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金属卤化物钙钛矿材料由于具有高的光致发光量子产率、高色纯度、带隙可调等杰出的光学性能, 被作为发光材料广泛地用于制备钙钛矿电致发光二极管(perovskite light-emitting diodes, PeLEDs). 虽然取得了较好的研究进展, 但是其效率和稳定性还未达到商业化的要求, 还需要进一步提高. 为了提高PeLEDs的效率和稳定性, 本文使用旋涂法, 引入了一种具有宽带隙和较好空穴传输能力的有机小分子材料4,4′-cyclohexylidenebis [N,N-bis (p-tolyl) aniline] (TAPC) 作为激子阻挡层, 获得了效率和寿命都得到提高的全无机PeLEDs. 研究表明, PeLEDs效率和寿命得到提高的物理机制主要源于两方面: 1) TAPC具有恰当的最高占有分子轨道能级, 与PEDOT:PSS的最高占有分子轨道能级和CsPbBr3的价带边形成了阶梯式能级分布, 有利于空穴注入和传输; 同时TAPC具有较高的最低未占分子轨道能级, 能够有效地阻止电子泄漏到阳极端, 并能很好地将电子和激子限制在发光层内; 2) TAPC层的引入可以避免钙钛矿发光层与强酸性的空穴注入材料Poly(3,4-ethylenedioxythiophene):poly(p-styrene sulfonate) (PEDOT:PSS)的直接接触, 进而免除钙钛矿发光层由于与PEDOT: PSS的直接接触所导致的激子淬灭, 从而提高了激子的发光辐射复合率.In recent years, metal halide perovskite materials, owing to their excellent photoelectric properties including high photoluminescence quantum yield, high color purity, tunable band gap, etc., have been regarded as new-generation lighting sources and are widely used to fabricate perovskite light-emitting diodes (PeLEDs). Though great progresses have been made in recent years, neither the efficiency nor stability has not yet reached the requirements of commercialization. Thus, further improvement is needed. In this work, a small organic molecule material, namely 4,4'-cyclohexylidenebis[N,N-bis(p-tolyl)aniline] (TAPC) with a wide bandgap and a good hole transport ability, is used as an exciton blocking layer by utilizing the spin-coating method to improve the stability and efficiency of PeLEDs. Highly efficient and stable CsPbBr3 PeLEDs are finally realized. The physical mechanism related to the improved electroluminescence performance is investigated thoroughly. Firstly, the stepped energy level alignment is formed, since the highest occupied molecular orbital energy level (HOMO) of TAPC is located between the HOMO of (3,4-ethylenedioxythiophene):poly(p-styrene sulfonate) (PEDOT: PSS) and the valence band of CsPbBr3, which is beneficial to hole injection and transport. Meanwhile, the lowest unoccupied molecular orbital level of TAPC is high enough to prevent electrons from leaking into the anode effectively and confine electrons and excitons well in the emitting layer. Secondly, the introduction of the TAPC layer can avoid the direct contact between the perovskite light emitting layer and the strong acidic layer of PEDOT:PSS, thereby eliminating the related excitons quenching, which can further increase the radiative recombination.
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Keywords:
- all inorganic halide perovskite /
- electroluminescent diodes /
- hole transport /
- exciton quenching /
- exciton blocking layer
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图 1 (a) PeLEDs的器件结构; (b) PeLEDs的能级图
Fig. 1. (a) Device structure of PeLEDs; (b) schematic energy level diagram of PeLEDs.
图 2 PeLEDs的EL性能表征 (a)电流密度-电压; (b)亮度-电压; (c)电流效率-电压-外量子效率; (d) PeLEDs (TAPC浓度为5 mg/mL)在不同电压下的EL光谱, 内插图是不同TAPC浓度的PeLEDs在电压为5 V时的归一化EL谱
Fig. 2. EL performance of PeLEDs: (a) Current density-voltage (J-V); (b) luminance-voltage (L-V); (c) current-efficiency-voltage-external quantum efficiency (CE-V-EQE); (d) EL spectra of PeLEDs with 5 mg/mL TAPC at different applied voltages; the inset is normalized EL spectra of PeLEDs with different concentrations of TAPC at the same applied voltage of 5 V.
图 4 (a) ITO/PEDOT:PSS/CsPbBr3和(b) ITO/PEDOT:PSS/TAPC/CsPbBr3样品的SEM图; (c) ITO/PEDOT:PSS/CsPbBr3和(d) ITO/PEDOT:PSS/TAPC/CsPbBr3样品的CsPbBr3颗粒尺寸统计分布
Fig. 4. SEM images of (a) ITO/PEDOT:PSS/CsPbBr3 and (b) ITO/PEDOT:PSS/TAPC/CsPbBr3; the size distribution of CsPbBr3 grain on (c) ITO/PEDOT:PSS/CsPbBr3 and (d) ITO/PEDOT:PSS/TAPC/CsPbBr3.
图 5 在PEDOT:PSS和PEDOT:PSS/TAPC衬底上的CsPbBr3薄膜的表征 (a)晶体结构(XRD); (b)紫外吸收, 内插图是在500−518 nm波长范围吸收的放大图; (c) PL光谱, 内插图是在520−535 nm波长范围PL的放大图; (d) TRPL曲线
Fig. 5. Characteristics of CsPbBr3 film on PEDOT:PSS and PEDOT:PSS/TAPC: (a) XRD; (b) absorption, and the inset is a large image of normalized PL spectra from 500 to 518 nm; (c) normalized PL spectra, and the inset is a large image of normalized PL spectra from 520 to 535 nm; (d) TRPL decay curves.
图 6 单空穴器件的电流密度-电压特性曲线
Fig. 6. Current density-voltage characteristics of hole-dominated devices.
图 7 激子界面复合效应 (a) PEDOT:PSS/CsPbBr3; (b) PEDOT:PSS/TAPC/CsPbBr3
Fig. 7. Exciton recombination interface effects: (a) PEDOT: PSS/TAPC/CsPbBr3; (b) PEDOT:PSS/CsPbBr3.
表 1 PeLEDs性能
Table 1. List of EL performance of PeLEDs.
器件 TAPC浓度/mg·mL–1 最大亮度/cd·m–2 最大电流效率/cd·A–1 外量子效率/% 色坐标(x, y) A 0 2396 1.81 0.47 (0.13, 0.80) B 2 6081 4.52 1.17 (0.13, 0.80) C 5 13198 6.84 1.77 (0.13, 0.80) D 8 3678 1.13 0.29 (0.13, 0.80) 
下载: 导出CSV
表 2 瞬态荧光寿命参数统计列表
Table 2. List of TRPL parameters.
Films B1/% B2/% τ1/ns τ2/ns τave/ns PEDOT:PSS/CsPbBr3 79 21 4.86 210.45 47.44 PEDOT:PSS/TAPC/CsPbBr3 75 25 5.72 212.65 57.64
下载: 导出CSV
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