钙钛矿组分和结构设计及其发光二极管器件性能研究进展

doi:10.6023/A20100463

摘要/Abstract

有机-无机杂化钙钛矿发光二极管(LED)的性能在短短几年时间内飞速提升, 近红外光器件的效率已达21.6%, 绿光器件效率也达到20.3%, 达到可以和商业化的有机发光二极管媲美的水平; 即使是稍有逊色的稳定性方面也有很大进展, 报道的最长器件半衰期已达到250 h. 器件性能的飞速提升得益于钙钛矿本身优异的光电性质, 而且通过丰富的化学手段可进一步对钙钛矿材料的组分和结构进行调控, 从而优化器件性能. 本综述从组分设计、缺陷钝化和界面修饰的角度出发, 重点分析了组分和结构设计对钙钛矿LED器件效率和稳定性的影响, 最后对钙钛矿发光二极管的未来发展进行展望.

关键词: 钙钛矿, 发光二极管, 组分设计, 缺陷钝化, 界面修饰

Over the past few years, the external quantum efficiency (EQE) of organic-inorganic hybrid perovskite light-emitting diodes (LEDs) has experienced a tremendous progress. The reported highest EQE of infrared and green perovskite LEDs has reached 21.6% and 20.3%, respectively, which is comparable to commercial organic light-emitting diodes. Even the slightly inferior blue perovskite LEDs have a recorded EQE of 12.3%. However, poor device stability is the biggest problem hindering the commercial application of perovskite optoelectronic devices, which is a severer problem in LEDs because the higher operating voltage will trigger acute ion migration. Encouragingly, however, the lifetime of perovskite LEDs has increased from the initial several seconds to over 200 hours, presenting a dramatic progress. The outstanding performance of perovskite LEDs is closely related with the excellent material properties, including tunable bandgaps, narrow full width at half maximum (FWHM), high defect tolerance, high electron/hole mobility and solution processibility. Moreover, the diversity of components and structure of perovskite makes the addition of various additives effective, enabling optimizing device performance through kinds of chemical methods. In this review, we analyzed the impacts of component and structure designing on the efficiency and stability of perovskite LEDs from the perspective of compositional designing, defect passivation and interfacial modification. We analyzed how compositional designing affects the optoelectronic properties through altering the ratio between organic and inorganic components or adding other molecules and ions to adjust the dimension of perovskites. As for defect passivation, we discussed various passivating reagents and their working mechanism. In addition, we summarized the significance of interfacial modification between different functional layers, including improving the wetting property of the substrates, achieving higher crystal quality of perovskite films, passivating the defects at the interfaces, blocking leakage current and reducing hole/electron injecting barrier. Finally, we discussed the scientific and technological challenges yet to be resolved before perovskite LEDs can be considered for commercial applications.

Key words: perovskite, light-emitting-diodes, compositional design, defect passivation, interfacial modification

引用此文

郭镇域, 周欢萍. 钙钛矿组分和结构设计及其发光二极管器件性能研究进展[J]. 化学学报, 2021, 79(3): 223-237.

Zhenyu Guo, Huanping Zhou. Research Progress of Composition and Structure Design in Perovskites for High Performance Light-emitting Diodes[J]. Acta Chimica Sinica, 2021, 79(3): 223-237.

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图/表 14

图1. (a) 常见钙钛矿LEDs器件结构[21]; (b) 不同类型的钙钛矿材料和电子、空穴传输层材料的能级图[23-26]

Figure 1. (a) Common perovskite LEDs device configurations[21]; (b) energy-level diagram of different kinds of perovskite and electron/hole transport layers[23-26]

图2. MAPbI3中各类点缺陷的计算能级位置和相应的形成能[27]

Figure 2. Calculated transition energy levels and formation energies of point defects in MAPbI3[27]

图3. (a) 过量的MABr抑制金属Pb对激子的猝灭[33]; (b) 不同MABr含量对钙钛矿结晶和载流子复合过程的影响[34]; (c) 钙钛矿在不同基底上的结晶过程[36]

