halide heterojunction system. This work provides fundamental insights into phase-stable perovskite design via composite crystallization kinetics, providing a viable pathway toward commercial-grade blue PeLEDs for full-color displays.

Keywords:

Authors and contacts

1.
Institute of Physical Science and Information Technology, Anhui University, Hefei 230601, China
2.
Key Laboratory of Materials Physics, Institute of Solid State Physics (ISSP), Hefei Institute of Physical Science, Chinese Academy of Sciences, Hefei 230031, China

Corresponding author: SHI Tongfei, tfshi@issp.ac.cn

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References

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Cited By

图 1 (a) CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆钙钛矿器件的能级图; (b), (c) Cs/Pb = 1和Cs/Pb = 1.1的钙钛矿薄膜的XRD图谱; (d), (g) Cs/Pb = 1和Cs/Pb = 1.1的钙钛矿薄膜的TEM图像, 比例尺为200 nm; (e), (h) Cs/Pb = 1和Cs/Pb = 1.1的钙钛矿薄膜的TEM图像, 比例尺为50 nm; (f), (i) Cs/Pb = 1和Cs/Pb = 1.1的钙钛矿薄膜的高分辨透射电子显微镜(HRTEM)图像, 比例尺为5 nm, 其对应的快速傅里叶变换(FFT)图案显示在左上角

Figure 1. (a) Energy level diagram of the CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆ perovskite device; (b), (c) XRD patterns of perovskite films with Cs/Pb = 1 and Cs/Pb = 1.1, respectively; (d), (g) TEM images of perovskite films with Cs/Pb = 1 and Cs/Pb = 1.1, respectively, at a scale bar of 200 nm; (e), (h) TEM images of perovskite films with Cs/Pb = 1 and Cs/Pb = 1.1, respectively, at a scale bar of 50 nm; (f), (i) HRTEM images of perovskite films with Cs/Pb = 1 and Cs/Pb = 1.1, respectively, at a scale bar of 5 nm, with their corresponding fast Fourier transform (FFT) patterns shown in the upper left corner.

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图 2 混合卤化物钙钛矿化合物CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆的光致发光(PL)特性　(a) x = 0.1时的PL光谱; (b) x = 0.2时的PL光谱; (c) x = 0.3时的PL光谱; (d) x = 0.4时的PL光谱

Figure 2. Photoluminescence (PL) mixed-halide perovskite compounds CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆: (a) PL spectrum for x = 0.1; (b) PL spectrum for x = 0.2; (c) PL spectrum for x = 0.3; (d) PL spectrum for x = 0.4.

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图 3 混合卤化物钙钛矿化合物CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆在温度从290 K降至150 K时的温度依赖性光致发光(PL) 光谱　(a) x = 0.1时的PL光谱; (b) x = 0.2时的PL光谱; (c) x = 0.3时的PL光谱; (d) x = 0.4时的PL光谱

Figure 3. Temperature-dependent photoluminescence (PL) spectra of mixed-halide perovskite compounds CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆ as the temperature decreases from 290 to 150 K: (a) PL spectrum for x = 0.1; (b) PL spectrum for x = 0.2; (c) PL spectrum for x = 0.3; (d) PL spectrum for x = 0.4.

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图 4 混合卤化物钙钛矿化合物CsPb(Br_1–xCl_x)₃和CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆在电流密度为50 mA/cm²时测量的电致发光(EL)光谱　(a), (b) CsPb(Br_1–xCl_x)₃和CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆在x = 0.1时的EL光谱; (c), (d) CsPb(Br_1–xCl_x)₃和CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆在x = 0.2时的EL光谱; (e), (f) CsPb(Br_1–xCl_x)₃和CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆在x = 0.3时的EL光谱; (g), (h) CsPb(Br_1–xCl_x)₃和CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆在x = 0.4时的EL光谱

Figure 4. Electroluminescence (EL) spectra of mixed-halide perovskite compounds CsPb(Br_1–xCl_x)₃ and CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆ measured under a current density of 50 mA/cm²: (a), (b) EL spectra of CsPb(Br_1–xCl_x)₃ and CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆ at x = 0.1, respectively; (c) and (d) EL spectra of CsPb(Br_1–xCl_x)₃ and CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆ at x = 0.2, respectively; (e), (f) EL spectra of CsPb(Br_1–xCl_x)₃ and CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆ at x = 0.3, respectively; (g), (h) EL spectra of CsPb(Br_1–xCl_x)₃ and CsPb(Br_1–xCl_x)₃/Cs₄Pb(Br_1–xCl_x)₆ at x = 0.4, respectively.

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图 5 (a), (b) Cs/Pb = 1和Cs/Pb = 1.1时CsPb(Br_1–xCl_x)₃的J-V曲线; (c), (d) Cs/Pb = 1和Cs/Pb = 1.1时CsPb(Br_1–xCl_x)₃的J-L曲线; (e), (f) Cs/Pb = 1和Cs/Pb = 1.1时CsPb(Br_1–xCl_x)₃的EQE曲线; (g), (h) Cs/Pb = 1和Cs/Pb = 1.1在50 mA/cm²电流密度下CsPb(Br_1–xCl_x)₃寿命曲线

Figure 5. (a), (b) J–V curves of CsPb(Br_1–xCl_x)₃ with Cs/Pb = 1 and Cs/Pb = 1.1, respectively; (c), (d) J–L curves of CsPb(Br_1–xCl_x)₃ with Cs/Pb = 1 and Cs/Pb = 1.1, respectively; (e), (f) external quantum efficiency (EQE) curves of CsPb(Br_1–xCl_x)₃ with Cs/Pb = 1 and Cs/Pb = 1.1, respectively; (g), (h) lifetime curves of CsPb(Br_1–xCl_x)₃ with Cs/Pb = 1 and Cs/Pb = 1.1 measured at a current density of 50 mA/cm², respectively.

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