Research Progress of Composition and Structure Design in Perovskites for High Performance Light-emitting Diodes

doi:10.6023/A20100463

Abstract

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

Cite this article

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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Fig. & Tab. 14

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]

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

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]

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

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]

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]

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]

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]

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]

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]

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]

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]

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]

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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