Figure 3. (a) Stoichiometry control using excess MABr to prevent exciton quenching from metallic Pb atoms[33]; (b) effect of different MABr content on the crystallization and carrier recombination process of perovskite[34]; (c) crystallization of perovskite on different substrates[36]

钙钛矿组分	最佳物质的量比	LED器件性能	参考文献
CsPbBr₃	CsBr/PbBr₂=2	L_max=407 cd·m^–2 CE_max=0.035 cd·A^–1	^[38]
CsPbBr₃	CsBr/PbBr₂=1.5	L_max=23828 cd·m^–2 CE_max=9.54 cd·A^–1	^[39]
CsPbBr₃	CsBr/PbBr₂=1.1	L_max=13752 cd·m^–2 CE_max=5.39 cd·A^–1	^[37]
FAPbBr₃	FABr/PbBr₂=2	L_max=109000 cd·m^–2 CE_max=21.3 cd·A^–1 EQE_max=4.66%	^[40]
MAPbBr₃	MABr/PbBr₂=3	L_max=6950 cd·m^–2 CE_max=34.46 cd·A^–2 EQE_max=8.21%	^[34]
FAPbI₃	FAI/PbI₂=2.4	EQE_max=20.7% ECE@100 mA·cm^–2=12%^a	^[14]
FAPbI₃	FAI/PbI₂=2	EQE_max=14.2% CE_max=10.7%	^[41]
(FACs)PbI₃	(FACs)I/PbI₂=2.5	EQE_max=19.6%	^[36]

表1. 三维钙钛矿LED器件中钙钛矿组分调控和性能参数

Table 1. Composition control and performance parameters in three-dimensional perovskite LED devices

图4. (a) 准二维钙钛矿中不同n值相的结构单元, 表示从二维(n=1)到三维(n=∞)的变化; (b) 多相钙钛矿在不均匀能级分布中的能量传输过程, 将载流子集中到带隙最小的发光相. 箭头代表载流子的转移过程[29]

Figure 4. (a) Unit cell structure of Quasi-2D perovskites with different ?n? values, showing the evolution of dimensionality from 2D (n=1) to 3D (n=∞); (b) multi-phase perovskite materials channel energy across an inhomogeneous energy landscape, concentrating carriers to smallest bandgap emitters. The arrows represent the carrier transfer process[29]

图5. (a)不同n值的准二维钙钛矿薄膜(PEA2(FAPbBr3)n-1PbBr4)在紫外灯照射下的荧光图片[25]; (b) n=1的二维钙钛矿(PEA2PbBr4)薄膜、MA基(PEA2(MAPbBr3)2PbBr4)、FA基(PEA2(FAPbBr3)2PbBr4)的准二维钙钛矿薄膜的X射线衍射(XRD)图; (c) n=1的相、MA基、FA基的准二维钙钛矿与载流子传输层的能级排布[46]

Figure 5. (a) Photoluminescence image of PEA2(FAPbBr3)n-1PbBr4 films with different compositions under ultraviolet lamp excitation[25]; (b) X-ray diffraction (XRD) patterns of the n=1 phase film (PEA2PbBr4), the MA-based PEA2(MAPbBr3)2PbBr4 film, and the FA-based PEA2(FAPbBr3)2PbBr4 film; (c) band alignment of the n=1 phase, MA-based and FA-based perovskites compared with the hole and electron injection layer materials[46]

图6. (a)不同大阳离子体系的准二维钙钛矿中的能量转移过程[55]; (b)不同大阳离子的锡基钙钛矿LED器件性能曲线[57]; (c)不同有机阳离子对钙钛矿有机插层宽度的影响示意图[58]

Figure 6. (a) Energy transfer mechanism in quasi-two-dimensional perovskite with different spacer molecules[55]; (b) EQE characteristics for Sn-based perovskite LED devices with different spacer molecules[57]; (c) schematic representation of the barrier width of perovskite films with various organic cations[58]

