钙钛矿发光二极管光提取性能增强的研究进展

陈佳楣; 苏杭; 李婉; 张立来; 索鑫磊; 钦敬; 朱坤; 李国龙

doi:10.7498/aps.69.20200755

摘要

钙钛矿发光二极管具有色纯度高, 发光层材料带隙可调等优点, 目前其外量子效率已经超过20%, 在平板显示和照明领域有很好的商业化前景. 然而, 同有机发光二极管类似, 钙钛矿发光二极管同样存在衬底模式、表面等离子体模式、波导模式引起的内部损耗问题, 在一定程度上限制了钙钛矿发光二极管的性能提升. 因此, 需要优化器件的材料和几何结构以获得更好的膜间光学导纳匹配, 改善钙钛矿发光二极管光提取效率以增强器件的发光性能. 当前, 通过改变电极材料、增加等离子体激元、引入微纳结构以及优化钙钛矿薄膜和器件结构, 可以增强钙钛矿发光二极管光提取效率, 通过增强光提取效率后的钙钛矿发光二极管外量子效率可达 28.2%, 电流效率可达88.7 cd/A. 本文针对钙钛矿发光二极管材料与结构的改变, 从以上四个方面进行重点阐述. 此外, 进一步分析了这四种方法在提升器件光提取效率方面存在的优点和面临的问题, 从而为钙钛矿发光二极管的制备和优化提供一定的借鉴.

关键词:

钙钛矿 /
发光二极管 /
光提取 /
效率

Abstract

Perovskite light emitting diodes (PeLEDs) have developed rapidly in recent years due to their advantages of tenability of band gap and high color purity. At present, the external quantum efficiency of PeLED has rised up to 20%. Like the scenario of organic light emitting diode, there exist various internal losses in PeLED with low light extraction efficiency. It arises from the absorption of substrates, waveguide transmission and surface plasmon resonance of metal electrode. To improve the luminescence performance of PeLED, a well-matched optical admittance between the thin-films inside the devices is required. In this paper, the strategies of enhancing the light extraction efficiency are adopted as the materials and structures in PeLED are concerned. The applications of alternative electrode in PeLED are discussed, such as graphene, silver nanowires, metal transparent electrode and some new-types of electrodes. In addition, the plasma effect is also introduced into the PeLED to deflect the emitting light. What is more, the nano-structure grating is inserted into device to reduce the optical losses due to the large refractive index difference between the interfaces in device. Therefore, the external quantum efficiency of PeLED rises up to 28.2%, and the current efficiency can reach 88.7 cd/A.

Keywords:

作者及机构信息

宁夏大学, 宁夏光伏材料重点实验室, 银川　750021

通信作者: 李国龙, liglo@163.com

基金项目: 宁夏自然科学基金(批准号: 2019AAC03001)资助的课题

Authors and contacts

Key Laboratory of Ningxia for Photovoltaic Materials, Ningxia University, Yinchuan 750021, China

Corresponding author: Li Guo-Long, liglo@163.com

Funds: Project supported by the National Natural Science Foundation of Ningxia, China (Grant No. 2019AAC03001)

文章全文

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施引文献

图 1 (a) PeLED器件中的光耦合损耗; (b)光在介质与空气界面的光学路径(垂直入射、折射、全反射)^[19,20]

Fig. 1. (a) Various kinds of light out-coupling losses in LEDs; (b) optical path of light at the interface between medium and air (vertical incidence, refringence, total reflection)^[19,20].

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图 2 基于CsPbI₃纳米晶的PeLED的器件结构示意图, 基底分别为ITO和Ag, 其中红色箭头表明该端电极为透明且为出光面^[26]

Fig. 2. Schematic diagram of the CsPbI₃ nanocrystal-based LED with ITO and Ag bottom cathodes. Red arrows indicate on which side the respective devices are transparent and emit light^[26].

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图 3 分别采用ITO和Au电极的PeLED　(a)能级结构排列图; (b)电压-电流效率图^[27]

Fig. 3. PeLED with ITO and ultrathin Au electrode: (a) Energy band structure; (b) current efficiency-voltage curves^[27].

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图 4 PeLED电极为ZnO-Ag-ZnO结构:　(a) ZnO-Ag-ZnO结构示意图: 底部为ZnO, 中间为Ag层, 顶部为ZnO层; (b)电极分别为ITO和m-ZnO-Ag-ZnO的器件电压-电流效率图(插图显示了在5 V条件下器件的辐射性)^[28]

Fig. 4. PeLED with ZnO-Ag-ZnO electrode: (a) ZnO-Ag-ZnO structure: bottom wetting ZnO layer, middle patterned Ag layer and top continuous ZnO layer; (b) current efficiency-voltage curves with ITO and ZnO-Ag-ZnO electrode (insets show the magnified view of emission uniformity on 5 V)^[28].

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图 5 阳极为AnoHIL的PeLED器件　(a)能级结构排列图; (b) PeLED 为不同电极的电压-外量子效率曲线^[29]

Fig. 5. PeLEDs with AnoHIL anode: (a) Energy band diagram; (b) voltage-EQE curves of PeLEDs fabricated on various anodes^[29].

