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Research Article

Multi-site anchoring lead-halide octahedral by benzylphosphonic acid to regulate phase distribution for efficient PeLEDs

Jiahao Tang1,§, Yifei Wang1,§, Hengyang Xiang1( ), Run Wang1, Kun Zhang1, Xinyi Lv1, Xinrui Chen1, Ziqing Xu1, Zhesheng Chen1, Lei Wang2( ), Aidi Zhang3, An Xie4( ), Haibo Zeng1( )
MIIT Key Laboratory of Advanced Display Materials and Devices, Institute of Optoelectronics and Nanomaterials, College of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, China
Engineering Research Center of Functional Polymer Membrane Materials of Jiangsu Province, Nanjing Bready Advanced Materials Technology Co., Ltd., Nanjing 211103, China
School of Materials Science and Engineering, Xiamen University of Technology, Xiamen 361024, China

§ Jiahao Tang and Yifei Wang contributed equally to this work.

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Graphical Abstract

This paper reveals that benzylphosphonic acid (BPA) contains multi-sites of P=O and P–OH, which can attract and anchor PEA+/Pb2+ to sufficient nucleation-growth during perovskite film formation. This interaction inhibits the formation of low phases (n = 1), promotes the development of a continuous intermediate phase characterized by n ≥ 2 phases, and facilitates the unimpeded transfer of energy from the low-n phase to the high-n phase. Subsequently, the optimized green device exhibits a maximum external quantum efficiency (EQE) of 20.6% and a maximum luminance of 24,352 cd/m2.

Abstract

Quasi-two-dimensional perovskite light-emitting diodes (quasi-2D PeLEDs) are emerging as high-potential candidates for new generation of wide-color gamut displays due to their simple, low-cost solution process, and high color purity. However, the luminescence performance of quasi-2D perovskite films is severely limited by dispersed phase distribution and excessive defect density, which are caused by excessive diffusion of nucleation sites during the perovskite growth stage. Here, the benzylphosphonic acid (BPA) molecule, owing to its strong P–O–Pb bond energy sites and strong electronegativity to PEA+, can aggregate lead-halide octahedron to grow high-dimensional phases, avoiding scattered low-dimensional phases (n = 1). The continuous gradient phase distribution will be beneficial to smooth carrier injection and effectively suppress the leakage current in PeLEDs. Meanwhile, the introduction of phosphonic acid groups will fill the vacancies of Pb ions and reduce non-radiative recombination. As a result, the maximum external quantum efficiency (EQE) of PeLEDs can be increased from 8% to 20.6% with a 514 nm light emission and a 21 nm full-width half maximum, and the device lifetime (T50) is nearly 6-fold of the pristine sample. In addition, this strategy is also suitable for other wavelength. For example, in blue light, performance improvement is also realized that the maximum EQE of 8% and the luminance increased from 1045 to 5264 cd/m2. These results provide a feasible strategy to regulate the phase distribution and passivate the defects of quasi-2D perovskites.

Keywords

quasi-2D perovskiteslight-emitting diodesbenzylphosphonic acidphase distributiondefect passivation

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Nano Research
Volume 17 Issue 11,
November 2024
Pages 10034-10041
DOI: 10.1007/s12274-024-6914-9
Cite this article:
Tang J, Wang Y, Xiang H, et al. Multi-site anchoring lead-halide octahedral by benzylphosphonic acid to regulate phase distribution for efficient PeLEDs. Nano Research, 2024, 17(11): 10034-10041. https://doi.org/10.1007/s12274-024-6914-9
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Received: 24 June 2024
Revised: 25 July 2024
Accepted: 25 July 2024
Published: 21 August 2024
© Tsinghua University Press 2024
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