图7. (a) 低维钙钛矿组分工程示意图[52]; (b) 含有PEA或PEA+NPA的钙钛矿膜中的异相扩散示意图[60]; (c) PEABr和NPABr2分子结构[60]

Figure 7. (a) Schematic diagram of low-dimensional perovskite components engineering[52]; (b) schematic diagram of different phase diffusion between two perovskite films with PEA or PEA+NPA[60]; (c) molecule structures of PEABr and NPABr2[60]

图8. (a) 在MAPbBr3中引入EA阳离子对Pb 6p和(Pb 6s-Br 4p)*轨道能量的影响示意图[66]; (b) 用烷基胺和芳香胺对CsPbBr3量子点进行阴离子交换的示意图(OAM-I, 烷基胺氢碘酸盐; An-HI, 芳香胺氢碘酸盐)[67]

Figure 8. (a) Schematic representation of variation of energy levels of MAPbBr3 in Pb 6p and (Pb 6s-Br 4p)* orbitals on insertion of EA cation[66]; (b) scheme of anion-exchange of synthesized pristine CsPbBr3 perovskite QDs using long alkyl ammonium and aryl ammonium. OAM-I, alkyl ammonium; An-HI, aryl ammonium[67]

图9. (a) CsPbBr3量子点表面的配体交换机理[72]; (b) CsPbBr3量子点表面配体密度和相应的分散液稳定性、PLQY和载流子注入能力[73]; (c) 不同配体策略的量子点的PLQY随储存时间的变化[75]

Figure 9. (a) The ligand-exchange mechanism on CsPbBr3 QD surfaces[72]; (b) schematic illustration of the control of ligand density on CsPbBr3 QD surfaces and the corresponding changes of ink stability, PLQY and carrier injection[73]; (c) PLQY variation of the above corresponding samples after different storage times[75]

图10. (a) 5AVA在氧化锌表面的反应以及构型示意图[14]; (b) 钝化分子结构[5]

Figure 10. (a) Dehydration reaction of 5AVA on top of the ZnO-PEIE surface and configuration of 5AVA on the ZnO surface[14]; (b) the molecular structure of passivating moleculars[5]

图11. (a) 钝化前后封装的钙钛矿LEDs在环境条件下归一化的亮度随器件工作时间的变化[97]; (b)初始亮度为4000 cd·m–2的条件下, 未处理的和边缘稳定的钙钛矿LED器件操作稳定性曲线[100]

Figure 11. (a) Normalized luminances of encapsulated PeLEDs with and without passivation under ambient conditions as functions of operation time[97]; (b) operational device stability of untreated controls and edge-stabilized perovskite LEDs at a starting luminance of 4000 cd· m–2 [100]

图12. (a) 过量卤素离子对卤素空位缺陷的调控的截面示意图, K+离子在晶界和表面与卤素形成良性的化合物, 固定了过剩的卤素[89]; (b) CsPbBr3钙钛矿薄膜表面卤素空位缺陷和无机分子LiBr钝化示意图[103]; (c) 富KBr的表面钝化抑制离子迁移示意图[104]

Figure 12. (a) Schematic of a cross-section of a film showing halide-vacancy management in cases of excess halide, in which the surplus halide is immobilized through complexing with potassium into benign compounds at the grain boundaries and surfaces[89]; (b) a schematic depicting the surface halide vacancies of CsPbBr3 perovskite films and passivated by inorganic molecules of LiBr[103]; (c) illustration of ion migration suppressed by KBr-enriched surface passivation[104]

图13. (a) D4TBP分子对不同缺陷位点的钝化机理示意图[106]; (b) 有无PEAI层的钙钛矿LED器件的工作稳定性[107]; (c) FPMATFA有机盐对钙钛矿晶界的缺陷钝化示意图[108]

Figure 13. (a) Schematic illustration of the origin of D4TBP passivation effect on different defect sites[106]; (b) operated stability of the PeLED devices with and without PEAI layer[107]; (c) schematic illustration of defect passivation at perovskite grain boundaries by FPMATFA[108]

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