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图 6 掺杂Ag纳米棒的PeLED的透射电子显微镜截面图及器件结构示意图^[33]

Fig. 6. Transmission electron microscope image of cross section and schematic diagram of device structure for PeLED with Ag nanorods^[33].

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图 7 FDTD模拟Au-Ag NP的电磁场分布^[35]

Fig. 7. FDTD simulation of the electromagnetic field distributed around the Au-Ag NP^[35].

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图 8 基于MAPbI₃的PeLED　(a)光栅在PEDOT:PSS/ITO衬底上的实像; (b)电流密度-辐射特性曲线; (c)电压-外量子效率曲线^[36]

Fig. 8. PeLED based on MAPbI₃: (a) Real image of grating on PEDOT:PSS/ITO substrate; (b) the curves of current density-radiance characteristics; (c) the curves of voltage-EQE^[36].

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图 9 PeLED带有纳米孔阵列、有机传输层的分子结构以及该结构的扫描电子显微镜^[37]

Fig. 9. Device structure of PeLEDs with NHA, the molecular structure of organic transportin layers, and scanning electron microscope images of the structure^[37].

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图 10 带有AAM结构的PeLED　(a)器件结构示意图; (b) PeLED带有ND, NW结构的电场强度; (c) PeLED带有ND结构的电场强度^[38]

Fig. 10. PeLED with AAM structure: (a) Device schematic; (b) electric field intensity of PeLED with ND, NW structure; (c) electric field intensity of PeLED with ND structure^[38].

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图 11 基于CsPbBr₃的PeLED压印纳米结构制备过程^[12]

Fig. 11. Fabrication process of a CsPbBr₃ PeLED with the imprinted nanostructures^[12].

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图 12 钙钛矿发光层为亚微米结构的PeLED结构示意图, 光线A, B, C表示光线原先束缚于发射层中, 通过亚微米结构进行光提取^[11]

Fig. 12. Device schematic with submicrometre structure. Rays A, B and C, which represent light trapped in devices with a continuous emitting layer, can be extracted by the submicrometre structure^[11].

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图 13 在厚度不同的钙钛矿发光层条件下外量子效率和电流密度的关系图, 钙钛矿发光层材料分别为(a) MAPbI₃, (b) Cs_0.2FA_0.8PbI_2.8Br_0.2, (c) FAPbI₃, (d) FAPbBr₃^[39]

Fig. 13. EQE vs. current density of PLEDs based on (a) MAPbI₃, (b) Cs_0.2FA_0.8PbI_2.8Br_0.2, (c) FAPbI₃, (d) FAPbBr₃ thin films with various thicknesses^[39].

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表 1 PeLEDs光提取研究进展

Table 1. Research progress of PeLEDs light extraction.

发表时间	器件结构	光提取方法	CE_max/cd·A^–1	EQE_max/%	最大亮度/cd·m^–2	寿命参数T50	参考文献
2017	4LG/Buf-HIL/MAPbBr₃/TPBi/LiF/Al	电极	18.0	3.8	13000	—	[25]
2018	Ag/(ZnO/PEI)/CsPbI₃NC /TCTA/(MoO₃/Au/MoO₃)	电极	—	11.2	1106	—	[26]
2018	Au/HIL/MAPbBr₃/TPBi/LiF/AL	电极	3.3	—	11270	—	[27]
2019	m-ZAgZ/HAT-CN/TAPC/CsPbBr₃/TPBi/Liq/Al	电极	7.21	—	4846	—	[28]
2018	Glass/AnoHIL/MAPbBr₃/TPBi/Li/AL	电极	42	8.66	—	—	[29]
2020	Glass/Au/ZnO/MQW perovskite/ TFB/MoO₃/Au	电极微腔	—	20.2	—	—	[31]
2017	Glass/ITO/PEDOT:PSS/(Agrods NPB)/ CsPbBr₃ NC/TPBi/LiF/Al	激元	1.42	0.43	8911	—	[33]
2017	Au NPs/PVK:MAPbBr₃:TPBi/ TPBi/Cs₂CO₃/Al	激元	7.64	1.83	16050	—	[34]
2019	Glass/NHAs/ITO/Poly-TPD/MAPbI₃/TPBi/LiF/Al	微纳	—	0.012	0.53 W·sr ^–1·m^–2	—	[36]
2019	Glass/Epoxy/AAM(TiO₂)/ITO/PEDOT:PSS/ BA: CH₃ NH₃ PbBr₃/F₈/Ca/Ag	微纳	—	17.5	48668	120 s	[38]
2019	Glass/ITO/ZnO/PEDOT:PSS/ CsPbBr₃/TPBi/LiF/Al	微纳	88.7	28.2	～25000	—	[12]
2018	Glass/ITO/ZnO/ZnO-PEIE/ FAPbI₃/TFB/MoO_x/Au	薄膜形貌	—	20.7	390 W·sr ^–1· m^–2	20 h	[11]
2020	Glass/ITO/ PEDOT:PSS/Perovskite/ B₃PyMPM/LiF/Al	器件结构	—	17.6	79700	—	[39]

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